Renewable and Sustainable Energy Reviews 54 (2016) 1148–1171

Contents lists available at ScienceDirect

Renewable and Sustainable Energy Reviews

journal homepage: www.elsevier.com/locate/rser

A review of potential innovations for production, conditioning

and utilization of biogas with multiple-criteria assessment
Wojciech M. Budzianowski n
Wrocław University of Technology, Wybrzeże Wyspiańskiego 27, 50-370 Wrocław, Poland

art ic l e i nf o a b s t r a c t

Article history: Biogas is a relatively mature renewable energy technology but still most commercial biogas power plants
Received 5 June 2014 require significant financial incentives. Additionally, local shortages of very cheap digestible feedstocks
Received in revised form limit biogas productivity, especially for larger biogas power plants ( 41 MWe). Innovations that could
7 August 2015
improve cost-effectiveness and resource efficiency of biogas energy technology are therefore required.
Accepted 20 October 2015
Available online 11 November 2015
Over the last few years a number of potential process innovations for biogas technology have been
proposed and investigated. However, the majority of these novel concepts has minimal or no impact on
Keywords: technology development. Disruptive innovations are very rare, but only they really matter for the economy.
Biogas Therefore review reports that systematically compare, analyze and evaluate the suitability of these emer-
Renewable energy ging methods with emphasis on technological excellence and realistic commercial potential are needed.
Process innovation
This study presents potential process innovations from most recent patent and academic literature
Multiple-criteria assessment
proposed for biogas (i) production, (ii) conditioning, (iii) utilization and (iv) industrial symbiosis. Within
Production
Conditioning
these four highly interdisciplinary categories the review attempts to provide short practical comments on
Utilization selected methods and briefly analyzes their perspectives and constraints. Further, relevant biogas process
innovation criteria are designed and multiple-criteria assessment of pre-selected potential process inno-
vations is made. The paper concludes with the characterization of innovativeness of selected solutions and
suggests future research needs for biogas energy technology that could bring new innovations in near term.
& 2015 Elsevier Ltd. All rights reserved.

Contents

1. Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1149
2. Potential process innovations in biogas production. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1150
2.1. Pretreatment to enhance digestibility of lignocellulosic biomass . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1150
2.2. Enhanced AD . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1152
2.2.1. Enhanced AD processes . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1152

Abbreviations: AD, anaerobic digestion; AER, absorption enhanced reforming; AFEX, ammonia fiber explosion; AHPD, autogenerative high-pressure digestion; ARP,
ammonia recycle percolation; AwR, alkaline with regeneration; BA, bottom ash; BM, biomethane; BS, biosyngas; C, degree of Celsius; CCR, CO2 capture and recycling; CCS,
carbon capture and sequestration; CH4, methane; CHHP, combined heat, hydrogen and power; CHP, combined heat and power; CI, compression ignition; C/N, carbon/
nitrogen; CO2, carbon dioxide; COD, chemical oxygen demand; COG, coke oven gas; CP, commercialization potential; CPB, cryogenic packed beds; CSTR, continuous stirred
tank reactor; CY, number of citations per year; DF, dark fermentation; DME, dimethyl ether; EECI, energy, environment and climate impact; Ef, factor of energy; EP,
electrochemical pretreatment; F–T, Fischer–Tropsch; FVW, fruit and vegetable wastes; GHG, greenhouse gas; GT, gas turbine; HCCI, homogeneous charge compression
ignition; HHV, higher heating value; HMF, hydroxymethylfurfural; HPRSS, high-pressure reactive solvent scrubbing; HRAP, high rate algal pond; HRT, hydraulic retention
time; HTL, hydrothermal liquefaction; IEA, International Energy Agency; IF, impact factor; IT, information technology; KOH, potassium hydroxide; KSAMBR, Kubota Sub-
merged Anaerobic Membrane Bioreactor; kWe, electrical kilo Watt; L, liter; LBM, liquid biomethane; LCA, Life Cycle Assessment; LHW, liquid hot water; LNG, liquid natural
gas; MBR, membrane bioreactor; MCA, multiple-criteria assessment; MCFC, Molten carbonate fuel cell; MEC, microbial electrolysis cell; MFC, microbial fuel cell; MFR,
microbial film reactors; MJ, Mega Joule; MOM, metal-organic material; MeOH, methanol; MSW, municipal solid waste; MWe, electrical Mega Watt; NaOH, sodium
hydroxide; NMMO, N-methylmorpholine-N-oxide; Nm3, cubic meter at standard temperature and pressure; NP, number of publications; NPK, nitrogen/phosphorous/
potassium; OLR, organic loading rate; ORFC, oxy-reforming fuel cell; O&M, operating and maintenance; PAH, polycyclic aromatic hydrocarbon; PEIO, primary energy input to
output; PEMFC, proton exchange membrane fuel cell; PSAP, patent status or academic performance; SCFA, short-chain fatty acid (or volatile fatty acids (VFA)); SI, spark
ignition; SNG, synthetic natural gas; SOC, soil organic carbon; SOFC, solid oxide fuel cell; SRT, solids retention time; SS-AD, solid-state anaerobic digestion; T, temperature
(K); t, tonne; TCOE, thermoeconomic cost of electricity; TRL, technology readiness level; TS, total solids; UASB, upflow anaerobic sludge blanket; USD, US dollar; Wh, Watt
hour; WWTP, waste water treatment plant; VPSA, vacuum pressure swing adsorption; VS, volatile solids; VSS, volatile suspended solids; %wt, percent by weight.
n
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E-mail address: [email protected]

http://dx.doi.org/10.1016/j.rser.2015.10.054
1364-0321/& 2015 Elsevier Ltd. All rights reserved.
 W.M. Budzianowski / Renewable and Sustainable Energy Reviews 54 (2016) 1148–1171 1149

2.2.2. Enhanced AD reactors . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1152

2.2.3. Solid-state AD . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1153
2.2.4. Two-stage AD. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1153
2.3. GHG mitigation in AD . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1154
2.4. Biohydrogen . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1154
2.5. Biorefineries integrated with AD . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1155
2.5.1. Integrated biorefineries for biofuels production involving AD. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1155
2.5.2. Algal biorefineries involving AD . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1155
2.6. Unconventional feedstocks for AD . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1156
3. Potential process innovations in biogas conditioning . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1157
3.1. Adsorption . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1157
3.2. Biological methods . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1157
3.3. Membranes . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1158
3.4. Absorption . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1158
3.5. Cryogenic methods . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1158
3.6. Hybrid methods. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1158
4. Potential process innovations in biogas utilization . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1159
4.1. Gas engines, gas turbines . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1159
4.2. Fuel cells . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1159
4.2.1. SOFCs . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1159
4.2.2. PEMFCs. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1160
4.2.3. MCFCs. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1160
4.2.4. MFCs. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1160
4.3. ORCs . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1160
4.4. Hybrid energy systems . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1161
4.5. Biofuels from biogas conversion . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1161
4.5.1. Biomethane . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1161
4.5.2. Biosyngas and biohydrogen. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1161
4.5.3. Biomethanol and bioDME . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1161
4.5.4. Higher biohydrocarbons . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1162
5. Potential process innovations in biogas relevant industrial symbiosis . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1162
6. Multiple-criteria assessment of potential biogas process innovations . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1162
6.1. MCA of innovations in literature. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1162
6.2. A new set of assessment criteria, indicators and weights designed for biogas innovations . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1163
6.3. MCA of potential biogas process innovations. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1164
7. Conclusions . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1165
8. Future research and development . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1167
Acknowledgments . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1167
References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1167

1. Introduction countries (e.g. technologies utilizing expensive energy crops)

because such biogas plants would make a loss. Consequently, for
Biogas is attracting significant attention as an increasingly those numerous countries [3–7], especially if they have limited
interesting renewable and sustainable energy technology. access to cheap digestible biomass, availability of innovations that
Although biogas technology seems relatively mature it is not could facilitate cost-effective production, conditioning and utili-
considered fully economically viable and usually requires sig- zation of biogas is of particular importance.
nificant financial incentives to successfully compete with com- An innovation is the implementation of a new or significantly
mercial fossil fuel based energy technologies [1–3]. Three major improved: (1) product (good or service), (2) process, (3) marketing
factors limit expanded adoption of biogas energy technologies: method, or (4) organizational method in business practices,
(i) high cost of digestible feedstocks, (ii) limited local availability of workplace organization or external relations. The minimum
such feedstocks and (iii) limited availability of innovations that requirement for an innovation is that the product, process, mar-
could make biogas energy more economically attractive. keting method or organizational method must be new (or sig-
In some highly developed countries such as Germany biogas nificantly improved) to the enterprise [8]. This study reviews only
production receives significant financial support which has led to process innovations in the field of biogas technology. A process
rapid expansion of this renewable energy technology over recent innovation is the implementation of a new or significantly
years. Attractive German financial incentives facilitate the use of improved production or delivery method. This includes significant
several raw materials as feedstocks for anaerobic digestion (AD) changes in techniques, equipment and/or software [8]. In general,
(e.g. dedicated energy crops) and therefore the overall production many new concepts are being constantly proposed for all com-
potential of biogas has significantly increased over the past two mercial technologies. However, only very few of them have or
decades. Also some other European countries like Denmark, Aus- might have realistic commercialization potential. Although
tria, Italy or Sweden have legislation and financial incentives breakthrough or disruptive innovations with significant commer-
beneficial for investments facilitating expanded use of biogas cialization potential are very rare, in practice only they matter for
energy. Unfortunately, most other countries offer insufficient or no the economy. Scientists should therefore constantly filter emer-
financial support for the production, conditioning and utilization ging concepts with potentially innovative character in order to
of biogas. Importantly, these countries usually cannot adopt most find most promising ones and to facilitate their diffusion and
of existing biogas technologies directly from highly developed possibly future commercialization. Academic [9–11] and patent
1150 W.M. Budzianowski / Renewable and Sustainable Energy Reviews 54 (2016) 1148–1171

[12,13] literature review studies can play this important role thus (2) manure, (3) lignocellulosic residues and (4) some cheap energy
supporting economic development. crops. Further, pretreatment of feedstocks with limited digest-
Recently published review studies have contributed to the ibility by various operations such as milling, comminution, disin-
current status of renewable biogas energy technology. Many tegration, hydrolysis, thermal and chemical treatment are high-
emerging potential process innovations have been thoroughly lighted as important processes to further increase the access to
analyzed. To mention only a few examples Zheng et al. [14] cheaper raw materials. Also processes associated with AD perfor-
reviewed several biomass pretreatment methods and discussed mance including stirring performance, mixing techniques, addi-
their advantages and shortcomings. Monlau et al. [9] reviewed tives (enzymes, trace elements), measurements and control tech-
suitability of lignocellulosic materials for biohydrogen and bio- niques receive much attention. Besides, novel enhanced and
methane productions. Ryckebosh et al. [15] reviewed techniques cheaper designs of reactors and auxiliary equipment are often
for biogas upgrading to biomethane while Abatzoglou and Boivin proposed. Finally, the use of AD in various integrated biorefineries
[16] reviewed biogas conditioning processes. Pöschl et al. eval- is addressed.
uated energy efficiency of various biogas utilization pathways [17].
Rasi et al. [18] reviewed trace compounds affecting biogas energy 2.1. Pretreatment to enhance digestibility of lignocellulosic biomass
utilization. However, original potential biogas process innovations
discussed in literature over the recent few years still need meth- Lignocellulosic biomass is often cheap and locally available raw
odological comparison with more recent ones to highlight process material. The production of lignocellulosic materials is about 200
innovations with realistic commercialization potential. billion tons per year [20]. However, complex, recalcitrant and
The main challenge in assessment of potential biogas process highly polymerized structures make them unsuitable for most
innovations is associated with their very low technology readiness conventional AD processes. Raw materials available for AD often
level (TRL). If for a promising process only an experimental proof include a fraction of lignocellulose which decreases biogas pro-
of concept was obtained (TRL 3) or a potential process innovation duction from unit feedstock mass. Pretreatment of lignocellulosic
was validated only in a laboratory (TRL 4), then very scarce biomass can decrease crystallinity of cellulose, reduce lignin con-
information is available and one cannot reliably evaluate such tent and thus facilitate access for microorganisms. Therefore,
potential process innovations and compare their performance processes for pretreatment that enhance digestibility of lig-
with alternative mature methods. Reliable numerical assessments nocellulosic materials have received much attention in recent lit-
of process performance within a whole energy system is possible erature. These processes include various physical, chemical and
rather for more mature processes with existing operational history biological methods. The major benefit from pretreating is the
and data [19]. For new, low TRL processes, even some basic data improved local availability of cheaper raw materials. However, an
needed for such evaluation is usually missing. From these reasons important drawback of many existing pretreatment methods is the
early stage potential process innovations should be rather pre- resulting increased cost of biogas production. Therefore, the suit-
evaluated based more on specialized expertise and on specifically ability of various pretreatment methods proposed in the literature
designed and easily measurable criteria. Such methods have been must be carefully analyzed for each specific business line.
exploited in literature (see Section 6.1) and additionally they are Major factors limiting the digestibility of the hemicellulose and
very affordable and cheap. Later, these pre-selected potential cellulose present in the biomass include: (a) lignin content,
process innovations can be further assessed via numerical meth- (b) crystallinity of cellulose, and (c) particle size. A successful
ods and finally via experimental research and piloting. Besides, pretreatment method aimed at improving the digestibility of raw
sometimes novel concepts need only minor improvement to reach materials should: (1) require low energy input, (2) avoid degra-
commercial status and for such cases review studies that sum- dation (especially oxidation) or loss of carbohydrates, (3) require
marize and analyze recent advances are very important. minimal and inexpensive chemicals and/or water, (4) avoid
Overall, the aim of this study is to highlight and as much as expensive pretreatment devices, (5) avoid formation of AD inhi-
possible evaluate potential biogas process innovations that have bitors, (6) avoid the need for waste disposal, (7) be flexible with
been recently suggested in patent sources and high impact aca- respect to the type of lignocellulosic biomass, and most impor-
demic literature. These potential process innovations are analyzed tantly (8) be cost-effective and environmentally friendly.
within four major categories: (i) biogas production (Section 2), (ii) An overview of state-of-the-art biomass pretreatment pro-
biogas conditioning (Section 3), (iii) biogas utilization (Section 4) cesses was provided by Zheng et al. [14]. The authors carefully
and (iv) biogas in industrial symbiosis (Section 5). Finally, Section reviewed several pretreatment methods, discussed their advan-
6 evaluates a few promising biogas process innovations within tages and drawbacks but still it was difficult to provide clear
each category by applying multiple-criteria assessment and positive recommendations as to which of the reported techniques
potential process innovations that might have significant com- achieved high biogas yield with low enough costs to be considered
mercialization potential are highlighted. The study is concluded in economically viable. It was however suggested that pretreatment
Section 7 while Section 8 provides outlook for future research and methods including dilute sulfuric acid, sodium hydroxide, liquid
development needs. hot water, and steam-explosion could not be recommended as
economically feasible. Three main factors must be accounted for
when evaluating pretreatment methods for AD: (1) improvement
2. Potential process innovations in biogas production in biogas yield, (2) cost of chemicals and (3) required temperature.
For example, Monlau et al. [21] showed that moderately costly
Biogas production is the first category where potential process sulfuric acid pretreatment gave 50% improvement in biogas yield
innovations are sought and analyzed. Within this category a sig- but on the other hand the required temperatures were as high as
nificant number of studies have been published over the last few about 170 °C. Consequently, this method would require integration
years. Topics address various ways of enhancing, controlling and with cheap thermal energy source, e.g. associated with biogas
optimizing anaerobic digestion (AD) and improving biogas yield combustion.
and/or biogas quality. Crucial points for improving the efficiency of Taherzadeh and Karimi [22] focused on lignocellulosic waste
biogas production that are frequently emphasized throughout lit- materials. It was concluded that thermochemical pretreatment
erature are associated with facilitated access to cheap raw mate- methods like hot water, dilute acid, ammonia fiber explosion
rials: (1) wastes from agriculture, industry and urban areas, (AFEX), and lime require significant capital investment [19], while
 W.M. Budzianowski / Renewable and Sustainable Energy Reviews 54 (2016) 1148–1171 1151

