Energy Conversion and Management 324 (2025) 119294

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Energy Conversion and Management

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

Municipal solid waste thermochemical conversion to substitute natural gas:

Comparative techno-economic analysis between updraft gasification and
chemical looping
Orlando Palone *, Luca Cedola , Franco Rispoli , Domenico Borello
Department of Mechanical and Aerospace Engineering, Sapienza University of Rome, Via Eudossiana 18, Rome 00184, Italy

A R T I C L E I N F O A B S T R A C T

Keywords: A comparative techno-economic analysis has been performed on two innovative pathways for municipal solid
Chemical looping hydrogen production waste (100 t/h) thermochemical processing to substitute natural gas. The first pathway is based on updraft
Municipal solid waste gasification with bottom hydrogen oxy-combustion and ashes melting, the second on autothermal chemical
Substitute natural gas (SNG)
looping hydrogen production with Fe2O3/SiC oxygen carrier. Catalytic methanation in a series of adiabatic fixed
Techno-economic analysis
Updraft gasification
bed reactors has been implemented and substitute natural gas quality has been evaluated based on the Italian
Waste-to-fuel legislation. Although the updraft gasification process shows higher substitute natural gas productivity (16.3 t/h
vs 13.7 t/h), better system energy efficiency (42 % vs 35 %) and energy intensity (125 vs 141 GJ/t), the levelized
cost of substitute natural gas is more competitive in the chemical looping configuration due to the lower capital
expenditure. Product prices of 2.26 €/kg and 1.76 €/kg have been calculated for updraft gasification and
chemical looping, respectively, assuming 8 % discount rate, 80 % capacity factor, and 90 €/MWh electricity cost.
Sensitivity analyses indicate that, among other parameters, the plant capacity factor and the electric power cost
have a relevant impact on the final product cost. Additionally, both pathways are shown to be economically
competitive with substitute natural gas production from H2O electrolysis and CO2 capture/purchase. Finally,
actions to reach competitivity with fossil natural gas for industrial uses are qualitatively discussed.

[4]. In this sense, methane (or more generally substitute natural gas) is
an optimal energy vector, given the variety of long-term industrial ap­
1. Introduction
plications in the chemical and power productions sector and the pres­
ence of a fully developed transport technology (in either gas or liquid
The world population is growing continuously and from todays’ 8.2
phase) [5].
billion people it is expected to increase up to 10.2 billion people by the
Presently, around 44 % of global waste is sent to landfill, while only
end of the century [1]. Among the numerous consequences of this pro­
the 11 % is incinerated with subsequent power production [6]. Ther­
cess, the global energy demand growth has been progressing at an
mochemical routes that can be used to reconvert solid waste to an en­
average of 1–2 % per year and should reach 18.9 billion TOE (tonnes oil
ergy resource are represented by incineration, hydrothermal
equivalent) by 2040 [2]. In an increasingly energy-dependent society,
liquefaction, hydrothermal carbonization, pyrolysis, gasification,
fossil fuels consumption will be dominant and will cause the continuous
chemical looping etc. Waste incineration is a waste to energy solution
CO2 accumulation in the atmosphere with global temperatures rise. At
where wastes are burnt at high temperature conditions and superheated
the same time, the world population growth will intensify the total solid
steam is produced by heat exchange with the flue gases [7]. Drawbacks
waste production, estimated to 2.1 billion tonnes in 2023 and predicted
of this pathway are represented by significant emissions due to incom­
to reach 3.8 billion tonnes in 2050 [3], thus exacerbating the challenge
plete combustion and competitive costs of power production from other
of identifying efficient and large-scale waste disposal technologies.
sources [6]. Example of flue gas pollutants are nitrogen oxides (NOx),
Municipal solid waste (MSW) reconversion to an energy carrier, i.e. the
carbon monoxide (CO), sulphur dioxide (SO2), hydrogen chloride (HCl),
Waste-to-Fuel concept, is a promising pathway to efficiently dispose of
hydrogen fluorides (HF), particulate matter (PM), and multiple heavy
waste and, if supported by low-carbon power supply and carbon capture
metals [8].
technologies, to produce decarbonized fuels or process intermediates

* Corresponding author.
E-mail address: [email protected] (O. Palone).

https://doi.org/10.1016/j.enconman.2024.119294
Received 21 September 2024; Received in revised form 11 November 2024; Accepted 15 November 2024
Available online 22 November 2024
0196-8904/© 2024 The Author(s). Published by Elsevier Ltd. This is an open access article under the CC BY license (http://creativecommons.org/licenses/by/4.0/).
O. Palone et al. Energy Conversion and Management 324 (2025) 119294