biological pretreatment methods are very slow [23]. Therefore, the thermo-chemical pretreatment of manure thus waste heat gen-
optimal pretreatment method should require limited capital and erated in biogas combustion could be employed. The combined
operating and maintenance costs as well as be sufficiently fast thermo-chemical pretreatment could use less expensive chemicals
leading to reduced volumes of pretreatment units. and thus achieve greater sustainability. In general, the pretreat-
Hendriks and Zeeman [11] reviewed the different effects of ment of manure had potential to improve about 3–8 times low
several pretreatment methods on the three main components of biogas production yield of manure compared with that of maize
the lignocellulosic biomass (lignin, cellulose and hemicellulose) to
silage [29]. Chen and Chen [30] suggested that biogas yield
improve its digestibility. It was found that steam, lime, liquid hot
dominated profits of pig manure projects and found that for a
water and ammonia based pretreatments had high potentials.
specific analyzed project the minimal required biogas yield was
They claimed that dissolving hemicellulose and alteration of lignin
structure are the main pretreatment mechanisms since they about 0.2 m3/kg manure. However, this figure may vary from
improved access of hydrolytic enzymes to cellulose. It was also country to country depending on existing economic incentives and
confirmed that chemical pretreatment methods such as con- energy prices.
centrated acids, wet oxidation, metal complexes, and solvents, NaOH vs. hydrothermal pretreatment of wheat straw were
although effective were too expensive to ensure economic feasi- compared by Chandra et al. [31,32]. NaOH pretreated feedstock
bility. On the other hand, pretreatment processes like steam, lime, enabled to achieve 87.5% higher biogas yield compared with the
liquid hot water (LHW) and ammonia were indicated as promising. untreated feedstock. Hydrothermally pretreated feedstock gave an
An economical evaluation of five different pretreatment technol- increase of 9.2% in biogas yield compared with the untreated
ogies (dilute acid, lime, hot water, ammonia recycle percolation feedstock. This result emphasizes that water/steam pretreatment
(ARP) and AFEX) was presented by Eggeman and Elander [19]. might have inhibiting effect on downstream biogas yield and thus
These authors used ASPEN Plus model of the ethanol plant and NaOH pretreatment is superior to hydrothermal pretreatment.
embedded each pretreatment process model in the plant model Pretreatment by ultrasonication was investigated by Cesaro
allowing for systematic comparison of impacts of various pre- et al. [33]. It was showed that ultrasonication was particularly
treatments on the full system. Most promising economic results
beneficial for lignocellulosic biomass where improvements in
were achieved with dilute acid and AFEX. Wyman et al. [24]
solubilization were achieved. Experimental results showed that
compared pretreatment methods by using identical analytical
ultrasonic energy intensity between 31 and 93 Wh/L enhanced
methods. The study selected following leading pretreatments
methods: (i) AFEX, (ii) ARP, (iii) dilute acid, (iv) flowthrough, biogas production up to 71%. Ultrasonication of sludge was also
(v) lime and (vi) controlled pH approaches. successfully analyzed by Pilli et al. [34]. Nevertheless, ultra-
Low intensity pretreatments such as mechanical, biological, sonication is an energy intensive technique and usually cannot
high pressure, and sonication often increase only the rate of AD. To improve the cost-effectiveness of biogas production.
increase both the extent of conversion and AD kinetics high Electrochemical pretreatment (EP) with a pair of Ti/RuO2 mesh
intensity pretreatments such as thermal hydrolysis are required plate electrodes that led to improved digestibility of sludge was
[25]. Although thermal hydrolysis has a high energy requirement, suggested by Yu et al. [35]. In general, EP improves conversion rate
it is needed in the form of thermal energy which is usually of organic materials and enables the use of smaller reactors with
available in biogas plants, e.g. from biogas combustion. reduced retention times. However, optimization of electricity
Cellulose dissolution is a relatively novel approach in biomass consumption would be required prior to demonstration of EP at a
pretreatment. Jeihanipour et al. [26] investigated the use of higher scale.
N-methylmorpholine-N-oxide (NMMO) for cellulose dissolution. Mechanical pretreatment of algal biomass was investigated by
Research results confirm very high dissolution of cellulose sug-
Tedesco et al. [36,37]. It was shown that significant improvement
gesting that an enhanced process employing moderate tempera-
in the digestibility of algal biomass (about 50%) could be achieved
tures (90 °C) and atmospheric pressure is feasible. Kabir et al. [27]
by mechanical pretreatment only with a Hollander beater. If
applied NMMO cellulose solvent to barley straw and forest resi-
mechanical pretreatment could be integrated with macroalgae
dues pretreated at 90 °C with 85% NMMO for 3–30 h. It resulted in
up to 90% improvement in biogas yield during the subsequent AD harvesting and made less energy intensive, the benefits in
compared with that of the untreated lignocelluloses. The main improved biogas yield would be interesting.
identified disadvantage was however the deteriorated efficiency of Siloxanes are major impurities in biogas derived from AD of
the recycled NMMO solvent for feedstocks with high lignin and sewage sludge from municipal waste water treatment plants
bark content. In addition, the use of chemicals for pretreatment (WWTP). Siloxanes can clog heat exchangers [38] and thus
usually have negative environment impact. Consequently, while increase O&M costs of municipal WWTP biogas plants. A process
using expensive chemicals for pretreatment, their multi-cycle for removal of siloxanes from sewage sludge by thermal pre-
performance and their environmental impact should carefully treatment with gas stripping was proposed by Oshita et al. [39].
accounted for. 90% of siloxanes were removed by thermal treatment with gas
Many other studies investigated several pretreatment pro- stripping at 80 °C with 0.5 L/min of air flow for 48 h. Additionally,
cesses but they dealt with various usually complex scientific issues biogas yield was increased by up to 60%. However, the out-gas
and were not aimed at providing recommendations on the suit-
from the sludge treatment process would contain much siloxane
ability of existing pretreatment methods. Solid state NaOH pre-
and odor. The out-gas could be however used as combustion
treatment was investigated by Pang et al. [28] by pretreating corn
oxidant in order to decompose the siloxanes and decrease the
stover with 4–10% solid state NaOH. Biogas yield improved by up
to 56%. Possibilities to reuse expensive NaOH were however not odor, e.g. in a sludge incineration process.
investigated thus economic feasibility remained unclear. Overall, pretreating all feedstocks with one technology is not
Thermal, chemical by calcium hydroxide and thermo-chemical realistic and therefore appropriate pretreatment method should
pre-treatments of pig manure were investigated by Rafique et al. be chosen taking into account primarily energy balance and costs.
[1] who found that the combination of thermal and chemical Since pretreatment requires usually high investment costs, only
pretreatments gave significant benefits in terms of biogas pro- methods that guarantee a very high increase in biogas production
duction. They identified 70 °C as the optimal temperature for rate and yield can make the pretreatment financially feasible [40].
1152 W.M. Budzianowski / Renewable and Sustainable Energy Reviews 54 (2016) 1148–1171

2.2. Enhanced AD increased biogas yield and a reduction in the H2S and CO2 con-
centration in the biogas were obtained. This process upgrades and
2.2.1. Enhanced AD processes purifies biogas and beneficially decreases pH in AD but the most
Enhanced AD can be achieved by applying various improved significant benefits could be expected by combining biogas spar-
bacteria, fungi and enzymes. Genetic engineering and nanoengi- ging with membrane enhanced reactors to prevent membrane
neering are considered two major pathways that can provide fouling.
support for enhanced AD. However, current technologies are most
frequently demonstrated only in lab (TRL 4) and further technol- 2.2.2. Enhanced AD reactors
ogy diffusion is limited by cost constraints of biological and One of the shortcomings of state-of-the-art AD technologies is
nanoscale materials production and application. In many cases it is high capital cost associated with reactors. The reactors are usually
unclear to what extent biological/nanoscale enhancement can made of expensive materials such as steel and/or concrete. Since
improve cost-effectiveness of biogas. Techniques such as thermo- AD is characterized by long HRT, large capacity reactors are
philic operation, process monitoring and control, biogas sparing required to hold slowly growing microbes. Besides, energy inten-
are other enhancement methods which can potentially produce sive stirring adversely impacts cost-effectiveness of the system.
additional benefits in terms of cost-effectiveness of AD. Reactors such as upflow anaerobic sludge blanket (UASB), fixed or
Merlin Christy et al. [41] reviewed enhanced AD through fluidized bed, textile, and membrane appear as countermeasures
microorganisms and enzymes. Research progress into cellulose that can enhance microbiological reactions. Moreover, reactor
degrading microbial strains, mixed consortia, and enzymes operation techniques such as multi-stage operation or effluent
enhancing AD were analyzed. Screened and genetically derived recirculation can offer further enhancement of AD reactors.
strains were shown as promising agents that could enhance biogas A combination of AD and a membrane bioreactor (MBR) – a
production from cheap resources, including difficult biomass such Kubota Submerged Anaerobic Membrane Bioreactor (KSAMBR)
as lignocellulosic one. However, the study reported few details and process was described by Kanai et al. [49]. Over recent years the
it is expected that the progress in this area might lead to business- KSAMBR has been successfully implemented in food and beverage
changing innovations. It was also emphasized that the adoption of industries at a full-scale. It consists of two main parts: (1) a
enzymatic hydrolysis in full-scale biogas plants would be limited solubilization tank and (2) a thermophilic AD reactor incorporat-
by high costs of enzyme production and there would be little ing submerged membranes. These membranes retain the metha-
chance for dramatic cost reduction. From such reasons it seems nogenic bacteria within the AD reactor allowing for the removal of
that developing an innovative cost-effective process for enhanced digestate. In addition, dissolved methanogenesis inhibitors gen-
AD based only on present-day biochemical knowledge will be erated during AD, such as ammonia, are separated in a permeate
difficult and future progress will require further researches clearly stream. This ensures the greater stability and CH4 yield of AD and
targeted at efficiency issues. makes the KSAMBR particularly suitable for the AD of feedstocks
Kazda et al. [42] claimed that especially fungi open new pos- with high nitrogen content, e.g. rich in proteins. Besides, due to
sibilities for AD of fiber-rich organic wastes. Due to higher tem- enhanced operation the KSAMBR has potential for down scaling
perature optima of fungal cellulolytic enzymes, the thermophilic AD reactors and for the use of increased solid matter content
process was suggested for AD of fiber-rich biomass. Fungi based (solid-state AD). Since the KSAMBR has been applied in several
AD needs research efforts before higher TRL can be achieved. full-scale plants and thus achieved TRL close to 9, it no longer can
Benefits from the use of thermophilic AD and its optimization be considered as a potential process innovation and is therefore
were investigated by Cavinato et al. [43]. The paper suggested excluded from the MCA made in Section 6. Nevertheless, further
55 °C as the optimal temperature for thermophilic AD of a mixture improvements based on the fundamental concepts exploited by
of cattle manure, agro wastes and energy crops. Biogas yield and the KSAMBR are feasible and need to be developed and investi-
methane content were improved under higher temperature AD. gated in the future.
Moreover, the process was more stable considering the parameters Youngsukkasem et al. [50] investigated the performance of
such as pH, ammonia or SCFA content. Thermally enhanced AD MBR for AD with focus on membrane type being the critical issue
gives opportunities for better thermal energy management in in MBRs. The synthesized hydrophilic hydroxyethylated polyamide
biogas plants at improved biogas yield and shorter HRT and thus 46 (HPA) and the commercial polyvinylidene fluoride (PVDF)
seems promising in a techno-economic perspective. membranes were found to be able to effectively supply nutrients
A significant shortcoming in AD is the lack of sufficiently reli- and separate dissolved metabolites, while retaining the slowly
able sensors to monitor key operating parameters. In addition, growing microbes. Biogas yield was slightly greater for PVDF
control systems able to ensure that AD continually operates under membranes compared with HPA membranes. No external pressure
optimized conditions are also lacking. Therefore, modern sensors driving force was required to operate the MBR-AD system because
[44] and powerful controllers capable of solving these problems autogenerated overpressure was just sufficient. Major advantages
are needed. Madsen et al. [45] reviewed novel monitoring tech- of MBRs for AD include: retaining microbial cells, separating AD
niques. Novel measurement techniques and reliable control tools inhibitors, improving process control and reducing biomass wash-
were analyzed. Most of these techniques would be however too out while main shortcomings are: membrane fouling, membrane
expensive for small-scale AD plants. Therefore, the authors sug- wetting, increased capital and O&M costs [51]. In a MBR-AD sys-
gested expanded use of cheap handheld and mobile process ana- tem membrane fouling could be to some extent controlled
lyzers. These mobile instruments can be shared between several through the optimization of operating parameters, especially of
smaller scale AD plants thus minimizing their operating costs. HRT and SRT [52].
In general, greater involvement of monitoring [46] and control in An enhanced membrane AD reactor (EMBADR) in which biogas
AD could be a significant source of enhancement in particular if AD was bubbled through the membrane surface preventing fouling
mathematical modeling tools achieve sufficiently high level [47]. was invented by Hong et al. [53]. Again, the EMBADR was operated
However, these solutions are recommended for larger biogas slightly above atmospheric pressure thus providing sufficient self-
systems where investment is justified by sufficiently high biogas generated driving force for permeation through the membrane
production. surface. By applying the EMBADR, the overall energy requirement
AD intensification by sparging biogas through raw liquid cow of the entire biogas system might be reduced compared with other
manure was proposed by Sanchez-Hernandez et al. [48]. An MBR-AD solutions. Bubbling biogas can have beneficial impact not
 W.M. Budzianowski / Renewable and Sustainable Energy Reviews 54 (2016) 1148–1171 1153

only on preventing membrane fouling but also on feedstock Dai et al. [62] addressed improved stability and performance of
characteristics [48]. SS-AD by digesting mixed food waste and sewage sludge where
Microbial film reactors (MFR) were reviewed by Singh and inhibiting effects observed in conventional mono-digestion were
Prerna [54]. With packing bed materials like PVC Pall rings, poly- successfully avoided in this mixed substrate SS-AD process.
urethane foam, carbon felt, nylon fibers, straw and wood chips the
MFR achieved reduced HRT and ultimately O&M costs. The film 2.2.4. Two-stage AD
and the pore structure immobilized microorganisms and led to Hydrolysis, acidification, acetic acid formation and methana-
increased methane yield. These reactors require however the tion are AD steps which conventionally are carried out simulta-
supply of hydrolyzate or alternatively biomass must be extremely neously in one reactor. These processes are however different and
well fractionated, otherwise the packing bed might be clogged. require different microbial strains and operating conditions. The
Effluent recirculation technique in two-stage AD reactors was combination of these four stages in one reactor degrades micro-
proposed by Aslanzadeh et al. [55] who found that the effluent biological biomass conversion efficiency. The build-up of metha-
recirculation supported the hydrolysis step [56] as well as enabled nogenesis microorganisms occurs slowly and hence conventional
to avoid nutrient loss at higher organic loading rate (OLR) leading single-stage AD reactors must have large dimensions to compen-
to the improved performance and stability of AD. Effluent recir- sate for the wash-out of microorganisms. In large single-stage AD
culation alleviated observed SCFAs inhibition in two-step AD due reactors energy-intensive stirring systems and the need for
to effects of dilution and pH adjustment [57]. increased heating requirements at low material conversion rates
Containerized scale or miniature AD reactors attract attention reduce cost-effectiveness. However, when AD is split into two
as suitable solutions for distributed biogas generation where the stages: (1) hydrolysis and acidogenesis in which the organic
transport costs of feedstocks can be reduced. The miniature AD matter is decomposed into liquid phase organic acids and other
reactors could be particularly suitable for low-income countries intermediates and (2) acetogenesis and methanogenesis in which
due to reduced capital costs. Rajendran et al. [58] evaluated a methane gas is produced from the liquid phase intermediates, the
novel design of a miniature AD reactor. The biogas yield from the resulting two AD reactors can be independently optimized and
miniature reactor was analyzed for the period of more than one thus biomass conversion efficiency can be improved. Besides, two-
year using a synthetic nutrient and an organic fraction of MSW as stage AD offers greater flexibility of biogas generation, an issue
feedstocks. For both tested feedstocks biogas productivity was which will be important to stabilize future solar and wind energy
about 570 L/(kg VS day), which indicated that the miniature AD rich energy systems with natural fluctuations [63].
reactor was effective in handling organic MSW fractions. In addi- One of solutions that exploits these considerations is a two-
tion, further capital cost reduction can be obtained by employing stage dry–wet AD with split hydrolysis and methanation process
cheap construction materials such as textile or other suitable (GICON process) which was commercialized a few years ago [64–
cheap polymers that can replace conventional AD reactors cur- 66]. The GICON process overcame several disadvantages of con-
rently made of expensive materials such as steel and/or concrete. ventional biogas plant designs. The two-stage operation made AD
more economical and versatile. Major claimed benefits included:
2.2.3. Solid-state AD (1) efficient yet stable AD process since the retention time of the
Conventional AD is operated at solid concentrations between feedstock in the system was decoupled from the methane forma-
0.5%wt and 15%wt. It is liquid AD. At solid concentrations higher tion, (2) decreased energy intensity since stirring was no longer
than 15%wt (up to about 40%wt) it is so called solid-state AD (SS- needed, (3) improved feedstock flexibility due to individually
AD). Animal manure, sewage sludge, and food waste [59] feed- controlled percolators, (4) higher methane content in produced
stocks are usually processed via liquid AD, while organic fractions biogas than that derived from conventional biogas plants (by
of MSW and lignocellulosic biomass can be treated also by using about 15–20%) because a portion of the CO2 was removed during
SS-AD. SS-AD requires smaller reactors and has alleviated energy hydrolysis, (5) resistance to feedstock rejects (plastic, glass, metal,
intensity associated with heating and stirring. Digestate of SS-AD etc.) and (6) solid residuals obtained from the percolators made
is characterized by lower water content and hence it is easier to both their transport and further processing more cost-effective.
handle than the effluent of liquid AD. On the other hand, SS-AD The GICON process seems to be an interesting process innovation
requires larger amounts of inocula, exhibits self-inhibiting effects disclosed in recent years, that will be able to improve cost-
potentially leading to process instability, and has much longer effectiveness of biogas energy technology.
HRT. Therefore, for successful operation SS-AD also requires var- A similar concept with split hydrolysis and methanation was
ious ways of enhancement. proposed by Hahn et al. [63] (ReBi process). The ReBi process is
The performance of SS-AD reactors was reviewed by Li et al. [60]. targeted at a flexible biogas production achieved through a tar-
The study focused on the impacts of solids content, temperature, C/N geted feeding of separated liquid hydrolysate into a fixed bed
ratio, and inoculation. The findings emphasize that biogas yield is reactor. In the first reactor during hydrolysis undissolved poly-
higher at higher operating temperature. The optimal C/N ratio is meric compounds are cracked into water-soluble monomers by
necessary to minimize the accumulation of SCFAs in the reactor since exoenzymes. The hydrolysate from the first step is sent to a screw
excess SCFAs inhibits the methanogenic activity. Besides, inoculation press to separate solid and liquid fractions. The solid fraction is
by digestate or leachate and decreasing the solid content both have processed in a CSTR to generate biogas. The liquid fraction com-
negative impact on the biogas generation. prising dissolved digestible materials is sent to a storage tank.
Zhu et al. [61] applied alkaline pretreatment to enhance biogas Further, a fixed bed reactor is fed whenever required with the
generation in a SS-AD reactor using corn stover as a feedstock. stored digestible materials to produce biogas. Advantageously,
Under their experimental conditions alkali pretreatment for 24 h the microbial consortium in fixed bed reactors is retained in the
led to depolymerization of corn stover including significant lignin reactor through a film formed on a packing medium that prevents
degradation at minimal cellulose loss. With 5% NaOH-pretreated a washout of bacteria and enables high OLRs.
corn stover the SS-AD generated 37% more biogas when compared A hydrolysis and acetogenesis step is particularly useful in
with the non-pretreated case. However, 7.5% NaOH pretreatment liquefying organic matter from unsorted MSW [67,68]. Bioliquids
caused inhibition of methanogenic activity due to too rapid obtained in the first AD stage are suitable for downstream high-
hydrolysis and acidogenesis leading to excessive SCFAs content. rate biogas production in the second AD stage. Any non-digestible
1154 W.M. Budzianowski / Renewable and Sustainable Energy Reviews 54 (2016) 1148–1171

constituents of MSW are retained and separated in the first AD under elevated pressure conditions. It subsequently increases the
stage and thus have no adverse impact on the second AD stage. content of methane in biogas and decreases CO2 emissions from
An experimental biogas production system exploiting two- biogas utilization [4]. Lindeboom et al. [81] investigated an auto-
stage AD in Szewnia Dolna (Poland) was described by Zalewski generative high-pressure digestion (AHPD) process suitable for
et al. [69–72]. The major claimed benefit was associated with biomethane production directly from high-pressure AD reactors.
greatly improved biomass conversion efficiency and thus biogas Operating pressures up to about 20 bar were most adequate for
yield. Both hydrolysis (1.5 m3) and methanogenesis (8 m3) reactors methane enrichment. Chen et al. [82] examined the pressure
were however conventional stirred tank reactors and although the effects in a two-stage AD, in terms of pH value, biogas yield and
process was claimed to have improved performance over single process stability. The results demonstrated that an increase in
stage AD, the energy use for stirring remained at a similar level. pressure led to a decrease in pH value in the reactor and CH4
Increased biogas yield from two-stage AD of maize silage was enrichment in the biogas. AD operation was stable with working
also showed by Colussi et al. [73]. In contrast, Ganesh et al. [74] pressure up to about 9 bar, despite the low pH value. The process
found that a one-stage AD process was superior over two-stage AD benefited from the production of compressed biogas which could
for investigated fruit and vegetable wastes (FVW). Ganesh et al. be injected into the public gas grid or bottled with minimized
[74] used a different two-stage AD process configuration than that requirements for pressurization. Since lower pH value alleviated
involved in the GICON process. Their two-stage process worked on the beneficial pressure effect on increased CO2-solubility, and thus
the principle of internal solids recycling after solid–liquid partly weakened the CH4 enrichment, an effective and economical
separation by centrifugation. Claimed advantage was very high method for maintaining pH value in the pressurized reactor should
substrate solubilization. In this research no attention was given to be developed, e.g. by employing mineral CO2 capture [83]. In [84]
decreased internal energy consumption due to reduced stirring 74.5% methane in biogas was obtained under 9 bar operating
requirements, etc. The results from [74] emphasize that claimed pressure in one step AD.
advantages of two-stage AD designs are not so obvious for all
available feedstocks and all possible configurations. Therefore, the
2.4. Biohydrogen
two-stage AD process must be very carefully designed and opti-
mized to maximize benefits. Various substrates may exhibit dif-
Biohydrogen is another gaseous energy carrier that can be
ferent performance while transitioning from one- to two-
obtained from biomass, often by involving techniques similar to
stage AD.
those used in AD. There are three major routes to produce bio-
Lemmer et al. [75] described a two-stage AD where the final
hydrogen: (1) fermentative production (dark and photo),
methanogenesis stage was realized under pressurized conditions
(2) enzymatic and (3) biocatalysed electrolysis. Dark fermentation
of 9 bar. The pressurized process allowed for generating methane
(DF) is the conversion of organic materials to bio-H2 via fermen-
enriched gas (up to 87% CH4).
tation. DF is a process involving several groups of bacteria and
multiple biochemical reactions using steps similar to AD. In con-
2.3. GHG mitigation in AD
trast to photofermentation DF proceeds in the darkness. In DF
biohydrogen is generated under lower pH than that applied in AD.
AD can be beneficially modified to reduce internal greenhouse
DF is today the most important biohydrogen production method.
gas (GHG) intensity [76,77]. In some cases such carbon manage-
However, the biohydrogen yields of DF are much smaller than the
ment has potentials to be value-added [78], i.e. changes originally
made only to improve a GHG balance, result also in improved cost- biogas yields of AD for similar substrates [85]. Therefore, DF can be
effectiveness, in particular when the whole value chain is taken employed only as a preliminary step in the conversion of biomass
into account. By adding or recycling CO2 the biomass conversion energy and usually needs to be followed by AD. Further, enzymatic
efficiency can be improved thus increasing biogas yield. The ability biohydrogen production is a non-natural route that generates
of AD to exploit additional CO2 is clearly a new emerging much more moles of H2 per mole of sugar, however it requires
enhancement option which requires more attention. very expensive enzyme materials. Finally, biocatalyzed electrolysis
An interesting two-stage AD process with CO2 management may use MCF to produce biohydrogen but this pathway has cur-
was proposed by Salomoni et al. [79]. In this process CO2 was rently very low energy conversion efficiency.
injected to the AD reactor in order to minimize CO2 production Results on high-rate bio-H2 generation employing mixed
and to enhance methane production. The process involving CO2 microflora were presented in [86]. They obtained about 1 mol H2/
injection attained high biomass degradation rate of 58% VSS mol sucrose and 15.6 m3 H2/(m3 day). The high-rate DF technology
reduction, was characterized by increased SCFA generation during was demonstrated in a pilot-scale using a 0.4 m3 digester. C. pas-
acidogenesis achieving the SCFA content of 8.4 g/L and increased teurianum and Bifidobacteria sp. were indicated as the preferable
biogas yield. Moreover, CO2 intake had a positive impact on the microbial species. The demonstration revealed that the factor of
overall GHG footprint of biogas generation. CO2 injection at low energy output compared with the energy input (Ef) ranged from
temperature and pH stimulated the acetogenic activity with about 14 to 29 on bio-H2. The obtained Ef was higher than in the
respect to methanogenic activity. case of biodiesel and corn/sugarcane ethanol but it was compar-
Bajón Fernández et al. [80] showed that by injecting CO2 into an able of cellulosic ethanol. Biohydrogen purity might be a less
AD reactor methane production increased. An enhancement of important parameter because biohydrogen rich streams can be
methane production was observed for food waste (by up to 13%) efficiently exploited within integrated biorefineries, e.g. for
and sewage sludge (by up to 138%), clearly demonstrating the injecting to AD for biogas to biomethane upgrading where high
potential of AD to utilize additional CO2. Associated CO2 reductions CO2 and methane contents in biohydrogen are no longer
for food waste (up to 11%) and for sewage sludge (up to 34%) were shortcomings.
estimated. It was concluded that the different substrate response González del Campo et al. [87] generated 1.3 L H2/L fruit juice
to CO2 enrichment enhanced the acetoclastic pathway of wastewater (1.4 mol H2/mol hexose) and proposed to utilize it in a
methanogenesis. downstream PEMFC stack without any purification step. The high
High-pressure AD has potential to improve also the overall concentration of CO2 (45%) did not lead to a failure in the opera-
GHG balance of a plant. The AD process minimizes the release of tion. The plant operated in a stable manner and achieved electrical
gaseous CO2 by improving CO2 solubilization in the liquid phase efficiencies close to 18.6% and 16% when it was running with
 W.M. Budzianowski / Renewable and Sustainable Energy Reviews 54 (2016) 1148–1171 1155