process involves endothermic and exothermic reactions, it is also

Nomenclature possible to tune the flow rates of solid and gases for (at least partially)
autothermal operation [17]. Main practical challenges are represented
AR Air Reactor by the limited experimental activity recorded on large sizes (> MWth)
ASU Air Separation Unit plants, which translates into approximations relating to process effi­
BEC Bare Erected Cost ciency, i.e. syngas production efficiency, and the long-term performance
CL-SNG Chemical looping − Substitute natural gas of the oxygen carrier, especially when complex feedstock such as MSW
CEPCI Chemical Engineering Plant Cost Index are involved. For instance, the latter can be influenced by mechanical (e.
FR Fuel Reactor g. attrition with fines formation), thermal (e.g. high temperature), and
FGD Flue Gas Desulphurisation chemical (e.g. contamination by heavy metals) stresses. In turn, this
G-SNG Gasification − Substitute natural gas impacts the process efficiency and the plant capacity factor, which are
HHV Heating Value crucial parameters to establish competitivity with alternative pathways.
LCOSNG Levelized Cost of SNG Considering the large availability of waste-to-fuel processes pro­
MSW Municipal Solid Waste posed in the literature, it is of interest to identify strengths and weak­
PSA Pressure Swing Adsorption nesses of different technological pathways under similar techno-
SNG Substitute natural gas economic assumptions. The critical discussion of benefits and draw­
SR Steam Reactor backs of several processes proposed in the literature is hindered by
TOC Total Overnight Cost differences in the initial conditions and assumptions. Therefore, in this
TASC Total As Spent Cost work a comparative energy and economic analysis has been undertaken
WGS Water Gas Shift between updraft gasification and chemical looping hydrogen production
as promising thermochemical pathways for municipal solid waste con­
version and valorization to substitute natural gas (SNG). Given the
increasing penetration of intermittent energy sources, the interest in
Gasification consists in the partial oxidation of a solid fuel, e.g. coal, waste reconversion is transitioning from power production (e.g. waste
biomass or solid waste, and is an endothermic process that takes place by incinerators) to the production of versatile energy carriers, such as
exposing the feedstock to an oxidizing agent, i.e. air, steam or oxygen, at synthetic methane, which can be exploited in case of low renewable
relatively high temperatures (800–900 ◦ C) [9]. The product is a mixture power availability and enforce the national energy security. Therefore,
of CH4, H2, CO and CO2 (N2 for air oxidation) with a series of contam­ this work contributes to identify the missing research questions to
inants such as particulate matter, tar, alkali compounds, sulphur com­ improve the key performance parameters of each scheme and hence
pounds, nitrogen compounds, and others [6]. The main advantage of competitivity with the fossil natural gas (NG) alternative.
this technology is that syngas composition can be adjusted by adapting
the oxidizing agent composition and flow rate. On the contrary, main 2. Method
challenges are represented by tar production, which requires additional
cracking units [10], and the relatively low H2 content in the products (< A comparative techno-economic analysis has been performed on two
60 % mol), which involves further downstream processing steps for H2 waste-to-fuel systems aiming at substitute natural gas production from
intensification and purification [11]. Different gasification reactors can municipal solid waste (MSW) thermochemical processing by using
be grouped into several categories: fixed bed, fluidized bed, entrained Aspen Plus software. A simplified scheme of the two described processes
bed, etc. Additionally, fixed bed gasifiers can be further divided into for SNG production, gasification (G-SNG) and chemical looping (CL-
updraft and downdraft according to the syngas flow direction. Updraft SNG) is given in Fig. 1.
gasifier have only been demonstrated over a limited range of conditions The G-SNG configuration (Fig. 1-a) is based on a fixed bed updraft
since they are affected by significant tar production (up to 200 g/Nm3) gasification and involves the following sections:
and unconverted char [12], which involve a specifically developed pu­
rification section. However, their main benefit is the ability to handle (1) updraft gasification of MSW with ashes melting and downstream
extremely inhomogeneous feedstocks, such as MSW [12]. catalytic tar cracking;
Chemical looping is a thermochemical process based on gas–solid (2) cleaning and purification of the syngas from gaseous and solid
reactions between a solid material, generally a metal oxide (known as contaminants;
the oxygen carrier) and the reactants stream. In chemical looping (3) intensification of the H2 content through water gas shift and
combustion, the fuel is oxidized by the interaction with the oxygen pressure swing adsorption;
carrier, which is then regenerated by a highly exothermic process (4) permanent storage of part of the CO2;
through air oxidation. In this way, the CO2 content in the combustion (5) power production by heat recovery from the tail gases oxy-
gases from the reduction step are intrinsically separated from the N2 combustion;
content of air without any complex separation step [13]. By adjusting (6) catalytic methanation of H2 and CO2.
the fuel to oxygen carrier ratio, chemical looping can also be used to
produce a syngas. In chemical looping reforming, the reduction step The CL-SNG configuration (Fig. 1-b) is based on a three-reactors
involves the partial oxidation of the fuel by the oxidation agent (H2O or chemical looping process and involves the following sections:
CO2) and by gas–solid reaction with the oxygen carrier [14]. In another
variant involving iron oxides as the oxygen carrier, known as chemical (1) three-reactors chemical looping cycle with Fe2O3/SiC oxygen
looping hydrogen production, the process is split in three steps: the fuel carrier producing high-purity H2;
is fully oxidized by the oxygen carrier, then the oxygen carrier is (2) power production by heat recovery in a boiler with three pressure
partially oxidized by H2O producing H2, and eventually the initial ox­ levels;
ygen carrier phase is completely regenerated by air oxidation [15]. The (3) cleaning and purification of the syngas from gaseous and solid
air coming from the last step, which has been deprived of part of its O2 contaminants;
content, evolves in gas turbines if the process is operated at high pres­ (4) permanent storage of part of the CO2;
sure conditions or can be used for high pressure steam production by (5) catalytic methanation of the CO2 from the fuel reactor and of the
heat recovery [16]. In this way, high purity H2 is produced without H2 from the steam reactor.
requiring any downstream separation process. Moreover, given that the

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O. Palone et al. Energy Conversion and Management 324 (2025) 119294

Fig. 1. Process flowsheet of: (a) the G-SNG plant, (b) the CL-SNG plant.

The Peng-Robinson state equation with the Boston-Mathias correc­ 2.1. Updraft gasification of the MSW
tion has been used to calculate the thermodynamic properties of the
conventional components in both plants. The Aspen Plus flowsheet of the updraft gasification section is given
in Fig. 2 and follows the modelling approach presented in Ref. [18].
In the Aspen Plus model, the updraft steam gasification reactor has
been divided in four regions to optimally simulate the reaction steps

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O. Palone et al. Energy Conversion and Management 324 (2025) 119294

Fig. 2. Aspen Plus flowsheet of the updraft gasification reactor including drying zone, decomposition zone, gasification zone, and oxy-combustion in the bottom
region. More details on the tar cracking section are shown in subsequent process flowsheets.

preliminarily separated from the gasification reactor by the CHARSEP

Table 1
separator block as unconverted carbon. In the actual process, most of the
Proximate and ultimate analysis of the MSW [18].
unconverted carbon reaches the combustion zone to react with the
Proximate analysis (wt %) Value oxidizing agent, high purity O2 in this case, and provide heat to the
Water content (wet basis) 6.37 reactor itself.
Ash (dry basis) 13.33 The volatiles released from pyrolysis are sent to the steam gasifica­
Volatile (dry basis) 76.34
tion section, which has been modelled as a series of two RGibbs blocks
Fixed carbon (dry basis) 10.33
Ultimate analysis (dry basis wt%) ​ (GASIFY AND GASIFY2), both operating at 900 ◦ C and 1 atm. Steam is
C 41.03 injected at 150 ◦ C and 1 atm and it is produced through thermal re­
H 5.86 covery from the hot gases in the plant. Since the oxy-combustion of H2 in
O 38.22 the melting zone generates H2O, an additional Calculator block has been
N 0.14
S 1.42
included to adapt the amount of external process water needed to reach
a steam to carbon (S/C) ratio of 2.4 [20]. This S/C ratio has been
selected in agreement with the experimental data used for model
occurring along the height of the reactor: (1) biomass drying (DRYER), validation.
(2) pyrolysis (DECOMP), (3) steam gasification (GASIFY + GASIFY2), The syngas from the first Gibbs reactor (GASIFY) is introduced into a
(4) ash melting (MELT). second Gibbs reactor (GASIFY2) to adjust the final syngas composition
The feed rate of raw MSW has been set at 100 t/h and 25 ◦ C, and the and align it with the experimental data. In general, a single RGibbs
reactor operated at atmospheric pressure. The MSW proximate and ul­ reactor (with chemical and physical equilibrium conditions) over­
timate analyses implemented in the model are shown in Table 1. estimates the CO concentration in the syngas and underestimates the
After a pre-treatment based on milling, drying, and pelletizing (not CH4. Hence, in GASIFY2 the Aspen Plus Restricted Equilibrium Method
included in the Aspen Plus simulation), the MSW undergoes further has been imposed on the reactions reported in Eqs. (1) to (5):
drying in the reactor by heat exchange with the rising syngas. This has
C + O2 = CO2 (ΔH298K = − 394 kJ/mol) (1)
been simulated with a RStoic block (DRYER) at 470 ◦ C and 1 atm. The
conversion fraction has been determined assuming a moisture reduction
C + CO2 = 2CO (ΔH298K = +172 kJ/mol) (2)
from 6.4 % to 5 % wt.
A RYield block (DECOMP) has been implemented to model the C + H2 O = CO + H2 (ΔH298K = + 131 kJ/mol) (3)
thermal decomposition of the feedstock at around 600 ◦ C and 1 atm. In
this step, char, tar and volatile matters are released from the feedstock, CO + H2 O = CO2 + H2 (ΔH298K = − 41 kJ/mol) (4)
as shown for instance in Ref. [19] for polypropylene decomposition. For
simplicity in this model the feedstock is split into its constituent ele­ CO + 3H2 = CH4 + H2 O (ΔH298K = − 206 kJ/mol) (5)
ments, i.e. C, H, O, N, S, Cl, and ash. In the gasification process not all the
pyrolysis char is converted into syngas due to the limited contact time To fit the experimental data, the temperature differences from the
with the gasification agents or the uneven temperature distribution in imposed 900 ◦ C have been set to − 40 and − 220 ◦ C for reactions R4 and
the reactor. Therefore, part of the produced char (2 % in wt [18]) is R5, respectively.