oxygen and air, respectively, and the overall energy efficiency was this concept residues from ethanol production were utilized
about 2.8% and 2.4% when oxygen and air were used, respectively. through AD. Obtained biogas was sent to a steam cycle to produce
A low-temperature (50 °C) process employing 13 enzymes to electricity and heat while process steam was beneficially recycled
convert xylose into bio-H2 achieving nearly full the theoretical to biomass pretreatment. This concept might benefit from using
yield was proposed in [88]. As xylose is a major constituent of mostly state-of-the-art technologies and could achieve some
lignocellulosic biomass (plants contain up to 30%wt xylose) this commercialization potential in future depending on cost-
novel biohydrogen production route might be promising in future. effectiveness of specific plant configurations and market needs.
But today, the process has TRL of 1 or 2, requires several expensive Bondesson et al. [95] also investigated integrated ethanol and
enzymes and thus has limited commercialization potential. biogas production. Innovativeness of their concept was associated
Shi et al. [89] found that 0.4% NaOH pretreatment of sweet with the use of sulfuric acid for biomass pretreatment which (in
sorghum stalks resulted in 2.3 fold higher biohydrogen production contrast to pretreatment by steam explosion) was claimed to give
rate with mixed microbial cultures. This beneficial pretreatment no rise to inhibition effects and high yields of both ethanol and
effect emphasizes that DF and AD have similar technological biogas could be therefore achieved.
requirements and can be applied to substrates pretreated in the The integration of AD into a biorefinery with simultaneous
same way. Therefore, DF and AD can be easily integrated within coproduction of bioethanol and biohydrogen (IBBB process) was
biorefineries. For example, Buitrón et al. [90] showed that by analyzed by Kaparaju et al. [96]. Wheat straw was pretreated by
applying sequential production of biohydrogen and biogas from water/steam and split into liquid hydrolizate and solid fiber frac-
tequila vinasses a high organic matter conversion rate of 75% and tions. The hydrolizate fraction was subject to biohydrogen pro-
consequently a high amount of gaseous biofuels were achievable. duction while fibers were further processed via enzymatic
hydrolysis and the obtained secondary hydrolizate was fermented
2.5. Biorefineries integrated with AD and distilled to bioethanol. Effluents from bioethanol distillation
and from biohydrogen generation were smoothly anaerobically
Biorefinery technologies are developing very quickly aiming at digested to produce biogas from residues unsuitable for any pro-
cheap and locally available feedstocks as well as highly integrated cessing. The IBBB process based biorefinery is therefore very well
and efficient systems [91]. AD supplements biorefineries by integrated and could offer significant commercialization potential,
ensuring a high conversion rate of organic waste streams pro- in particular if feedstocks other than wheat straw could be
duced within biorefineries. Biorefinery wastes are converted to employed.
useful forms of energy such as biomethane, electricity, and heat A different approach for integrating AD into a biorefinery was
which are employed within biorefining processes leading system proposed by Hoffmann et al. [97]. First, organic feedstocks were
integration, both in terms of energy and material. It can be even converted via AD. Biogas was reformed to biohydrogen while
claimed that biorefinery concepts with commercialization poten- residual digestate was processed via hydrothermal liquefaction
tial have to involve AD because it is able to improve their resource (HTL). Main innovation arise from the fact that HTL products
use efficiency and economic viability. Today most significant (biocrude) were upgraded with biogas-derived hydrogen and
challenges are associated with methodologies for integration of AD further processed to biofuels. It was claimed that the process could
into rapidly developing biorefinery concepts. Very simple and recover 62-84% of bioenergy as biofuels. Besides, significant
small biorefineries can be applied locally and benefit from the potentials for internal heat integration exist as well as the authors
availability of local feedstocks with minimal transport costs. On clearly indicates potentials for synergies with other sectors, e.g.
the other hand, more complex and larger scale biorefineries can with wind, solar, CHP, biomethane and organic fertilizers.
produce a range of higher value products and can benefit from Huerga et al. [98] also suggested that biodiesel production from
potentials associated with improvement by material and energy Jatropha curcas could benefit from integration with AD, where AD
integration. Innovations for biorefineries of different scales are mainly served as residues converting technology (meal from oil
therefore needed. extraction and glycerin from biodiesel were employed as AD
feedstocks). Biogas received only 8.4% of total energy in favor of
2.5.1. Integrated biorefineries for biofuels production involving AD biodiesel (35.7%) and husks/shells (39.5%). The process is simple
Several processes integrating AD with the production of bio- and can be suitable for locations with access to cheap Jathropa
hydrogen, bioethanol or biodiesel have been developed over curcas biomass. However, even if the general direction is correct
recent years. These processes, especially when integrated together, [99] the economics of the integrated biodiesel/biogas process will
can contribute to the emerging biorefining industry [92]. For be largely determined by future biodiesel prices. The integration of
example, a biorefinery concept in which organic materials were a biodiesel plant with a dedicated biogas plant employing only
directed to DF for biohydrogen production was proposed by Poggi- clean feedstocks from biodiesel processing seems to be a more
Varaldo et al. [93]. Residues from DF were split into a liquid frac- favorable option than co-digestion of biodiesel derived residues
tion including short-chain fatty acids (SCFA) and a solid fraction. (including glycerol) with sewage sludge [100]. The reason is that
The liquid fraction with SCFA was converted via a microbial fuel by excluding impure sewage sludge, biofertilizers of high quality
cell (MFC) to electricity and via photo-fermentation to biohydro- can be obtained from a biorefinery improving its overall economic
gen. Electricity from the MFC was utilized in a microbial electro- performance.
lysis cell (MEC) to produce additional biohydrogen. Further, the
solid fraction from DF was directed to AD and optionally to bio- 2.5.2. Algal biorefineries involving AD
logical processes to produce high value biomaterials. Biomethane AD is required to make algal biorefineries sustainable [101]. In
and solid fertilizers were the two final products from this well recent years a few interesting integrated algal biorefinery concepts
integrated biorefinery. However, major shortcoming is the neces- utilizing AD have been proposed. The simplest design was ana-
sity for the use of MFC and MEC which seem rather inefficient and lyzed by Collet et al. [102] where algal biomass was fed to AD for
are still emerging technologies with very limited commercializa- biomethane production. This technologically simple solution can-
tion potential today requiring huge progress in novel materials and not be however cost-effective today because production costs of
processes. algal biomass are very high thus rather unsuitable for direct use in
A simple integrated biorefinery involving bioethanol and bio- AD. However, in LCA only perspective algal-AD biorefineries are
gas co-production was analyzed by Djuric Ilic et al. [94]. Within clearly promising and additionally they are characterized by lower
1156 W.M. Budzianowski / Renewable and Sustainable Energy Reviews 54 (2016) 1148–1171

land use than conventional energy plant crops [103]. Therefore, in Overall, algal AD based biorefineries still require fundamental
the future the reduction of algal production costs in algal-AD researches directed toward improved energy performance and
systems is a central issue. It can be achieved by employing algal economic feasibility. The most important shortcoming of algal AD
biomass for the production of high-value materials and chemicals based biorefineries is the requirement for expensive nutrients and
and exploiting residues for biofuels production. This would how- growth control agents supply for algae cultivation that are usually
ever require sophisticated technologies for the conversion of algal produced in highly energy intensive processes with little poten-
biomass which today are still at low TRL levels. tials for dramatic cost reduction. Therefore, biorefineries involving
The enhanced utilization of algal biomass in a biorefinery was recycling of water, CO2 and nutrients and thus needing less addi-
proposed by Zhu [104]. Algal oil was extracted from algal biomass tional costly nutrients are very promising as regards to the
and used for biodiesel production via transesterification. Residues reduction of algal biomass cultivation costs [110]. Nevertheless,
from oil extraction were fermented to bioethanol. Residues from agricultural and forest biomass are much cheaper today than algal
bioethanol were sent to AD and only the final residues in very biomass. Hence, the future of algal biorefineries integrated with
small quantities were recycled to the algal plant. Water and CO2 AD to large extent depends on the availability of algae processing
produced within transesterification, fermentation and AD steps methods converting algal biomass to high value products and only
were also recycled to the algal plant. This ever recycling integrated unusable residues to biogas. When algal biomass processing
biorefinery converting algal biomass to high-value liquid biofuels technologies develop to higher TRLs, e.g. those for the extraction of
has greater potentials for achieving resource and energy efficiency amino acids or lipids, great amounts of residual algal biomass
than the concept relying only on converting algal biomass into might be available for economically viable AD treatment and
biogas. A similar concept was presented in [105], see their Figure 3. biogas production [111,112]. Consequently, the relevance of algal
The presented system enabled effective recycling of water and CO2 biorefineries involving AD will be more pronounced with the
from ethanol fermentation and AD as well as nutrients such as N growing demand for algal products and the development of the
and P from the recirculation of digestate. Economic feasibility of entire bioeconomy.
these algal technologies depends on the prices of biofuels (bio-
diesel, bioethanol and biomethane), algae production costs and 2.6. Unconventional feedstocks for AD
specific cost requirements associated with recycling, especially of
CO2. Most processes discussed above utilize various approaches for
A biorefinery concept involving algae cultivation, CO2 feeding ensuring greater resource flexibility, e.g. by biomass pretreatment
derived from fossil fuel-fired power plants and AD was proposed or by employing residues. This Section addresses feedstocks other
by Gong and You [106]. This technology encompassed the fol- than conventional biomass. It is shown how innovative processes
lowing stages: power plant flue gas purification, algae farming, can be used to more significantly improve resource flexibility by
harvesting and dewatering, followed by lipid extraction, residues apply AD to feedstocks which seem rather unconventional, e.g. to
treatment by AD, biogas utilization and finally algal oil upgrading. coal or organic industrial wastes. Also processes that convert
Residues from lipid extraction were partly recycled to algae cul- residues from AD itself are addressed.
tivation as nutrients and partly anaerobically digested to biogas. High methane content biogas can be produced via AD from
Biogas was reformed to H2 and used in lipids (algal oils) hydro- coal, including coal residues or abandoned mines (coal-AD pro-
genation to obtain biodiesel. This proposed process might benefit cess) [113]. Microbes utilized in this study were isolated from
from technological simplicity and could have potentials for cost- gassy coal mine water. Coal used in this study was hard coal of the
effectiveness in case of high biodiesel prices. Additional benefits Jitpur coal mine. Biogas with methane purity of 90% CH4 was
would arise from CO2 utilization and this could to some extent obtained at optimum condition with little CO2. This coal-AD pro-
balance significant algae cultivation and post-processing costs. cess could be useful in improving exploitation of coal mines where
A mixed trophic state process for biodiesel and biogas copro- usually only about 60-70% of coal is extracted. Also, this coal-AD
duction was proposed by Bohutskyi et al. [107]. Although, the process might have commercialization potential as non-thermal
authors confirmed that conversion of algae into biomethane and thus low energy intensive coal gasification technology
through AD, as a sole conversion technology, had a higher useful enabling underground coal gasification [114] to methane rich
energy production potential compared with conversion into bio- biogas. The coal-AD process can be especially useful for coal mines
diesel or bioethanol alone [108] since AD converts all biomass where conventional coal extraction methods are not economically
fractions, including lipids, into biogas. However, they suggested feasible. Since coal is very cheap nowadays, coal mines in several
that liquid biofuels, such as jet fuel and drop-in biodiesel, were countries operate sell coal without profits and thus they seek
likely to be greatly preferred as commercial biofuel products. viable alternative solutions. Taking into account the molar C:H
Therefore, coupling biodiesel with biomethane production pro- ratio of methane (1:4), the coal-AD process may enable the tran-
vided both the largest total energy output and the most eco- sition of conventional coal mines to low-carbon counterparts.
nomically feasible process, especially for algae with high lipid Organic wastes are a significant problem of waste management
content. Such studies emphasize the most suitable role for AD in modern cities. The study of Molino et al. [115] demonstrated
technology. Namely, AD needs to be dedicated to conversions of that several types of organic wastes can be converted into biogas
feedstocks that cannot be processed to products with values via AD. The process discussed by Molino et al. [115] is somewhat
higher than that of biogas. AD is the most cost-effective when real similar to the previously discussed GICON process [66] where
organic residues are used as feedstocks. organic wastes are pretreated through hydrolytic liquefaction by
An advanced biorefinery concept including numerous tech- percolation. Percolation is highly resistant to non-digestible
nologies able to convert algal biomass not only to biofuels (bio- impurities in MSW while the liquid product of percolation
diesel, bioethanol, biohydrogen) but also to value-added chemi- (hydrolyzate) is highly suitable for methanogenesis. This process
cals, food and fertilizers was proposed by Uggetti et al. [109]. Such emphasizes that AD can be adjusted for difficult feedstocks.
multiple product biorefineries could potentially maximize cost- Residues from AD can be also utilized as fuels, fertilizers and
efficiency, even if biomass would have to be transported from other value-added products. In the work of Abubaker et al. [116] it
larger distances. However, their commercialization potential is was shown that household digestate was a very useful soil ferti-
limited because present-day and even near-term processes are lizer improving yield in wheat cultivation. Fertilization results
insufficient to implement these multiple product biorefineries. were improved over the application of conventional NPK
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fertilizers. Kim et al. [117] proposed to utilize hydrothermal car- adsorbent for simultaneous separation of carbon dioxide and
bonization process to convert residues from AD into C-rich fuel. hydrogen sulfide was proposed by Mostbauer et el. [120] (BABIU
The study determined optimal temperature for hydrothermal process). The study described a pilot scale demonstration of the
carbonization at 220 °C. BABIU using up to 1 000 kg of BA and up to 10 Nm3/h of real
landfill gas. Under the variable input gas flow rate the optimal
process performance was found at an input flow rate of 3.7 Nm3/(h
3. Potential process innovations in biogas conditioning tBA) allowing for 99% removal of hydrogen sulfide. The BABIU was
operated in a batch mode. Biogas was pumped through a column
Biogas conditioning is generally aimed at: (i) a purification containing BA rich in calcium, CO2 and H2S were absorbed in the
process including the removal of trace components adversely BA and thus the resulting biomethane met the requirements for
affecting the gas transmission grid, appliances or end-users and H2S content and had a high concentration of CH4. BABIU is
(ii) an upgrading process targeting at the removal of CO2 in order environmentally benign as it uses waste adsorbents [121] from
to adjust the calorific value and relative density complying the technologies beneficially employed in the same plant thus allow-
Wobbe Index requirements. Biogas purification is a compulsory ing for material integration. The sorption performance is too large
step while biogas upgrading is usually optional. It is usually ben- extent dependent on the content of calcium in BA and hence
eficial when these two processes are integrated. before any waste adsorbent is considered for biogas purification/
In biogas purification main trace contaminants include H2S, upgrading calcium content needs to be estimated.
NH3 and siloxanes. However, the content of these impurities lar- Metal-organic materials (MOMs) for CO2 separation analyzed
gely depends on the biogas origin. For example, biogases gener- by Nugent et al. [122] enabled an improvement in kinetics and
ated at landfills and obtained from cattle manure/corn silage AD thermodynamics that offered high volumetric uptake at low car-
have completely different contents of contaminants. These bon dioxide partial pressure well below 0.15 bar. In addition, high
unwanted species may imply e.g. corrosion, erosion or fouling as CO2-N2 and CO2-CH4 sorption selectivities were attained under dry
well as harmful environmental emissions. A comprehensive and moist operating conditions. TRL of this option is however still
overview of commercial and developing biogas purification pro- too low and further fundamental research with the use of real
cesses was provided by Abatzoglou and Boivin [16]. biogases is needed. Because MOMs are relatively expensive
In biogas upgrading bulk CO2 is separated to raise the calorific materials, the operational benefits would have to be significant to
value of biogas. Since biogas comprises usually about 35% of CO2, achieve economic feasibility of MOMs based biogas conditioning
upgrading processes are likely to be energy intensive. A compre- projects.
hensive overview of commercial and developing biogas upgrading
processes was provided by IEA [118]. This reference highlighted
3.2. Biological methods
four upgrading processes: (1) cryogenic upgrading (GPP system),
(2) in-situ methane enrichment, (3) ecological lung and
An alkaliphilic microalgal-bacterial consortium to generate
(4) removal of methane from the off-gas. However, these four
biogas within a system comprising a high-rate algal pond (HRAP)
processes seem to have limited commercialization potential in the
and an absorption column for the removal of CO2 and H2S from
near-term. Namely, cryogenic upgrading is the most promising for
biogas involving a liquid recycle loop was applied by Bahr et al.
some niche applications such as the production of liquid bio-
[123]. The process efficiently separated CO2 and H2S while O2
methane (LBM), equivalent of liquid natural gas (LNG) [119], but
content in biomethane was kept below 0.2% by utilizing only
for other, more conventional applications, the reduction of internal
process control strategies. The application of algal based biogas
energy requirement remains a challenge. Energy efficiency of in-
conditioning methods leads to biomethane with some oxygen
situ methane enrichment is unclear due to significant energy
content which is suitable for direct combustion but other appli-
requirement for air venting and additionally air venting may lead
cations such as biomethanation might require very low oxygen
to unwanted emissions when fermentative solution is bubbled
content that is difficult to achieve with algal methods.
with fresh air. Ecological lung suffers from very unstable carbonic
A microbiological photobioreactor connected to AD was pro-
anhydrase performance in realistic systems. Carbonic anhydrase
posed by Converti et al. [124] but issues such as oxygen enrich-
requires sophisticated techniques to retain its catalytic activity in
ment in biomethane and biogas dissolution need further clar-
realistic conditions because it is lost very quickly. Finally, removal
ification before demonstration could take place. In addition solar
of methane from the off-gas is only a side technology of minimal
practical importance in biogas upgrading. Consequently, in view of driven microbial processes are usually very slow and hence the
these challenges, this study must analyze and evaluate more entire economic feasibility of this technique is questionable.
examples of process innovations that can improve cost- A process in which raw biogas was scrubbed with a sodium
effectiveness of biogas conditioning. carbonate rich growth liquor derived from an algae plant (biogas-
The removal of trace contaminants can be beneficially carried ALG process) was disclosed by Kampanatsanyakorn [125]. CO2
out together with CO2 separation. Such integrated solutions can reacted with carbonate to form bicarbonate which was fed to the
offer significant cost reduction of biogas conditioning. Most of algae plant. Algae metabolized bicarbonate and the obtained car-
biogas upgrading methods discussed below have the ability to bonate solution was recycled back to the scrubber. Since biogas
simultaneously separate trace contaminants and CO2. Adsorption, was not bubbled through algae solution, as in the conventional
biological methods, membranes, absorption and cryogenic meth- algal biogas upgrading processes, no oxygen was beneficially
ods can all use multi-step operation, biogas recycling, advanced present in the biomethane. Biogas-ALG has also no limitations
multifunctional materials, trace contaminants conversions and regarding kinetics because the CO2 separation and carbonate
other process intensification techniques to increase the efficiency consumption are decoupled and their scales can be suitably
of integrated trace contaminants/CO2 separation. adjusted. Consequently, the biogas-ALG process has potentials to
achieve greater operational flexibility and improved cost-
3.1. Adsorption effectiveness. However, high costs of algae cultivation remains a
challenge. Nevertheless, biogas-ALG is a step forward to reduce the
A process in which biogas was converted to a high CH4 content production costs of algal biomass by integrating an algae farm
gas with the use of MSW incineration bottom ash (BA) as an with biogas conditioning.
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3.3. Membranes minimized waste generation due to improved utilization of spent