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O. Palone et al. Energy Conversion and Management 324 (2025) 119294

Table 2 A summary of the main operating parameters of the gasification

Main parameters of the steam gasification section. section is given in Table 2.
Unit Values Block

Inlet 25 C, 1 atm
◦
​ 2.2. Gas cleaning and purification in G-SNG
Drying 470 ◦ C, 1 atm RStoic
Pyrolysis 600 ◦ C, 1 atm RYield The Aspen Plus flowsheet of the syngas cleaning zone is shown in
Gasification 900 ◦ C, 1 atm 2 RGibbs
Fig. 3 and is based on the scheme presented in Ref. [22].
Tar reforming 900 ◦ C, 1 atm Heater
Oxy-combustion 1400 ◦ C, 1 atm RGibbs After heat recovery from the hot syngas in a Rankine cycle, a cooler
separates the water content in the syngas before entering the particulate
removal zone (PM-REM), which is based on a baghouse filter. The par­
2.1.1. Tar reforming/cracking ticulate removal block (PM-REM) operates at 130 ◦ C and it is designed to
To simulate the upward rise of the syngas exiting the gasifier, the remove solid impurities in the syngas, which is crucial to protect the
syngas is finally injected into the DRYER block. Since the experimental subsequent reactors from erosion and friction losses [23]. As in
syngas composition used for model validation includes downstream tar Ref. [22], this section is simulated with a pressure drop valve to indicate
cracking after the fixed bed reactor [20], in this model the raw syngas at the pressure drop that would occur in this block. Subsequently, the
the outlet of the updraft gasifier (which is already characterized by a tar- stream is heated to 220 ◦ C by heat exchange with the purified gases and
free molar composition due to the modelling approach) is heated to sent to the hydrolysis reactor (HYD-REAC), where COS and HCN are
900 ◦ C by tail gases oxy-combustion to reproduce the presence of the tar removed according to the reactions in Eqs. (7) and (8):
cracking reactor. In this way, the outlet conditions (900 ◦ C and 1 atm)
from the tar cracking reactor are correctly reproduced. Model validation COS + H2 O→H2 S + CO2 (7)
is presented in the Figures S1 to S4 of the Supplementary Material and is
HCN + H2 O→NH3 + CO (8)
based on the experimental results in Ref. [20].
The reactor is modelled as a separator block with 99 % COS and HCN
2.1.2. Ashes melting and oxy-combustion separation efficiency from the syngas [24]. In this case, products for­
After gasification, the ashes are totally separated from the gases by a mation from the cleaning reactions and water consumption have been
cyclone and sent for melting to the MELT block. In the melting zone, neglected. Removal of mercury (HG-REM) is also simulated at 180 ◦ C by
preheated H2, O2 and the unconverted char are injected into a RGibbs a pressure valve representative of the pressure drop occurring in this
block, where oxy-combustion increases the temperature above the ash section, although the Hg concentration has not been included in the
melting temperature. Since the melting point of MSW ashes is around adopted modelling approach. Subsequently, the syngas evolves in the
1300 ◦ C [21], the melting block temperature has been set at 1400 ◦ C. H2S purification section, which is based on two successive steps. The
The flow rate of H2 directed to the melting zone of the steam gasifier, first step is the Lo-Cat process from Merichem [25], a reliable method
which is extracted from the pressure swing adsorption (PSA), is set via a that employs a chelated iron oxide solution to convert H2S into low-
Design Spec imposing the following energy balance in the gasifier: value sulphur [26]. By means of this technology the H2S concentration
QTOT = QMelt + QDrying + QDecomp + QGASIFY + QGASIFY2 = 0 (6) can be reduced below 10 ppmv [27] at atmospheric pressure according
to Eq. (9), while the iron solution is regenerated by air oxidation ac­
Where QMelt , QDrying , QDecomp , QGASIFY , and QGASIFY2 represent the heat cording to Eq. (10):
duties released in the melting zone, and absorbed in the drying, pyrol­
H2 S + FeO→FeS + H2 O (9)
ysis, and gasification zones of the reactor, respectively. If the H2 flow
rate required to meet 1400 ◦ C in the melting zone is lower than the 2FeS + O2 →2FeO + 2S (10)
amount generated, autothermal operation is met, otherwise an external
energy input is required. The stoichiometric flow rate of O2 is set by a To further drop the H2S concentration in the syngas a second step based
Calculator block according to the molar flow rate of H2 and char in the on a ZnO guard bed has been considered, according to the reaction in Eq.
melting zone. This is supplied by an air separation unit (ASU) that has (11). This process ensures total removal of residual H2S to concentra­
not been simulated but has been included in the economic analysis. tions below 1 ppmv [27] and for simplicity a 99 % separation factor has

Fig. 3. Aspen Plus flowsheet of the gas cleaning and H2 intensification sections for G-SNG.

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O. Palone et al. Energy Conversion and Management 324 (2025) 119294

Table 3 2.3. H2 intensification and CO2 storage

Summary of the operating conditions and separation factors of the cleaning
section. After the cleaning section, the H2 concentration in the syngas is
Unit Operating Removal Ref. intensified by water gas shift (WGS) reactors and then separated by PSA.
conditions efficiency Two equilibrium adiabatic reactors operating at atmospheric pres­
Particulate removal 130 ◦ C, 1 atm ​ [23] sure simulate the WGS process. The syngas is preheated (HE5 in Fig. 3)
Flue gas desulphurization 50◦ C, 1 atm 0.95 SO2 [24] to 450 ◦ C and mixed with heat recovery steam from the STEMAWGS
Hydrolysis reactor 220 ◦ C, 1 atm 0.99 COS, 0.99 [24] stream before entering the high-temperature WGS reactor (HT-WGS in
HCN
Fig. 3). The low-temperature WGS reactor is adiabatic and operates with
Hg removal 180 ◦ C, 1 atm Assumed1 [22]
Lo-Cat 40 ◦ C, 1 atm See DEEP-H2S [26,27] an inlet syngas temperature of 200 ◦ C (LT-WGS in Fig. 3) for high CO
ZnO guard bed 370 ◦ C, 1 atm 0.99 H2S2 [27] conversion efficiency. Since the WGS reaction is exothermic, the energy
Selective Catalytic 370 ◦ C, 1 atm 0.85 NO, NO2 [28] generated during the reaction can be partially recovered for steam
Removal production, which is exploited in the steam gasification block (WATER
1
No Hg is present in the gas stream due to model simplification in Fig. 3). After the WGS section, the syngas contains mainly H2 and CO2
2
Combined H2S removal efficiency of the Lo-Cat and subsequent ZnO bed has (traces of CO and other gases) and is compressed in a multi-stage inter-
been assumed unitary for simplicity. refrigerated compressor to 23 bar.
The PSA unit is simulated in a simplified way using a separator (PSA
been set in the DEEP-H2S separator accounting for both the Lo-Cat in Fig. 4) with an H2 separation rate of 87 % [29]. The separated H2 is
process and the ZnO bed. then split into two streams: one is sent to the melting zone of the gasifier
for oxy-combustion, the rest, which is already at high pressure condi­
H2 S + ZnO→ZnS + H2 O (11)
tions, is sent to methanation. The tail gases (CO2-GA in Fig. 4) from PSA
cannot be directly sent to permanent storage due to the residual content
In the subsequent economic analysis, the Lo-Cat capital and operating
of CO and H2, and are fully burned with pure O2 in a dedicated
expenditures have been calculated by linearly scaling and the additional
combustor (BURNER in Fig. 4). The hot gases are then sent to heat ex­
H2S produced by HCN and COS removal has been included in the cost
change (HE10) with the raw syngas stream before the tar cracking
scaling.
reactor (TARCRACK in Fig. 4). After tar cracking, heat recovery from the
The syngas at this point has been purified from harmful compounds,
syngas has been included based on a simplified Rankine cycle (PUMP,
especially sulphur-based contaminants that may compromise the cata­
BOILER, T1 and COND in Fig. 4).
lysts of the subsequent reaction sections. Although the blocks in the
After water separation, the resulting stream with high purity CO2 is
cleaning zone have been modelled in a simplified manner, in the eco­
partly sent to methanation according to a H2/CO2 molar ratio of 4, and
nomic analysis the catalysts and chemicals consumption of the cleaning
the rest to permanent storage. The compression unit consists of a
section have been appropriately evaluated.
multistage compression to 83 bars [30].
A summary of the removal efficiencies assumed in each block of the
A summary of the main operating parameters of this section is given
two plants is given in Table 3.
in Table 4.

Fig. 4. Aspen Plus flowsheet of the PSA tail gases oxy-combustion, the CO2 compression section, and the heat recovery section in the G-SNG configuration

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O. Palone et al. Energy Conversion and Management 324 (2025) 119294

Table 4 gases are recirculated with a recirculation factor of 0.7. After the reac­
Main operating parameters of the H2 intensification and separation section. tion section, the wet SNG is cooled to 42 ◦ C (SG-LP1) before passing into
Unit Values Block a flash drum for water removal. The resulting outlet temperatures of the
four reactors have been checked to be within the range for safe catalyst
HT-WGS Adiabatic, 1 atm RGibbs
Intercooler 200 ◦ C (syngas), 1 atm HeatX operation, while the reactor pressure is set at 20 bar because high
LT-WGS Adiabatic, 1 atm HeatX pressure conditions promote the conversion to CH4 according to ther­
Condenser (after LT- 40 ◦ C, 1 atm HeatX modynamics [31]. For simplicity, the pressure losses occurring in the
WGS) methanation reactors have been neglected, but a recirculation
PSA compressor 30 ◦ C, 23 bar (outlet) 2 Comps, Flash and
Cooler
compressor (MC) has been included to provide a slight overpressure to
PSA adsorption vessel 30 ◦ C, 2.3 bar − tail gases, 23 bar Sep the flow and promote its recirculation into the first reactor (MR1).
− H2 Although no reaction kinetics has been implemented in the final
CO2 compressor 30 ◦ C, 83 bar (outlet) 3 Comps, Flash and simulation, a conventional Ni/Al2O3-based catalyst is assumed due to its
Cooler
high activity, good selectivity towards CH4, and moderate material cost.
Tail gases combustor Adiabatic, 1 atm RGibbs
Syngas fired heater 1 900 ◦ C (syngas), 1 atm HeatX After water removal, the SNG stream is treated in a dehydration
Rankine Cycle 40 bar, 61.2 t/h H2O ​ More blocks membrane which is modelled by a separator block (DEHYD-ME in Fig. 5)
Rankine Cycle – boiler 470 ◦ C (syngas), 1 atm ​ HeatX with a capture efficiency of 90 % [31]. Once the water content has been
Compressors 85 % isentropic, 95 % ​ MComp removed, the SNG stream is compressed in a two-stage inter refrigerated
mechanical
Pump (MP) 75 %-83 % efficiency, 95 % ​ Pump
compressor (35 ◦ C outlet temperature) to the grid pressure of 60 bar. The
driver heat removed from the streams leaving the methanation reactors is
Steam Turbine (MP) 92 % isentropic, 95 % ​ Comp effectively recovered through a two-stage pressure steam generation
mechanical system. This system comprises a low-pressure line at 3 bar (LP-STEAM in
1
The syngas is heated to 900 ◦ C before the tar cracking reactor. Fig. 5) and a high-pressure line at 42 bar (HP-STEAM in Fig. 5). The
steam produced is then expanded in two steam turbines, one for low
2.4. Methanation section in G-SNG pressure (LP-T in Fig. 5) and one for high pressure (HP-T in Fig. 5).
To assess the suitability of the produced SNG for transport into the
The CO2 stream from the gasification plant is first compressed in a gas grid, the Higher Heating Value (HHV), the Wobbe Index, and the Gas
two-stages inter-refrigerated compressor to 20 bar and then mixed with Gravity (evaluated at 15 ◦ C), has been computed and compared with the
the H2 stream from the PSA at 35 ◦ C and 20 bar. values indicated by the Italian legislation.
According to the plant layout shown in Fig. 5, the methanation HHV
section consists of the following main units: WOBBE = (13)
√GG