absorbents as fertilizers (K, N based carbonates and sulfates) and
Progress in membrane based biogas upgrading largely depends less energy intensive biogas upgrading process by applying pres-
on the availability of new materials. Biogas upgrading by mem- surized CO2 absorption. The resulting biomethane had higher
branes was reviewed by Basu et al. [126]. The authors concluded pressure and was more suitable for grid injection, bottling and
that only 8-9 polymer materials were investigated in relation to transport applications thus additionally benefiting from reduced
biogas conditioning. Polyimide and cellulose acetate based mem- energy requirement of biogas conditioning. The HPRSS integrates
branes were found to be the most suitable commercial membranes several benefits in one process that can be operated in a stand-
for biogas upgrading and cleaning. Future research on more tar- alone version suitable for distributed biogas based systems.
geted polymers that would reduce plasticization and improve The AwR and HPRSS do not require a desorption step needed in
membrane longevity was recommended. Inorganic membranes all conventional absorption based technologies for spent absor-
which were reported to produce 5-10 fold higher selectivities than bent recovery. Desorption is usually very energy intensive, espe-
conventional polymeric membranes still could not more broadly cially for chemical absorption since a lot of energy needs to be
enter the membrane market dominated by polymeric materials. delivered for the release CO2/H2S that was absorbed via strong
Similar conclusions were more recently provided by Zhang et al. chemical bonds. Therefore, vacuum desorption of CO2 from CO2-
[127]. loaded solvents that can operate below 80 °C and thus use low
Single stage gas permeation processes are usually not able to temperature heat is promising for improving energy efficiency of
generate a sufficiently high CH4 purity and at the same time obtain desorption in absorptive biogas conditioning. Ahn et al. [137]
a sufficiently high CH4 recovery. Hence, multistage membrane demonstrated that vacuum desorption was feasible at 80 °C in the
systems are necessary in biogas upgrading plants [128]. Mem- system that was enhanced by membranes. The required minimal
brane based processes employing four types of polymeric mem- temperature level depended on pressure range applied.
brane modules were evaluated via techno-economic methods
[129] revealing that the two stage in cascade membrane module 3.5. Cryogenic methods
with a recycle loop was sufficient for biogas upgrading. The total
upgrading cost, including the cost of raw biogas, was about 0.17 Cryogenic biogas upgrading is still meeting some operational
USD/Nm3 which was competitive with the natural gas market challenges. However, since some groups of stakeholders show the
price at that time. large interest in cryogenic methods, the technology may soon
CH4/CO2 membrane separation from landfill biogas was suc- undergo more rapid development, especially if effective solutions
cessfully demonstrated by Kim et al. [130] at the Gyeong-ju landfill for the existing problems are found [138].
site, Korea achieving CH4 with 88% purity and 86% CO2 removal Cryogenic biogas upgrading using a GPP process disclosed in
efficiency. These recent demonstrations bring membrane based [139]. This process was also mentioned by IEA [118]. The GPP
process innovations for biogas conditioning closer to the market. process could be most promising for some special applications
such as the production of liquid biomethane (LBM), equivalent of
3.4. Absorption liquid natural gas (LNG) [119]. The claimed benefit of the GPP
system includes the production of pure liquid CO2, which can be
Physical and chemical absorptions are both feasible for biogas utilized in CO2 utilization technologies requiring high purity CO2.
conditioning. Methods involving cheap and environmentally Optionally, purified biomethane can also be liquefied [140]
benign absorbents such water [131] are usually energy intensive and therefore the GPP process could be an innovative solution for
due to pressurization requirement. More effective absorbents are the production of LBM. Other more conventional cryogenic options
expensive and usually have adverse environmental impacts. without significant co-benefits cannot be recommended at this
Therefore, innovative approaches to solvent based CO2 absorption stage because of too high internal energy consumption
are needed [132]. Process innovations must meet the requirement requirements.
of economic feasibility and minimized environmental impact. It A process for biogas cleaning employing cryogenic packed bed
mainly depends on the appropriate selection of an absorbent, (CPB) operated in a dynamic manner was proposed by Tuinier and
energy intensity of an associated separation process, and effec- van Sint Annaland [141]. It was calculated that the CPB requires a
tiveness of integrating biogas conditioning into the entire plant 22% lower energy duty (2.9 MJ/kg CH4) than more conventional
system. vacuum pressure swing adsorption (VPSA) (3.7 MJ/kg CH4). These
A few interesting process innovations have been recently pro- calculations show that the CPB uses only about 5% of methane’s
posed for biogas conditioning involving chemical absorption heat of combustion.
relying on the use of residues for absorbent regeneration or co-
production of fertilizers from spent absorbents. For example, a 3.6. Hybrid methods
KOH and NaOH absorption process (alkaline with regeneration,
AwR process) was described by Starr et al. [133]. In the AwR By integrating two or more purification/upgrading methods
process CO2 was absorbed by using an alkaline solution of potas- one can exploit their advantages and hinder drawbacks. Potentials
sium hydroxide (KOH) or sodium hydroxide (NaOH). Spent are also associated with integrating different upgrading technol-
absorbent was regenerated at a rate of 70% when put into contact ogies in one device thus minimizing capital costs. For example, by
with residues comprising a significant proportion of calcium. using an absorbent in the form of a liquid membrane physically
Regenerated alkaline solution was reused for CO2 removal from detached from the biogas by a solid porous membrane [142]
biogas, see Figure 1 in [134]. The major benefit of the AwR is the innovative CO2 separation is obtained. Namely, impurities from
improvement in economic feasibility by exploiting calcium rich biogas do not degrade the absorbent. In addition, the hybridized
waste materials [135]. But in locations where the access to free or system achieves a high CH4/CO2 selectivity and the absorbent can
better cost negative calcium residues is limited the innovativeness be more easily regenerated involving minimized CH4 slippage
of the AwR is also limited. being a huge problem in realistic biogas conditioning technologies
Another concept is a high-pressure reactive solvent scrubbing such as water wash.
process with fertilizing effects of KOH and NH3 based salts that Scholz et al. [143] analyzed seven membrane based hybrid
was proposed in [136] (HPRSS process). The HPRSS offers biogas upgradation methods. It was revealed that two studied
 W.M. Budzianowski / Renewable and Sustainable Energy Reviews 54 (2016) 1148–1171 1159

hybrid processes involving pressurized water scrubbing were efficiency (about 45%) and ultra-low NOX emissions (o0.27 g/
characterized by the minimal upgradation cost. This work kWh) were achieved (biogas-HCCI). These studies clearly show
emphasizes that process hybridization is an attractive approach to that a biogas fueled HCCI engine is a promising alternative for a
generate process innovations which can compete with the state- small-scale biogas based distributed stationary power generation
of-the-art biogas conditioning techniques. applications.
A method for the removal of NOX from biogas engine exhausts
by contacting flue gases with liquid digestate in underground tank
4. Potential process innovations in biogas utilization reactors filled with packing media to increase contact surface area
(biogas-NOX process) was invented by Matelich [159]. This process
Biogas can be utilized in raw and upgraded forms via various ensures decreased NOX emissions, however, odor emissions are
pathways. Commercially feasible biogas utilization methods still a problem.
include: (1) electricity generation with CHP or fuel cells, (2) mul- Flameless combustion (also known as diluted or mild com-
tigeneration of heat, steam, electricity and cooling in industry, bustion) is a combustion technique with potentials to alleviate
(3) injection in the gas grids, (4) transport fuel, and (5) production unwanted emissions and improve fuel conversion efficiency. It
of chemicals [144]. Biogas can be also utilized for (6) energy sto- applies high degree of preheating of the combustion oxidizer and/
rage applications, (7) to stabilize intermittently operated wind and or recycled flue gases. Flameless combustion was applied to dif-
solar renewable energy systems [3] or (8) in cooking and lightning ferent fuels in the past, but applications to biogas are still rela-
applications especially in rural districts of underdeveloped coun- tively novel. Effugi et al. [160] investigated biogas flameless com-
tries. Other useful products of this renewable energy resource bustion and identified operating parameters maps for stable bio-
include (9) digestate, (10) organic fertilizers derived from poorly gas flameless combustion. Moreover, it was found that not only
digestible biomass and (11) biohydrogen. Digestate and organic flameless combustion could be effectively used for biogas, but also
fertilizers are useful in sustainable cropping systems while bio- that it was able to reduce soot and PAHs emissions. Hosseini and
hydrogen can be applied in biorefineries. Wahid [161] (biogas-flameless) claimed that for flameless biogas
According to [17] the Primary Energy Input to Output (PEIO) of combustion in a furnace based system electrical efficiency of 53%
small and large-scale biogas utilization methods ranges between and CHP efficiency of 82% together with low NOX emissions were
about 4–46% and 1–34%, respectively, depending on the applied possible.
energy conversion systems and fossil fuel substitution. This broad More conventional approaches such as lean burn or exhaust gas
range achievable by state-of-the-art technologies suggests that the recirculation were also systematically analyzed showing some
structure of the biogas based system and the involvement of efficiency improvement and emission reduction at very low
process innovations play a significant role in ensuring energy investment cost [162].
efficiency enhancement and finally economic viability of biogas
utilization systems. 4.2. Fuel cells

4.1. Gas engines, gas turbines Fuel cells is a new class of power-generation technologies
converting chemical energy of fuels directly and with relatively
In most commercially run biogas power plants internal com- high efficiency into electricity at reduced harmful emissions [163].
bustion engines such as gas engines [145] have become the stan- Biogas utilization in fuel cells is more challenging than natural gas
dard technology. Other state-of-the-art options include: (1) dual utilization due to trace impurities that can poison catalysts and to
fuel engines [146–149] in which biogas can be co-fired with CO2 enrichment which can contribute to carbon deposition.
usually very small proportion of e.g. bio-diesel, bio-ethanol or bio- Therefore, biogas fed fuel cells require special configurations and
DME, (2) micro-gas turbines [150] that are available on the market fuel handling approaches to minimize these negative effects.
but they are rarely used since they are expensive and their
maintenance requires specific skills, and (3) Stirling engines [151] 4.2.1. SOFCs
which are also expensive and have lower electricity production SOFC is characterized by the involvement of solid oxide or
than other state-of-the-art engines. Typical electricity production ceramic construction materials. It exhibits all typical benefits of
efficiencies range from about 20% for Stirling engines to 45% or fuel cells while the most significant shortcoming associated with
more for gas engines and micro-gas turbines. However, for very the high operating temperature is longer start-up time resulting in
small engines relevant to smaller distributed biogas plants poor operational flexibility. It is relatively resistant to biogas fuel
achieving greater efficiencies is a challenge [152]. CHP efficiencies impurities. For example, according to [164] a direct biogas fed
of over 80% can be achieved if heat of both the exhaust gas and SOFC operates in a stable manner and achieves complete recovery
water heated within the cylinder jacket is utilized [153,154]. Heat of cell voltage and reaction rate after stopping the H2S supply. It
is commercially exploited in district heating applications, green- suggests that a direct-biogas SOFC operated at 1000 °C is tolerant
houses applications and digestate drying to produce granulated under fueling conditions comprising up to 1 ppm of hydrogen
fertilizers. sulfide. Also Papurello et al. [165] indicated that SOFC with Ni
Recently, homogeneous charge compression ignition (HCCI) based catalyst fed with biogas after H2S removal operated with no
mode of engine operation has attracted attention in literature as sign of degradation.
an alternative biogas combustion pathway [155]. HCCI engines use Biogas dilution by air aimed at the reduction of the risk of
diluted fuel-oxidizer blends leading to the rapid combustion pro- carbon formation was proposed by Shiratori et al. [166]. SOFC fed
cess, hence the impact of CO2 contained in biogas is less pro- with air-diluted biogas operated in a stable manner without
nounced than that experienced in conventional SI engines [156]. compromising cell voltage due to the lowering of anodic
Swami Nathan et al. [157] investigated a diesel–biogas engine overvoltage.
operated in a HCCI mode and emphasized that although normally Three different biogas-fueled energy systems involving SOFC
biogas addition led to a decrease in thermal efficiencies of SI and were evaluated by Farhad et al. [167]. In each of these systems a
CI engines, in the case of HCCI thermal efficiencies close to diesel different technique was applied for conditioning the biogas fuel in
engine values were achievable (up to about 50%). Another order to prevent excessive carbon deposition. Partial oxidation was
experimental study on HCCI was [158] where again high indicated found to be the best method with the highest CHP efficiency of
1160 W.M. Budzianowski / Renewable and Sustainable Energy Reviews 54 (2016) 1148–1171