(1) a heat exchanger (PRE-H) to preheat the feed gases with the GG = ρSNG /ρair (14)
product gases from the first reactor;
(2) four adiabatic reactors (MR 1,2,3 and 4) in series with interme­ Where ρSNG and ρair stand for the SNG and air densities at 15 ◦ C. The
diate gas cooling at 250 ◦ C; HHV has been extracted from Aspen Plus results.
(3) a flash drum for water removal from the SNG; A summary of the main operating parameters of the methanation
(4) a two-stages inter-refrigerated (35 ◦ C) compressor to reach 35 section is given in Table S1 of the Supplementary Material.
bar, which is the operating condition for membrane adsorption of
the residual H2O content;
2.5. Chemical looping hydrogen production plant
(5) a two-stages inter-refrigerated (35 ◦ C) compressor to reach 60 bar
and be injected into the gas grid.
The selected oxygen carrier is composed of 66.2 % wt of Fe2O3 and
33.8 % wt of SiC for thermal support. The mass flow of the oxygen
The methanation reactor has been modelled assuming chemical
carrier is set at approximately 1.26 kt/h, so that the mass ratio between
equilibrium and adiabatic conditions. The use of RGibbs blocks is suit­
OC and input MSW (0.1 kt/h) is 12. This threshold has been set to ensure
able to model the methanation reactors, since in the experimental
that the model is capable of correctly reproducing the experimental data
practice the gases at the outlet of each reaction step reach full chemical
used in the validation [33]. The reaction pathway expected in the
equilibrium [31,32]. Four RGibbs in series reach suitable SNG compo­
chemical looping process is given in Table 5.
sitions by means of the CO2 hydrogenation reaction in Eq. (12):
CO2 + 4H2 →CH4 + 2H2 O (12) 2.5.1. Fuel reactor modelling
The fuel reactor (FR) and steam reactor (SR) have been modelled as
To limit the temperature rise in the first catalytic bed (MR1) the product counter current moving bed reactors given the higher gas–solid contact

Fig. 5. Aspen Plus flowsheet of the methanation section based on the TREMP process by Tospoe.

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O. Palone et al. Energy Conversion and Management 324 (2025) 119294

Table 5 2.5.2. Steam and air reactors modelling

Reaction pathway occurring in the three reactors of the chemical looping plant. The SR (OXY in Fig. 6) has been modelled with a series of five
Reactor Reactions adiabatic RGibbs blocks, while the AR (COMB in Fig. 6) with a single
reactor RGibbs, which is generally deemed sufficient to reproduce the
Fuel Reactor MSW→Char + Volatiles (CO, H2 , CH4 , etc) + Ashes
CO + 3Fe2 O3 → 2Fe3 O4 + CO2 thermodynamic conditions of an entrained bed [37]. In this way the
H2 + 3Fe2 O3 → 2Fe3 O4 + H2 O three reactors operate under adiabatic conditions and the system is
Cs + Fe2 O3 → 2FeO + CO autothermal.
Cs + Fe3 O4 → 3FeO + CO The steam enters the SR at 180 ◦ C and 2 bar from the heat recovery
Steam Reactor 3FeO + H2 O→Fe3 O4 + H2
Air Reactor 4FeO + O2 →2Fe2 O3
steam generation section. The FeO stream leaving the FR is divided into
4Fe3 O4 + O2 →6Fe2 O3 two streams directed to the SR (66 % wt) and AR (34 % wt). This strategy
is meant to enhance the heat release in the AR from the exothermic
oxidation reactions and compensate for the endothermicity in the FR.
time of these configuration, which allows for higher solid conversion, The air mass flow to the AR (AIR) has been adjusted to meet two
while the air reactor (AR) is an entrained bed. Counter current moving conditions:
bed reactors are generally simulated with a series of at least five adia­
batic/isothermal RGibbs blocks, as indicated in Ref. [34]. The modelling (1) complete oxidation of the Fe3O4/FeO stream flowing into the AR,
scheme adopted for the FR is schematically presented in Figure S5 of the (2) solid products temperature from the AR equal to the oxygen
Supplementary Material, while the model validation is presented in carrier inlet temperature to the FR (autothermal operation).
Tables S2 and S3, and Figures S6 and S7. The Aspen Plus flowsheet of the
chemical looping plant is shown in Fig. 6. Before injection into the AR, the air stream is compressed to 3 atm
The temperatures of the five isothermal RGibbs reactors have been (COMP in Fig. 6) and preheated by heat exchange (PRE-HEAT in Fig. 6)
set to reproduce a temperature range of 850 ◦ C − 950 ◦ C along the with the high-temperature gaseous products from the AR, as shown in
moving bed reactor, which has been observed in the experimental work the process scheme of Fig. 6. At the outlet of the three reactors, the gas
of Ref. [35]. Isothermal RGibbs have been selected to include in the total
heat balance the MSW thermal decomposition heat duty, which is often
Table 6
neglected in the literature. The system total pressure has been set at 1 Main operating parameters for the chemical looping plant.
atm, and autothermal operation is achieved by tuning the inlet tem­
Unit Values Block
perature of the oxygen carrier, i.e. the outlet temperature from the AR,
to respect the energy balance in Eq. (15). MSW 25 ◦ C, 1 atm, 100 t/h Inlet FR
Oxygen Carrier 66.8 % Fe2O3, 33.2 % SiC, 1.26 kt/y Inlet FR
Qdec + QR1 + QR2 + QR3 + QR4 + QR5 = 0 (15) oxygen carrier
Pyrolysis 600 ◦ C, 1 atm RYield
Where Qdec is the thermal decomposition heat duty, QR1 , QR2 , QR3 , QR4 Fuel Reactor 850–950 ◦ C, 1 atm, 5 RGibbs
Steam Reactor Adiabatic, 1 atm, 94 t/h H2Oin 5 RGibbs
and QR5 are the heat duties associated with the reactions occurring along Air Reactor Adiabatic, 1 atm, 893 t/h airin RGibbs
the height of the reactor (RED in Fig. 6).The summation of these six heat Air compressor 3 atm, isentropic Comp
duties corresponds to the global heat absorbed or released by the FR, Air Preheater 900 ◦ C (air), 1 atm HeatX
which must be zero for adiabatic operation in the reactor. HRSG 136.2 bar, 11.7 bar, 3.45 bar; 93.6 ton/h Hierarchy
H2Oin
The presence of tar in the outlet gases has been neglected considering
Compressors 85 % isentropic, 95 % mechanical ​ MComp
the large OC to biomass ratio adopted and the use of CO2 as gasifying Pumps (MP) 83 % efficiency, 95 % driver ​ Pump
agent. However, specific data on this regard are still scarce and are Steam Turbines (LP-MP- 88 %-92 %-94 % isentropic, 95 % ​ Comp
mainly focussed on biomass chemical looping combustion [36]. HP) mechanical

Fig. 6. Aspen Plus flowsheet of the autothermal chemical looping hydrogen production plant.

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O. Palone et al. Energy Conversion and Management 324 (2025) 119294

Fig. 7. Aspen Plus flowsheet of the cleaning and purification section in the CL-SNG plant.

streams are sent to a heat recovery steam generator unit feeding a utilization factor of 0.80 for both plants, as for the waste incinerator
conventional Rankine cycle with three pressure levels (136.2 bar, 11.7 plant modelled in Ref. [41].
bar, 3.45 bar) and no superheating, as described in detail in Ref. [38]. The cost basis used for estimating the capital costs is the Bare Erected
A summary of the main operating parameters of the chemical looping Cost (BEC), which represents the erection costs incurred for each
plant is given in Table 6. equipment, including installation costs, steel structures, and all neces­
sary instrumentation (control valves, piping, etc.). The BEC has been
2.6. Gas cleaning section in CL-SNG calculated according to Eq. (16).
( )n ( )
S CEPCI2023
The Aspen Plus flowsheet of this section is given in Fig. 7. The BEC = BECref ⋅ ⋅ (16)
Sref CECPCIref
cleaning section of the CL-SNG plant is organised into three lines, i.e.
one for each gas stream from the chemical looping plant. The most Where BECref is the reference bare erected cost of the block or single
complex line is dedicated to the treatment of the CO2-rich stream leaving equipment; S is a characteristic parameter or size of the equipment; n is
the FR, as it has a greater variety of pollutants [39], and involves par­ the scale factor; and CEPCI stands for Chemical Engineering Plant Cost
ticulate matter removal by baghouse filters, wet flue gas desulphuriza­ Index, which considers the effect of inflation on the equipment costs. If
tion (FGD), HCN and COS hydrolysis, mercury removal, Lo-Cat and ZnO the scale factor n values are not available from the literature, the con­
bed for deep H2S removal. The wet FGD block removes SOx by absorp­ ventional value of 0.67 is generally selected.
tion with an alkaline-based slurry and has been modelled with a sepa­ The data used for calculating the BEC of each unit are collected and
rator of 95 % removal efficiency [24]. detailed in Tables S4 to S7 of the Supplementary Material. For
In contrast, the gas stream from the SR is purified from H2S by the simplicity, coolers and heat exchangers costs have been taken from the
series of a Lo-Cat reactor and a ZnO guard bed. The presence of H2S in Aspen Economic Analyzer, while the rest has been derived by scaling
the stream from the SR is due to the hydrogenation of FeS that forms in costs according to Eq. (16). The cost calculation also includes process
the FR by the interaction with the MSW, as confirmed by experimental units not simulated in Aspen Plus, such as the feed pre-treatment
analyses in Ref. [40]. On the contrary, the gas stream from the AR is (milling, drying, pelletising) and the ASU. From the BEC, the Total As
designed to remove SOx by flue gas desulphurization and NOx by se­ Spent Cost (TASC) has been computed by following the calculation
lective catalytic removal (SCR). procedure in Table S8 of the Supplementary Material, which is derived
A summary of the assumptions on the removal efficiency of con­ from Ref. [42].
taminants for each block of the cleaning section is provided in Table 3. Fixed operating costs include maintenance, insurance and taxes, and
The CO2 stream exiting the cleaning section is divided into three the annual cost of workers. The average wage of each employee has been
streams, as shown in the Figure S8 of the Supplementary Material. The set at 34.5 €/hour, assuming 13 operators per shift (estimated from a
first stream is mixed with the H2 stream from the SR, compressed to 20 correlation provided by Turton et al. [43]).
bars, and sent to methanation; the second one is sent to the FR as Conversely, variable costs encompass all cost items dependent on the
enhancer in the FR (100 kmol/h CO2); the third one, which is in excess, plant’s usage and can be divided into raw materials (process water,
is sent to permanent storage after inter-refrigerated compression to 83 feedstock, fuels, chemicals, etc.) and utilities (cooling water, electricity,
bar. etc.). The cost of the MSW has been calculated as the sum of literature
costs for milling, thermal pre-treatment (drying and combustion), and
2.6.1. Methanation in CL-SNG pelletizing. The electricity consumption of the ASU has been assumed
The methanation section of the CL-SNG plant has been modelled as equal to 150 kWh/tO2 [44]. The cooling water flow rate has been
already described for the G-SNG configuration. In this case the two- calculated by imposing a temperature variation of the water between
stages compressor (20 bar outlet, 35 ◦ C intercooling) at the inlet elab­ 20 ◦ C (inlet) and 30 ◦ C (outlet) in all coolers. The cooling water cost
orates both the H2 and CO2 streams, because both are at atmospheric includes the water makeup due to losses in the cooling tower and the
pressure conditions from the chemical looping plant. electricity consumption associated with the fans. All other cost items,
including those related to process parts that have not been simulated in
2.7. Economic analysis method detail, have been estimated by linearly scaling specific consumption
values from the literature according to the inlet reactants flow rate of the
The operational lifetime of the plant has been set to 25 years with a

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O. Palone et al. Energy Conversion and Management 324 (2025) 119294

Table 7 Table 8
Financial assumptions and operating cost parameters. Energy and environmental KPI.
Parameter Value Ref. KPP Units Expression Eq.