80.5%. Demonstration results for 1 kWe SOFC further ensured the A biogas fed combined heat, hydrogen and power (CHHP)
feasibility of biogas fueled SOFCs [168]. system involving MCFC was designed by Hamad et al. [180]. A
As emphasized by Lanzini and Leone [169] by enriching biogas commercial FuelCell Energy DFC1500 was selected as the MCFC.
with hydrogen superior operation of SOFC is achieved because This sustainable biogas fed system was able to provide electricity
carbon deposition at a certain threshold hydrogen content is for local use, heat for the biogas plant and hydrogen for local
completely avoided. Coupling a biogas fed SOFC and water elec- transport fleet. After further validation by experimental demon-
trolysis may enable a sustainable power system with no sign of stration the system might achieve commercialization potential.
carbon deposition. An innovative process for biogas desulfurization by adsorption
SOFC in a direct internal reforming configuration benefits from on Cu–Zn doped 13X zeolites thus enabling downstream applica-
the direct heat exchange between the exothermic electrochemical tion of MCFC was proposed by Micoli et al. [181]. Bove and Lunghi
reactions and the endothermic reforming reactions taking place in [182] successfully experimentally tested the suitability of MCFC for
one device. It may lead to the increase of the overall system effi- biogases with varying compositions. However, the commercial use
ciency and to minimization of reforming components consump- of MCFCs seems to require some further researches. Chacartegui
tion. Biogas dry reforming for SOFC with Ni/YSZ anodes was et al. [183] showed that hybrid MCFC-gas engine with CO2
demonstrated by Guerra et al. [170] and the study emphasized that sequestration by simple water condensation could achieve direct
stable conversion performance was maintained over a test period
CO2 emissions intensity of 285 gCO2/kWhe.
of 70 h. Various biogas reforming options were estimated in [171]
and the highest SOFC-based power plant efficiency of 74% was 4.2.4. MFCs
reached by involving partial oxidation reforming of biogas (biogas- The combination of the conventional AD and a microbial fuel
SOFC process). cell (MFC) allows for further innovativeness of biogas utilization.
Pressurized SOFC based power plants were claimed to offer
The niche application field for MFCs relates to diluted AD mixtures
further cost reduction benefits and a 25% reduction of thermo-
and low temperature operating conditions [184]. Ge at al. [185]
economic cost of electricity (TCOE) was obtained at 20 bar [172].
investigated long-term operation of MFC for treating primary and
digested sludge. In general, MFCs can hardly achieve attractive
4.2.2. PEMFCs
PEIO [186] and thus they require further innovative approaches
A proton exchange membrane fuel cell (PEMFC) operates at
and basic researches to shift from waste management technology
lower temperature/pressure ranges (50–100 °C) and uses a special
polymer electrolyte membrane. PEMFCs are less suitable for biogas to energy technology.
utilization because they usually require clean fuels enriched with
hydrogen. 4.3. ORCs
Biogas processing and use in PEMFCs was experimentally stu-
died by Schmersahl et al. [173]. The biogas was processed in a The integration of Organic Rankine Cycle into AD was pre-
steam reformer to produce hydrogen with purity 450% which sented in [187]. The best energetic utilization of the biogas was
was sufficient for an efficient and stable operation of the PEMFC. achieved for ORC compression ratios from 1.5 to 2 and for max-
A high temperature PEMFC (HT-PEMFC) with modular stack imum air temperatures from 335 to 340 K. In these conditions, by
design was proposed by Birth et al. [174]. Biogas underwent using a micro-ORC system (i.e. o 15 kW), it was possible to con-
treatment and reforming to yield hydrogen rich gas for down- vert about 20% of the energy content of the biogas into electrical
stream oxidation. The calculated electrical efficiency of the pro- energy. The best utilization efficiency of the energetic content of
posed HT-PEMFC was approximately 40% thus being interesting the biogas was achieved for low compression ratios and maximum
for distributed applications. exhaust air temperatures, similar to that of the aerobic process.
An oxidative reforming fuel cell (ORFC) system was disclosed in
Results showed that biogas energy could be exploited via ORC
[175] (biogas-ORFC process). In the ORFC system biogas was con-
with efficiency levels lower than conventional combustion engine.
verted to a mixture of CO2 and H2, which was separated to yield
Another ORC system for waste heat recovery from biogas
hydrogen enriched gas [176]. The hydrogen enriched gas was sent
combustion engine (biogas-ORC process) was proposed by
to a fuel cell stack, e.g. PEMFC. The ORFC cycle involved oxidative
Schuster et al. [188]. It was indicated that only 25% of heat from
reforming of biogas (requiring around 0.35 mol O2/mol CH4 for
biogas combustion was needed to heat AD and the remainder
autothermal operation without external heat source). The calcu-
could be converted to additional electricity that could increase
lated electrical efficiency of about 56% was comparable or higher
the electrical efficiency by about 2.6 basis points. The hydro-
than that of two analyzed gas turbine (GT) cycles [177]. This sys-
fluorocarbon R245fa was chosen as a working fluid. Thermal oil
tem has however low TRL and requires further research and
was heated up in a heat exchanger by flue gases that left the motor
demonstration to bring it to higher TRL and commercialize. Its
at 760 K. Economic analysis showed that electricity production
major claimed advantage is the suitability for CO2 separation to
achieve negative CO2 emission from biogas [176]. cost was about 40% of the actual German refunding of electricity
Guan et al. [178] showed that a reformed biogas fed PEMFC from biomass. However, without economic incentives ORC based
stack with a 40% of electrical efficiency integrated with CHP could biogas systems will be less economic since the capital cost of the
ensure energy self-sufficiency of a dairy farm and a biogas plant. ORC installation is very high.
Overall, ORCs can be used in AD if other uses for biogas-derived
4.2.3. MCFCs heat are not in place. However, significant investment needed,
Molten carbonate fuel cell (MCFC) is a promising power gen- compared with moderate ORC efficiencies usually lower than 20%
eration system owing to the high efficiency, low environmental [189], seem to limit their commercialization potential, at least in
impact and ability to utilize a wide variety of fuels. Due to high countries with low refunding to electricity from biogas. Never-
operating temperatures (600–700 °C) MCFC can employ catalysts theless, ORCs can be considered in larger biogas plants having
based on Ni cheaper than noble metals [179]. MCFC is able to use biogas engines where they can slightly improve overall electricity
reformed biogas, because CO also is a fuel for this type of fuel cells. production. Besides, ORCs can find application in some bior-
Nevertheless, H2S must be removed from raw biogas. efineries and industrial symbiosis systems involving AD.
 W.M. Budzianowski / Renewable and Sustainable Energy Reviews 54 (2016) 1148–1171 1161

4.4. Hybrid energy systems to demonstrate the technology in working environments and to
prove their realistic commercial potential. With the use of surplus
Hybrid energy systems can simultaneously exploit advantages wind or solar renewable energy this technology could have some
of two (or more) energy technologies. For biogas utilization SOFC- potential in the future.
GT hybrid systems have attracted attention in recent literature. A solid oxide electrolyzer cell (SOEC) configuration was pro-
SOFC ensures high utilized fuel-to-electricity conversion ratio posed for biogas upgrading [197,198]. It was suggested that the
while GT improves fuel utilization ratio and exploits thermal integration of SOEC and steam generation from the methanation
energy of flue gases derived from high temperature SOFC. could provide unique efficiency (biogas-SOEC process). High
A biogas fed SOFC-GT hybrid cycle was optimized by Facchinetti pressure steam from the methanation might be used to pre-treat
et al. [190]. The optimization results indicated the existence of the biomass feedstock for higher biogas output. SOEC has not yet
optimal designs achieving exergy efficiency higher than 65% in been demonstrated outside the lab. Electrical biogas upgrade
biogas utilization. Wongchanapai et al. [191] provided parametric might only be profitable with 48000 h of electrolysis per year
analysis of a hybrid SOFC-GT CHP system and showed feasibility of implying very little potential for load balancing. SOEC stacks had
electrical efficiencies of 55% and CHP efficiencies of more than 80%. the possibility also to operate as fuel cell stacks in a SOFC mode.
Overall, such hybrid systems although potentially can achieve This could provide an opportunity for more dynamic operation of
high electrical and CHP efficiencies are rather expensive thus not the system and hence to give the desired load balancing capability
particularly economically attractive for smaller scale biogas power of the electrical upgrade systems. The biogas-SOEC technology is
plants in distributed generation. In future hybrid systems would however found rather too expensive as of today and can only be
have to be miniaturized and made less expensive to find extended considered in countries with attractive refunding schemes to
application in biogas utilization. biogas electricity.

4.5. Biofuels from biogas conversion 4.5.2. Biosyngas and biohydrogen

Biosyngas or other biohydrogen rich gases obtained via biogas
Various biofuels can be obtained via biogas conversion. Once reforming has several potential applications including fuel cells
the associated CO2 emissions costs are included, a biofuels pro- and the production of methanol, DME or higher hydrocarbons.
duction cost can be comparable with petrol production costs However, biogas is not a perfect fuel for catalytic reforming since
[4,192]. The economic feasibility of biofuels production from bio- exotic trace contaminants can poison catalysts thus reducing
gas is therefore to large extent a policy issue. However, since overall cost-effectiveness. Deep biogas purification and/or more
biomass is a most significant cost contribution, thus when biogas robust catalysts are therefore required.
is derived from organic wastes, biogas-derived biofuels production A gliding arc reactor that combines utilization of plasma and
costs can be extremely reduced. Innovations are required at all catalysts [199] and thus could improve biogas reforming efficiency
biogas-to-biofuels stages in order to improve technological excel- was analyzed by Yang et al. [200]. By using the gliding arc process
lence and bring some of emerging concepts to sufficiently biogas was converted to hydrogen enriched gas comprising 41% of
high TRLs. hydrogen with thermal efficiency of 35%. A new spark-shade
plasma method was presented by Zhu et al. [201] where energy
4.5.1. Biomethane cost of 1.0 eV/molecule was claimed. Ni–Co catalysts are often
Biomethane or bio-synthetic natural gas (bio-SNG) is a clean recommended for biogas reforming [202,203]. In search of cata-
fuel that can be used in transport or injected into natural gas grids. lysts with less pronounced carbon deposition tendency as that of
Biogas can be upgraded to biomethane by separating CO2 or by Ni other catalysts like La-doped hydrotalcite compounds were
converting CO2 to CH4. Pressurized catalytic methanation of suggested [204]. Sulfur tolerant catalysts for biogas reforming
hydrogen enriched biogas is one of possible pathways (a Sabatier were evaluated by Saha et al. [205]. It was highlighted that a
process). Although biogas methanation is technically feasible and bimetallic catalyst in which cobalt was impregnated before nickel
might be optimized to ensure acceptable energy efficiency, some gave the best overall performance. Also an increase in a pore
other marketable fuels, especially liquid biofuels, that can be volume/surface area ratio, metal dispersion, reducibility and sup-
synthesized from biogas attract more attention from economic port basicity further improved catalyst activity.
reasons. Methanation of biogas by CO2 hydrogenation typically The process of tri-reforming [206,207] seems particularly pro-
undergoes under pressures of up to 20 bar. A heat exchanger mising for biogas, because it needs oxygen and thus could exploit
integrated with the methanation reactor enables the removal of biogas upgraded via microbiologal pathways, where some oxygen
heat of exothermic reaction. To ensure sustainability of biogas is usually found. By applying tri-reforming to biogas, oxygen
methanation, biohydrogen or hydrogen obtained from water content becomes a benefit not a problem in biomethane handling.
electrolysis by applying surplus renewable electricity (e.g. wind or Additionally, by avoiding the use of air as an oxidant, tri-reforming
solar) can be utilized [193,194]. products are beneficially not diluted with nitrogen.
A method for hydrogen based biogas upgrading (biogas-H2 Very efficient syngas/hydrogen production from biogas can be
process) was disclosed by Angelidaki et al. [195]. According with achieved via sorption enhanced reforming [208] in particular if
the invention wind surplus electricity was fed to a water electro- cheap or waste sorbents are available locally.
lyzer to produce hydrogen. In one of proposed embodiments
hydrogen was fed directly to an AD reactor and resulting methane 4.5.3. Biomethanol and bioDME
comprised very little CO2. CO2 conversion to methane led an Biomethanol (bio-MeOH) is a promising sustainable liquid
increase of pH to levels that could not be tolerated by micro- transport fuel and building block chemical for future biobased
organisms. Therefore, another claimed innovation was associated industries. Catalytic synthesis of methanol from natural gas using
with the supply of acidic organic wastes to the AD reactor in order Cu–Zn catalysts is a commercial process as well as methanol
to control pH. production from geothermal energy is also well demonstrated
Another innovative method for biogas upgrading by CO2 elec- today [209]. Catalytic conversion of biogas to liquid methanol is
trochemical conversion to mostly one or two carbon hydrocarbons however more challenging due to the presence of various trace
was proposed by Gattrell et al. [196]. The process utilized the contaminants that can poison catalysts and reduce overall pro-
copper electrode. It looks promising but more research is needed duction efficiency.
1162 W.M. Budzianowski / Renewable and Sustainable Energy Reviews 54 (2016) 1148–1171