Capacity Factor 80 % [41] CO2 Storage Ratio [-] mCO2 ,stored ​

(21)
​ CSR =
Plant Lifetime [years] 25 ​ Assumed mCO2 ,total
Discount rate 8% Assumed SNG to MSW Mass Ratio [-] mSNG ​
(22)
​ G/M =
Fixed Operating Costs ​ ​ ​ mMSW
​
SNG Production [-] m ⋅LHVSNG (23)
Operating Labor Rate (Base) [€/h] 31.5 ​ Assumed ηSNG = SNG
Efficiency mMSW ⋅LHVMSW
Labors Per Shift 13 ​ Calculated ​
[43] Energy Intensity [GJ/t] EI = (24)
mMSW ⋅LHVMSW + Wnet, el
Operating Labor Burden (% OLR) 30 % ​ [45]
mSNG
Labor Overhead Charge Rate (% OLB + 25 % ​ [45] mCO2,avoided ​
Specific CO2 Avoided [kg/ (25)
OLR) CO2, avoided =
MWh] mSNG ⋅LHVSNG
Property taxes and Insurance (% TOC) 1% ​ [42] mH2 Oprocess
Specific Water [kg/ H2 Ocons = ​ (26)
Maintenance (% TOC) 2.5 % ​ [42]
Consumption 1
MWh] mSNG ⋅LHVSNG
Variable Operating Costs ​ Cons/ ​
day1 1
Referred to the process water employed for WGS, gasification, and chemical
MSW pretreatment [€/t] 23.122 ​ Calculated looping sections.
Process Water [€/m3] 6.00 ​ [45]
Iron Oxide [€/kgFe2O3] 1.82 ​ [45]
WGS Catalysts [€/ft3] 453.48 1.37 [11]
Methanation Catalyst [€/ft3] 400.00 1.40 [11] Table 9
Hg-Rem Catalyst [€/lb] 1.48 291.63 [45] SNG quality parameters assessment by comparison with the Italian legislation
ZnO [€/kg] 11.43 62.75 [11] requirements [47].
Ammonia (19 % NH3) [€/t] 300.00 80.51 [45]
Parameters G-SNG CL-SNG Italian legislation Units
SCR Catalyst [€/m3] 8125.5 1.91 [45]
FGD (Water + Gypsum) [€/tSO2] 95.00 ​ [11] SNG flow rate 16.3 13.7 ​ t/h
Hyd-React Catalyst [€/m3] 2670.00 0.11 [11] CO2 1.3 0.7 < 3.0 %moldry
Lo-Cat chemicals [€/tS] 136.4 ​ [27] H2 3.5 3.6 < 0.5 %moldry
Carbon Transport and Storage [€/tCO2] 20.00 ​ Assumed CH4 95.1 95.2 − %moldry
Electricity [€/MWh]3 90.00 ​ Assumed N2 0.15 0.5 − %moldry
Cooling Water [€/m3] 0.34 ​ [43] H2O 0.018 0.018 < 0.015 %volwet
Bottom Ash disposal [€/tash] 22.83 ​ [45] Outlet pressure 60 60 − bar
Slag Handling [€/t] 14.75 ​ [11] Outlet temperature 35 35 < 50 ◦
C
1
Wobbe Index 48.67 48.94 47.31–––52.33 MJ/m3
For simplicity the consumption per day (expressed in the same unit of HHV 36.33 36.33 34.95–––45.28 MJ/m3
measure of the specific operating costs) has been calculated by linearly scaling Gas Gravity 0.5553 0.5511 0.5548–––0.8 −
the values reported in the literature or in scientific reports according to the inlet
mass flow rate of gases.
2
Calculated from Ref. [46] by scaling the electricity consumption for milling, perspective, which allows for a reduction in the taxes, thus providing a
drying + combustion, and palletisation. tax benefit as evident from Eq. (18).
3
The electric energy produced by the turbines has been subtracted in the total
electricity consumption. The electricity consumption of the ASU has been Costtaxes = 0.24⋅(Ri − O&Mi − Di ) (18)
assumed equal to 150 kWh/tO2.
Where Ri represents the yearly revenues; O&Mi the annual operation
reference. and maintenance costs (already accounting for the capacity factor), Di
The main assumptions and data used for the economic analysis have the depreciation value. The corporate income tax rate in Italy since 2017
been collected in Table 7. is 24 % [57].
The value of the annual cash flow CFi is calculated through Eqs. (19)
2.7.1. Financial parameters and (20). The annual depreciation is added to the net income (NIi) and
The economic feasibility of the plant is assessed through a series of therefore does not represent a cash outflow incurred during the opera­
financial parameters aimed at evaluating the levelized cost of SNG tional life of the investment.
(LCOSNG). The LCOSNG has been calculated as the selling price NIi = Φi ⋅(LCOSNG⋅ PSNG,i ) − O&Mi − Costtaxes − Di (19)
required to have a zero net present value of the investment at the end of
the plant operational life. CFi = NIi + Di (20)
The Net Present Value (NPVt) for the generic year t has been eval­
uated according to Eq. (17). Where PSNG,i indicates the annual production of SNG; φi is the annual
t
capacity factor of the plant; O&Mi represents the annual operation and
∑ CFt maintenance costs (already accounting for the capacity factor).
NPVt = C0 − (17)
n=1
(1 + i)n
2.8. Energy and environmental parameters
Where C0 represents the capital cost of the plant, namely the Total
Overnight Cost (TOC), CFt is the annual cash flow, and i is the discount
The energy and environmental performances of the plant have been
rate, which has been set to 8 %. The construction period has been
evaluated based on the key performance parameters (KPP) collected in
neglected. The value of the plant capital cost has been amortized over
Eqs. (21) to (26) of Table 8.
the entire operational life of the investment through the depreciation
(Di)1. To obtain a first indication of the economic feasibility of the plant,
3. Results and discussion
a constant depreciation value has been assumed. This annual contribu­
tion must be considered as an actual cost from an accounting
3.1. SNG quality assessment

In both configurations, the reactants feed molar ratio is equal to H2/

1
Di = TOC
30 CO2 = 4. The SNG at the outlet of the multistage compression section is

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O. Palone et al. Energy Conversion and Management 324 (2025) 119294

Table 11
Economic comparison between the configurations in terms of CAPEX, OPEX, and
LCOSNG.
Capital costs (M€) G-SNG CL-SNG

Bare Erected Cost 831.5 430.3

EPC 83.2 43.0
Total Direct & Indirect Cost 914.6 473.3
Contingencies 91.5 94.7
Total Plant Cost 1000 568.0
Owner’s Cost 150.1 85.2
Total Overnight Cost 1157.0 653.2
Total As Spent Cost 1285.4 725.7
Fixed Operating Costs (M€) Annual Cost
Labor cost 5.8 5.8
Maintenance Cost 28.9 16.3
Property taxes and Insurance 11.6 6.5
Total Fixed OPEX 46.3 28.7
Variable Operating Costs (M€) Annual Cost
MSW 16.20 16.20
Fig. 8. Gas composition variation across the methanation plant (G-SNG and Process Water 6.18 3.94
CL-SNG). Oxygen carrier (Fe2O3/SiC) 0 1.8
WGS Catalysts 0.18 0
Methanation Catalysts 0.16 0.15
Table 10 Hg-Rem Catalyst 0.13 0.14
Energy and environmental parameters comparison between G-SNG and CL-SNG ZnO bed 0.21 0.27
configurations. Ammonia (19 % NH3) 0 7.1
Water + Gypsum for FGD 0 0.94
Parameter G- CL- Literature Units Hydrolysis Reactor Catalyst 0.0087 0.096
SNG SNG Lo-Cat Chemicals 1.27 0.55
SCR Catalyst 0 4.54
CO2 Storage Ratio 69 % 74 % − [-]
Carbon Transport and Storage 13.77 15.2
SNG/MSW Mass Ratio 0.16 0.14 − [-]
Electricity 24.76 7.65
Specific CO2 avoided 655 978 190 [kgCO2/MWhSNG]
Cooling Water 2.11 0.45
Specific H2O consumption 673 509 627 [kgH2O/
Slag Handling 1.29 0
MWhSNG]
Bottom Ashes Disposal 0 2.00
Energy Intensity1 125 141 − [GJ/tSNG]
Total Variable OPEX (M€) 68.58 60.77
SNG Process Efficiency 42 % 35 % 44.6 % [-]
LCOSNG [€/kg] 2.26 1.76
1
LHV of MSW equal to 18.9 MJ/kg.