Due to energy efficiency and economic requirements, targeted terms of reduced environmental impact, GHG emissions, resource
bio-MeOH synthesis from biogas is less attractive than co- use efficiency as well as energy efficiency.
synthesis of bio-MeOH together with other one or two carbon AD is important in recycling various wastes, including indus-
biofuels and optionally bioalcohols. Corradini and McCormick. trial wastes [215]. This feature of AD makes it suitable for imple-
[210] disclosed a process where biogas processing followed menting in industrial parks, where various stakeholders could
reforming, bio-MeOH synthesis, bio-DME synthesis, biohy- benefit from exchanging and re-using their wastes. Apart from
drocarbon fuel synthesis (optional) and fractionations (biogas- utilizing waste organic materials, AD can also use waste heat
MDH). Such an integrated process can include parallel reactions generated in other technologies and provide renewable biogas in-
that produce bio-MeOH, bio-DME and optionally higher biohy- situ, i.e. without any transmission costs.
drocarbons and thus achieve improved reaction performance in A process for biomethanation by the injection of coke oven gas
terms of reaction time, temperature and pressure. (COG) to an AD reactor enabled to achieve 98–99% CH4 in the
Olah et al. [211] proposed a bi-reforming process to yield obtained biogas [216] (COG-AD process). The employment of
metgas with a H2:CO ratio of 2:1. Metgas was suitable for the hydrogen from COG to reduce CO2 content in biogas is a very good
synthesis of methanol due to the right elemental composition. The example of synergy between the unsustainable coke industry
proposed catalyst for bi-reforming was NiO/MgO, applied pres- struggling with unwanted emissions and biobased AD technology.
sures were 5–30 atm and temperatures were 800–950 °C. This is also an excellent example of using AD for handling gaseous
emissions from conventional industries, an example that can be
4.5.4. Higher biohydrocarbons adopted widely in other industries with unwanted gaseous emis-
The production of higher biohydrocarbons requires more sions. Before extended deployment takes place, this technology
complicated processes which are usually much more energy must however address a few important issues, e.g. enhanced gas
intensive compared with processes for the production of one or solubility techniques in AD liquids without parasitic emissions
two carbon biofuels. The commercialization potential of process must be developed. Enhanced gas solubility is required because
innovations depends primarily on market issues and the avail- the productivity of biomethane in the COG-AD process is limited
ability of competitive technologies, including microbiological by the mass transfer rate of reactants from a gas to liquid phase
technologies that can efficiently and sustainably synthesize higher [217].
biofuels such as biobuthanol. In search for further examples of industrial symbiosis with
A process for AD followed by biogas reforming, methanol and biogas it was found interesting that Ellersdorfer and Weiss pro-
C2 þalcohols syntheses (biogas-C2 þA process) was invented by posed the integration of a biogas plant with a cement plant [218]
Offerman [212]. The three catalytic reactors were followed by (cement–AD). The main claimed benefits of this symbiosis is the
appropriate separators that split the obtained fuel mixture into utilization of excess thermal energy from a cement plant to heat
fractions and finally the remaining CO2, syngas and methanol digesters and the direct utilization of in-situ generated biogas as
fractions were recycled back to the relevant catalytic reactors. The CO2-neutral fuel for high temperature processes of the cement
entire system was claimed to efficiently use CO2 contained in the plant, e.g. for clinker burning. Besides, due to the symbiosis, biogas
biogas and convert it fully into liquid biofuels. This process has less plant improved its energetic performance since plant energy
requirements for reaction selectivity and thus can be operated output per unit generated biogas raised from 63% to 84%. More-
under milder temperature and pressure conditions. over, the biogas generation costs are reduced and for the inte-
Another process for higher biohydrocarbons synthesis from grated AD/cement plant with biogas production larger than 90 m3/
biogas using an Al–Co–Ni–Cr based catalyst was disclosed in [213]. h are claimed to be below the natural gas market price. The major
According with the invention biogas was fed to a first reactor advantage of this concept is enhanced energy utilization since
comprising a catalyst immersed in a liquid phase. The product gas biogas fuel is fully utilized in the cement plant while heat from the
was vaporized and drawn from the reactor, condensed, and fed to cement plant is utilized in the biogas plant. This symbiotic tech-
a second reactor from which condensate was separated as liquid nology is an excellent example of how AD can be used to green
biofuel. The non-condensable gases were recycled back to the first state-of-the-art industries. In addition, strong synergies are
reactor. Main synthesized products were paraffins (25–35%), achieved by these industries and by biogas systems.
naphthenes (58–63%) and aromatics (6–17%). Energy efficiency
issues must be however carefully addressed before upscaling this
simple two-reactor catalytic biofuel generation technology. 6. Multiple-criteria assessment of potential biogas process
CO2 contained in biogas is a suitable resource for microbial innovations
production of higher biohydrocarbons by using electric current
[214]. These kind of bioelectrocatalytic process innovations, Multiple-criteria assessment (MCA) is a sub-discipline of
although very promising, require significant fundamental resear- operations research explicitly considering multiple criteria in
ches before made suitable for the full-scale commercial production decision-making processes. Making decision requires evaluation of
of biofuels and other co-products. multiple conflicting criteria. A typical example is quality and cost,
because high quality cannot be achieved at low cost. The problem
needs to be structured and multiple criteria explicitly evaluated by
5. Potential process innovations in biogas relevant industrial providing measurable indicators thus enabling well-informed
symbiosis decisions. The difficulty associated with most MCA problems lies
in the presence of several criteria because it is unclear how
Industrial symbiosis relies on sharing services, utility, and by- important are different criteria. To address this difficulty the cur-
product resources among industries in order to improve economic rent study provides preference information based on weights
viability, efficiency, and minimize adverse environmental impacts. reflecting relative importance of different criteria.
Biogas technology is particularly suitable for creating innovations
promoting industrial symbioses at various levels from biogas 6.1. MCA of innovations in literature
production through conditioning to utilization. Industrial sym-
biosis with biogas seems to be a great opportunity to improve The critical issue in MCA is the selection of a set of criteria that
current unsustainable, energy and GHG intensive industries in represents most important qualities of innovations. Further,
 W.M. Budzianowski / Renewable and Sustainable Energy Reviews 54 (2016) 1148–1171 1163

Table 1
Summary of assessment criteria, indicators information, scores and weights.

Assessment criterion Indicator information Weight

Score

TRL TRL 1 TRL 2 TRL 3 TRL 4 TRL 5 TRL 6 TRL 7 TRL 8 TRL 9 0.2
1/9 2/9 3/9 4/9 5/9 6/9 7/9 8/9 1
CP Expert’s opinion: poor, fair, average, good, very good, excellent 0.3
0–1
EECI Expert’s opinion: poor, fair, average, good, very good, excellent 0.3
0–1
PSAP PSAP 0 PSAP 1 PSAP 2 PSAP 3 0.2
0 1/3 2/3 1
NP IF CY
1 2–5 ⩾6 o1 1-4 4–7 47 o2 2–5 5–10 410
0.1 0.2 0.3 0.1 0.2 0.3 0.4 0 0.1 0.2 0.3

measurable indicators together with appropriate weights should Overall, the sets of assessment criteria available in literature are
be defined for each criterion. from various reasons mostly unsuitable for the MCA of biogas
Literature on MCA of biogas innovations is very scarce and process innovations. Only one or two single criteria, after neces-
focused rather on the entire biogas systems than on specific pro- sary modifications, can be adopted. Therefore, this study has to
cess innovations suitable for the incorporation into these entire develop or adopt from other sources a new set of specifically
biogas systems. Two such examples are presented below. Namely, designed criteria together with relevant indicators and weights.
Abbasi and Abbasi [219] proposed six, mostly environmental,
assessment criteria: (1) fate of methane, (2) global warming 6.2. A new set of assessment criteria, indicators and weights
potential, (3) suitability of feed material, (4) anthropogenic energy designed for biogas innovations
input, (5) energy balance, and (6) potential for pollution control.
The study assessed only three biogas production systems, see MCA A new set of assessment criteria must be suitable for executing
results in their Table 3. Further, Nzila et al. [220] proposed nine the MCA of biogas process innovations, in particular for early stage
assessment criteria: environmental – (1) exergy equivalent, concepts, when scarce information is available in literature. This
(2) GHG saving, (3) cumulative energy demand; technical – study proposes four assessment criteria which aggregate addi-
(4) energy balance, (5) energy payback period, (6) operational tional 15 assessment sub-criteria.
reliability; and economic – (7) total capital investment cost, The first proposed assessment criterion is technology readiness
(8) fossil energy replacement saving, (9) direct labor (technology level (TRL). The TRL is characterized through the following set of
specific labor). The study assessed three biogas production sys- definitions:
tems described in Table 1, see MCA results in their Figures 5–8. As
abovementioned studies determine the criteria for the entire TRL 1 – basic principles observed,
biogas plants and not for specific process innovations, these cri- TRL 2 – technology concept formulated,
teria are not fully useful for evaluation of process innovations TRL 3 – experimental proof of concept,
addressed by this current study. TRL 4 – technology validated in laboratory,
Literature on the MCA of other than biogas process innovations TRL 5 – technology validated in relevant industrial environment,
is more diverse but still very few criteria can be adopted for biogas. TRL 6 – technology demonstrated in relevant industrial
Namely, Budzianowski [177] proposed 5 assessment criteria: environment,
(1) CO2 generation intensity, (2) electricity production capacity, TRL 7 – system prototype demonstration in operational
(3) cost of electricity, (4) perspectives for near-term deployment in environment,
Poland and (5) risks. The study assessed 12 low-carbon electricity TRL 8 – system complete and qualified,
production technologies in Poland, see results in Table 4 of this TRL 9 – actual system proved in operational environment. The
reference. Unfortunately, all these criteria were designed specifi- TRL of each biogas process innovation is estimated by using
cally for power technologies and thus cannot be used in an expert’s opinions and the author serves as the expert.
unmodified form for the MCA of biogas process innovations.
Carrillo-Hermosilla et al. [221] proposed eight assessment criteria: The second proposed assessment criterion is commercializa-
(1) design of component addition, (2) design of sub-system tion potential (CP). The CP aggregates six additional assessment
change, (3) design of system change, (4) user development, sub-criteria: (1) process potential, (2) technical potential, (3) eco-
(5) user acceptance, (6) change in product service deliverable, nomic potential, (4) market potential, (5) perception potential and
(7) change in product service process and (8) governance change. (6) regulatory/policy potential. The CP is estimated based on
The study assessed five different eco-innovations, see results in expert’s opinions within two groups of sub-criteria: (a) process/
their Table 1. Unfortunately, these criteria are poorly measurable, technical potential and (b) economic/market/perception/reg-
very general (product, process, management and organizational ulatory potential. The expert’s opinion is expressed as poor, fair,
innovations are all put together) and thus not very useful for the average, good, very good and excellent. The base score of 0.5 is
MCA of biogas process innovations. Dereli and Altun [222] pro- awarded for cases with one ‘average’ and one ‘good’ opinion in
posed three assessment criteria: (1) commercialization potential, (a) and (b) sub-criteria groups while for other cases additional
(2) imitation potential and (3) trendiness. The study assessed nine 70.1 point is added/subtracted for each higher/lower opinion
broad IT areas, see results in their Table 4–6 and Figure 8. The than the ‘average/good’ one. For example one ‘very good’ and one
detailed methodology to assess commercialization potential can ‘excellent’ opinion is scored 0.9.
be found in [223,224] and this important criterion after some The third developed assessment criterion is energy, environ-
necessary modifications will be adopted in this study. ment and climate impact (EECI). It aggregates nine assessment
1164 W.M. Budzianowski / Renewable and Sustainable Energy Reviews 54 (2016) 1148–1171

sub-criteria related to the performance of biogas process innova-

Total MCA
tions: (1) improved energy balance potential, (2) improved overall
energy efficiency potential [225], (3) decreased fossil fuel intensity

score

0.83

0.69

NP 2–5 IF 4–7 0.63

0.60

0.48
potential, (4) improved resource efficiency potential, (5) improved
waste management potential, (6) easily available and envir-

NP 1 IF 4–7

NP 1 IF 4–7
onmentally friendly materials requirement, (7) reduced global

PSAP (0.2)

CY 4 10
warming potential, (8) fate of methane potential, and (9) oppor-

CY o 2
CY 2–5
PSAP 3

PSAP 2
tunities for industrial symbiosis potential. The EECI is estimated

2/3
0.7

0.6

0.4
1
based on expert’s opinion within two groups of sub-criteria:
(a) energy impact and (b) environment/climate impact. Similarly,

Excellent, significant negative GHG

Very good, can use waste organic
the base score of 0.5 is awarded for cases with one ‘average’ and

Average, can exploit abandoned

Environment/climate impact

Very good, efficiently recycles

one ‘good’ opinion in (a) and (b) sub-criteria groups while for

Very good, improved biogas

other cases additional 7 0.1 point is added/subtracted for each
higher/lower opinion than the ‘average/good’ one. For example

emissions possible
one ‘poor’ and one ‘fair’ opinion translates into the score of 0.1.
The fourth proposed assessment criterion is patent status or

composition
academic performance (PSAP). For patented biogas process inno-

materials

wastes
vations the PSAP is characterized through the following set of

mines
definitions: (PSAP 0) – no patent or information is not available,
(PSAP 1) – patent application, (PSAP 2) – patent pending in one

Good, benefits from autogenerative

country, (PSAP 3) – patent pending in more than one country. In

Good, less emission and energy

Very good, no energy intensive
case there is no patent/patent application or patent information is

Very good, can be very well

unavailable the PSAP is calculated based on academic literature.

Good, no stirring required

intensive mining possible

Namely, in this case the PSAP aggregates three assessment sub-
criteria characterizing publications which describe relevant pro-
cess innovation: (1) number of publications (NP) on the potential

Energy impact

pressurization
process innovation, (2) impact factor (IF) of the best journal,

operations
integrated
EECI (0.3)
(3) number of citations per year (CY) for the best publication. The
PSAP is estimated by using patent data available in Espacenet

0.7

0.8

0.8

0.8

0.5
database or publication data available in Scopus database.
Table 1 provides indicator, scoring and weight information. The
Very good, can use various cheap wastes

Good, further demonstration needed in

proposed weights enable to reflect relative importance of different

Good, other materials than wheat Good, multi fuel production feasible

especially in industrial environment

Economic/market/perception/ reg-

Good, still pH stabilization needed Good, needs further demonstration

assessment criteria. The TRL obtains weight of 0.2 in order not to

Good, simple configuration is an

penalize too much early stage potential process innovations since
promising emerging concepts, if indeed successful, would be able
to achieve higher TRL very quickly. The CP and EESI reflect most

working environment
important qualities of innovations and thus they have the weights
ulatory potential

of 0.3. The PSAP has thus the weight of 0.2. In descriptive eva-
Multiple-criteria assessment of potential biogas process innovations in biogas production.

luation of the CP and EESI assessment criteria six quality levels are
advantage
used: poor, fair, average, good, very good and excellent.
The current study uses expert’s opinions for preliminary scor-
ing the CP and EESI assessment criteria which is the most feasible
and quickest approach at this initial evaluation stage. However, in
future works for most promising biogas process innovations some
Very good, still careful process

Good, membrane fouling still

Good, can exploit abandoned

assessment sub-criteria of the CP and EESI are planned to be

Process/technical potential

evaluated using independent tools such as numerical models of

optimization is required

straw should be tested

biogas process innovations and entire power plants [177], eco-

nomic/regulatory/policy analyses [3,226] and thermodynamic/
energy/exergy/LCA analyses [227].
problematic

Table 1 summarizes assessment criteria, indicator information,

CP (0.3)

scores and weights that will be used for the MCA of biogas process
mines

innovations in following Section 6.3.

0.8

0.6

0.6

0.6

0.6
TRL 8

TRL 6

TRL 4

TRL 2

TRL 3
(0.2)

6.3. MCA of potential biogas process innovations

TRL

8/9

6/9

4/9

2/9

3/9

The MCA results for Section 2 – biogas production, 3 – biogas

Potential biogas process

conditioning, 4 – biogas utilization and 5 – biogas industrial

symbiosis are presented in Tables 2–5, respectively. The potential
process innovations are ranked against the total MCA score. Short
innovation

comments justifying the scores are provided for the CP criterion

EMBADR

coal-AD

within (a) process/technical potential and (b) economic/market/

GICON

AHPD
Table 2

IBBB

perception/regulatory potential and for the EECI criterion within

(a) energy impact and (b) environment/climate impact.
 W.M. Budzianowski / Renewable and Sustainable Energy Reviews 54 (2016) 1148–1171 1165

Table 3
Multiple-criteria assessment of potential biogas process innovations in biogas conditioning.

Potential biogas TRL CP (0.3) EECI (0.3) PSAP Total

process (0.2) (0.2) MCA
innovation Process/technical potential Economic/marke/percep- Energy impact Environment/climate score
tion/regulatory potential impact

GPP TRL 6 Good, suitable only for Average, not suitable for Good, suitable only if Very good, can produce PSAP 3 0.69
liquified biomethane (LBM) small scale biogas upgrad- liquified biomethane is pure CO2 stream
production ing, very niche market the target
6/9 0.5 0.7 1
BABIU TRL 6 Good, simultaneously sepa- Good, uses waste sorbents Very good, favorable Very good, recycles wasteNP 2-5 IF 0.63
rates CO2 and H2S from the same plant sorption kinetics materials 1-4 CY
o2
6/9 0.6 0.8 0.4
biogas-ALG TRL 3 Good, eliminates oxygen in Average, algae farming is Good, additional energy Very good, simultaneously PSAP 3 0.63
biomethane very costly content of algal biomass removes CO2 and H2S
3/9 0.5 0.7 1

7. Conclusions In the biogas utilization category 10 potential process innova-

tions were suggested:
This review study analyzed process innovations that had
potentials to improve biogas energy technology. Four categories of  The biogas-HCCI process that benefited from rapid homo-
potential process innovations were studied: (i) biogas production, geneous combustion retaining high engine efficiencies for
(ii) biogas conditioning, (iii) biogas utilization and (iv) biogas biogas fuel comprising ballast gas (CO2) and additionally
industrial symbiosis. Further, promising biogas process innova- ultra-low NOX were achieved.
tions were evaluated within each category by applying the
 The biogas-NOX process that benefited from contacting flue
gases with liquid digestate in underground tank reactors
multiple-criteria assessment (MCA). The developed assessment
filled with packing media to increase the contact surface area.
criteria included: (1) technology readiness level (TRL), (2) com-
 Direct injection of waste or underutilized hydrogen rich gas
mercialization potential (CP), (3) energy, environment and climate
into AD resulting in complete methanation of generated
impact (EECI) and (4) patent status or academic performance biogas (biogas-H2 process).
(PSAP). Finally, the most promising potential process innovations  Energy efficient one and/or two carbon biofuel synthesis and
were presented in tabular form, scored and ranked against the separation (biogas-MDH and biogas-C2 þA processes).
total MCA score. This procedure was likely to screen biogas solu-  The biogas-SOEC process that integrated SOEC-derived
tions with potentially significant innovativeness. renewable hydrogen for thermo-catalytic biogas upgrading
In the biogas production category five potential process inno- to biomethane.
vations were found promising:  High air preheating and massive flue gas recycle to com-
pensate low methane content in biogas and achieve high
 The GICON process that exploited feedstock flexible two-stage electrical and CHP efficiencies (biogas-flameless process).
biogas production where hydrolysis percolators were followed  The biogas-SOFC process that used renewable biogas for elec-
by energy efficient methanogenesis reactors without stirring. tricity with improved catalysts suitable for hybrid systems.
 AD well integrated into a biorefinery (bioethanol, biohydrogen,  Waste heat recovery from a biogas combustion engine and
biogas) benefiting from sequential production of high-value conversion to additional electricity (biogas-ORC process).
fuels with effective recycling of wastes within the entire  Oxidative biogas reforming to yield hydrogen for a fuel cell
biorefinery (IBBB process). and a stream of pure CO2 for carbon re-use or sequestration
 The AHPD process that used self-generated high-pressure in AD (biogas-ORFC process).
reactors (up to about 20 bar) in order to reduce CO2 content in Finally, in the biogas industrial symbiosis category two
biogas, driven by higher solubility of CO2 in relation to methane. potential process innovations were found promising:
 The EMBADR process that benefited from a membrane AD
reactor with little self-generated overpressure ensuring driving  The COG-AD process that benefited from using hydrogen rich
force for permeation. Additionally biogas was bubbled through coke oven gas (COG) directly fed to AD that resulted in
the membrane surface to reduce membrane fouling. complete biomethanation of biogas. The COG-AD was an
 AD of (waste) coal, including potentials for underground example of synergy between AD and conventional emission
microbiological coal mining (coal-AD). intensive industries - steel industry.
Further, in the biogas conditioning category three potential  The cement-AD process that beneficially integrated cement
process innovations were highlighted: production with AD thus providing heat source to AD and
 Cryogenic biogas upgrading with pure CO2 stream and with using renewable biogas generated in-situ. Again, the cement-
option to liquefy resulting biomethane thus being recommended AD was an example of synergy between AD and conventional
mainly for the production of liquefied biomethane (GPP process). emission and energy intensive industry - cement industry.
 The BABIU process that benefited from using municipal solid
waste incineration bottom ash available in the same waste Thus, literature sourced biogas process innovations were
water treatment plant to upgrade and purify biogas. screened by means of specifically designed criteria. The obtained
 The biogas-ALG process that produced oxygen free bio- material highlighting 20 promising innovations can be used for
methane by recycling carbonate/bicarbonate solutions progressing biogas technology or for innovation based research
between the AD and the algal plant. projects.
 1166
Table 4
Multiple-criteria assessment of potential biogas process innovations in biogas utilization.

Potential biogas pro- TRL CP (0.3) EECI (0.3) PSAP (0.2) Total MCA
cess innovation (0.2) score
Process/technical potential Economic/market/perception/ reg- Energy impact Environment/climate impact
ulatory potential

W.M. Budzianowski / Renewable and Sustainable Energy Reviews 54 (2016) 1148–1171

Biogas-HCCI TRL 8 Very good, rapid combustion with reduced Very good, a biogas upgrading step can be Very good, higher energy conversion Very good, reduced NOX emissions NP ⩾6 0.82
impact of CO2 dilution avoided efficiency due to homogenized combustion IF 4–7
CY 5–10
8/9 0.8 0.8 0.8
Biogas-NOX TRL 6 Good, packing ensures high contact area Good, low investment and O&M costs Very good, minimal parasitic energy Good, low NOX emissions but odor PSAP 3 0.72
between digestate and flue gases requirement emissions still to be handled
6/9 0.6 0.7 1
Biogas-H2 TRL 3 Good, relatively simple solution is an Good, fuel valorization effect achieved Very good, increased energy content Very good, significant negative CO2 PSAP 3 0.69
advantage due to biogas-to-biomethane transition due to methanization of CO2 emissions feasible
3/9 0.6 0.8 1
Biogas-MDH; biogas- TRL 5 Good, expensive catalysts required; no Good, higher prices of obtained liquid Good, biogas energy storage as liquid Good, can substitute fossil fuels in PSAP 3 0.67
C2 þA need for high reaction selectivity is an fuels in comparison with biogas biofuels transport
advantage
5/9 0.6 0.6 1
Biogas-SOEC TRL 5 Good, demonstration in realistic environ- Average, expensive equipment must be Good, can be enhanced by use of Good, minimal environmental PSAP 3 0.64
ments required involved surplus renewable electricity impacts is expected
5/9 0.5 0.6 1
Biogas-flameless TRL 6 Good, no temperature peaks in a combus- Average, more expensive infrastructure Good, effective recirculation of flue Good, low NOX and PAHs emissions NP ⩾6 0.62
tion chamber needed than in conventional combustion gas energy IF 4–7
CY 5–10
6/9 0.5 0.6 0.8
Biogas-SOFC TRL 6 Good, requires biogas cleaning to protect Good, suitable for small scale distributed Good, can achieve high electrical Average, emissions evaluation in NP ⩾6 0.62
catalyst damage; fuel utilization ratio must generation systems efficiencies LCA perspective needed IF 4–7
be kept high
6/9 0.6 0.5 CY 5–10
0.8
Biogas-ORC TRL 7 Good, only proven technologies required to Average, high investment cost required Good, ORC coupled to an engine Average, emissions evaluation in NP 1 0.58
operate biogas-ORC thus the solution is less suitable for increases electricity production LCA perspective needed IF 1–4
developing countries CY 410
7/9 0.5 0.5 0.6
Biogas-ORFC TRL 2 Good, demonstration in working environ- Good, techno-economic evaluation Good, has potentials for high elec- Very good, significant negative CO2 PSAP 2 0.57
ment needed needed trical efficiencies with reduced CO2 emissions feasible
emissions
2/9 0.6 0.7 2/3
 W.M. Budzianowski / Renewable and Sustainable Energy Reviews 54 (2016) 1148–1171 1167

Table 5
Multiple-criteria assessment of potential biogas process innovations in biogas industrial symbiosis.

Potential biogas TRL CP (0.3) EECI (0.3) PSAP Total

process (0.2) (0.2) MCA
innovation Process/technical potential Economic/market/perception/ Energy impact Environment/climate score
regulatory potential impact

COG-AD TRL 6 Very good, techniques for Very good, exploits coke oven gas Good, energy bal- Very good, but possible NP 1 0.70
enhanced gas (COþ H2) solu- and minimizes biogas upgrading ance to be clarified parasitic emissions from AD IF 4–
bility in fermentative liquid costs especially in LCA need clarification 7
required CY 5–
10
6/9 0.8 0.7 0.6
cement-AD TRL 6 Very good, demonstration Very good, many synergistic Very good, utilizes Good, ensures CO2 neutral NP 1 0.66
project required to confirm economic benefits, e.g. improved waste heat from fuel produced in-situ for IF 4–
expected significant energy heat management, sustainable cement production cement manufacturing 7
benefits fuel produced in-situ CY
o2
6/9 0.8 0.7 0.4

8. Future research and development addition new biogas utilization methods such as (i) biomethane
(CO2 separation and electrocatalytic hydrogenation), (ii) biogas
Innovations are required in biogas production, conditioning physical and chemical liquefaction, and (iii) alternative uses (bot-
and utilization. Great potentials for innovations lie also in indus- tling, grid injection, etc.) should receive attention.
trial symbiosis between AD based systems and conventional Within the fourth biogas industrial symbiosis category the
resource intensive industries. Research and development (R&D) integration of AD with conventional emissions/energy intensive
efforts should be primarily directed toward areas where disruptive industries seems extremely promising. Biogas plants can use waste
innovations could be generated relatively quickly. heat and waste materials while providing clean fuel in-situ. Fur-
As regards to the reviewed biogas production category R&D ther, well designed industrial parks with comprehensively defined
needs to relate to novel feedstocks, biomass conversion routes and waste materials recycling and clearly defined economics should
AD products. R&D in the area of novel feedstocks is needed within: receive attention. Greater drop-in of other than biogas renewable
(i) short rotation digestible plants, (ii) aquaculture, (iii) feedstock energy (e.g. surplus renewable electricity) should be admitted and
design (cell wall composition, genetic engineering), and (iv) integrated with biogas to achieve greater sustainability of such
wastes and residues (agriculture, processing bioindustry, MSW). multi-source renewable energy systems.
R&D in the area of novel biomass conversion routes is needed for: Policy options will also be essential because they could shape
(i) two or multi-stage fermentation, (ii) biomass pretreatment and directions of innovativeness in biogas technology. For example in
(iii) sustainable catalytic routes. R&D in novel AD products should countries with high subsidies to biogas energies, innovations may
relate to: (i) biofertilizers. include advanced and expensive technological options. In contrast
Disruptive innovations might be associated with genetic engi- countries having minimal or no subsidies to biogas require only
neering, e.g. genetically modified microbes and potentially short inexpensive and thus very affordable innovations. With decreasing
rotation digestible plants. Potential lies also with dedicated pre- economic incentivization expensive solutions need to be replaced
treatment methods, enhanced reactor configurations and inte- by more cost-effective ones. In addition, economic incentives
grated agriculture based systems. Highly integrated biorefineries shape directions of technology evolution. For example, as long as
able to produce transport fuels, biobased chemicals and other incentive relate only to power generation, mainly power tech-
biobased materials from locally available versatile resources where nology related innovations, such as engine related, are developed.
AD can play roles in waste management and sustainable energy In case biomethane generation is supported, also biomethanation
supply is one another area for disruptive innovations. The ability of related innovations, such as associated with biogas upgrading, are
AD to utilize waste CO2 and surplus renewable electricity is also a more likely to develop. Consequently, relevant policies need to be
new emerging option able to generate further innovations. in place before biogas technology is selected to play a significant
As regards to the second biogas conditioning category biogas role in the economy of any country.
upgrading techniques using CO2 removal via more energy efficient
pathways should be investigated. Waste and locally available
materials should be extensively used as sorbents for biogas com- Acknowledgments
ponents. Biomethanation through microbial electrocatalytic routes
involving surplus renewable electricity should also obtain atten- This study has been financially supported by National Science
tion. Also more focus on the utilization of separated CO2 in agri- Centre (Poland) under the project “Innovative process- and
culture (applications in controlled ripening of fruits and vege- system-level research for expansion of biogas energy in Poland”,
tables, greenhouses etc.) and in algal biomass growth enhance- No. DEC-2012/07/B/ST803334.
ment should be achieved.
In the third biogas utilization category fuel cells (in particular
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