[47] on SNG production from captured CO2 in waste incinerator flue

at suitable conditions for transportation into the gas grid (60 bar, 35 ◦ C),
gases and water electrolysis.
and is characterized by the molar composition illustrated in Table 9. The
In the G-SNG case, the CO2 sent to storage is approximately 69 % of
final SNG productivity are equal to 16.3 t/h in the G-SNG and 13.7 in the
the total compared to 74 % for the CL-SNG case, while the remaining
CL-SNG scenario, because of the higher H2 productivity from the updraft
portion is involved in the methanation process. This translates into
gasification.
higher CO2 utilization in the updraft gasification configuration, though
Compared to the indications of the Italian gas operator (SNAM), the
part of the CO2 is also used as enhancer in the FR.
SNG quality obtained in both configurations falls within the limits
The process water consumption (673 kg/MWh and 509 kg/MWh for
specified for CO2, while it present slightly higher moisture content and
G-SNG and CL-SNG, respectively) is associated with the WGS section,
sensibly higher H2 concentration (around 3.5 % mol in both cases).
steam gasification, and the SR of the chemical looping plant, and can be
However, SNAM has reported to have successfully tested for one month
reduced by recirculating the quantities separated in the flash drums.
a NG/H2 blend up to 5 % supplying two industrial facilities in the south
However, the reported values for H2O consumption are aligned with the
of Italy [48], so it is expected that higher H2 concentrations will be
values reported by Salomone et al. [47] for SNG production from water
allowed in the future. Differently, membrane separation can be
electrolysis and waste incineration CO2.
considered for SNG upgrading [49].
The energy efficiencies of SNG production (ηSNG ) settle at 42 % and
To assess the conformity of the produced SNG with the Italian
35 % for G-SNG and CL-SNG, respectively, similarly to the energy in­
legislation, the Wobbe index, the HHV, and the Gas Gravity have been
tensity (EI) being lower in the G-SNG configuration (125 GJ/t vs 141
evaluated. The values obtained in both configurations are within the
GJ/t). Optimization of the chemical looping plant operating conditions
validity ranges reported by the SNAM network code in Ref. [47], except
would be beneficial to improve the energy and environmental perfor­
for the Gas Gravity, where a slight deviation from the lower limit is
mance of the process and enhance competitivity with the updraft gasi­
detected in the CL-SNG case.
fication case. It is out of the scope of this work to model the power
The syngas composition variation from the inlet to the injection into
production plant supplying to the system, although as a Waste-to-Fuel
the gas grid is given in Fig. 8 for both the plants. Starting from the inlet
(or Power-to-Gas) strategy renewable or nuclear power should be
conditions of H2/CO2 = 4 (ENTER), the methane concentration in the
considered as a low-carbon source.
gas products increases steadily with each reaction step (OUT-1 to 4 in
Details on the mass flows, compositions, temperature and pressure of
Fig. 8) and then, after deep water removal by successive flash conden­
each stream are available in the Supplementary Material.
sation and membrane adsorption (SNG-COMP in Fig. 8), the final syngas
composition of Table 9 is achieved.
3.3. Economic analysis results
3.2. Energy and environmental performance results
In Table 11, the two plants are compared in terms of capital costs,
Table 10 shows the energy and environmental analysis of the two operational costs, and LCOSNG. The BEC values of each process unit are
configurations and compares the results with data by Salomone et al. reported in detail in the Supplementary Material. Although the G-SNG

11
O. Palone et al. Energy Conversion and Management 324 (2025) 119294

Fig. 9. CAPEX and OPEX breakdown for: (a) and (b) G-SNG; (c) and (d) CL-SNG.

configuration presents a higher SNG productivity, the larger CAPEX and operating costs, as shown in Fig. 9 (b) and (d). These costs account for
OPEX lead to 22 % higher LCOSNG (2.26 €/kg vs 1.76 €/kg) compared the MSW preparation by drying and pelletizing, which has been assumed
to the CL-SNG case. as feedstock cost, the process water consumption, the catalysts
As shown in Fig. 9 (a) and (c), for both configurations the most replacement, and the chemicals consumption for the gas cleaning sec­
significant portion of the capital costs is allocated to the utilities and tion. The utilities account for the 26 % and 9 % of the total in G-SNG and
other equipment, i.e., pumps, heat exchangers, compressors, steam CL-SNG, respectively, due to lower electric power and cooling water
turbines, boilers etc., which accounts for 31 % and 56 % of the total BEC consumption of the latter case. For instance, the intrinsic separation of
of G-SNG and CL-SNG, respectively. In the CL-SNG scenario, the air the H2 stream from the CO2 stream in the chemical looping plant avoids
preheater has been evaluated by using Turton cost correlations [43]. The the presence of the PSA unit and the required compression duty to 23
TASC of the CL-SNG configuration is around 56 % of that in the G-SNG bars. Similarly, no air separation unit is required in the CL-SNG plant
case. This is due to the larger number of process units involved in the because the oxygen supply occurs by gas–solid reactions. On the con­
latter configuration, such as the air separation unit for oxygen produc­ trary, the CO2 tax covers a higher share in the CL-SNG section because
tion, the water gas shift reactors and the PSA unit for H2 intensification the H2 productivity is lower in the CL-SNG (6.6 t/h vs 7.8 t/h to the
and separation, the tar reformer. On the contrary, the syngas cleaning methanation plant) and therefore the CO2 fraction sent to methanation
section impacts more in the CL-SNG scenario, given that three parallel is lower compared to the G-SNG scenario.
cleaning lines must be installed.
The raw materials costs cover the 28 % and 42 % of the total

12
O. Palone et al. Energy Conversion and Management 324 (2025) 119294

Fig. 10. LCOSNG sensitivity analyses by ± 50 % on the capital cost, discount rate, electricity cost, MSW pre-treatment cost, and capacity factor (0.65–0.95) for: (a)
G-SNG and (b) CL-SNG.

3.3.1. Cost sensitivity analyses availability of the plant is therefore crucial to ensure economic
Sensitivity analyses have been conducted to evaluate the effect on competitiveness, although the complexity of the feedstock may be
the LCOSNG of the electricity cost, the MSW pre-treatment cost, the responsible for frequent plant shutdowns. The capital cost sensitivity
discount rate, the capital plant cost, and the capacity factor. The results analysis shows the maximum oscillation from the baseline (± 27.7 % in
are collected in Fig. 10. For simplicity, the percentage variations from G.SNG and ± 23.6 % in CL-SNG). Investment cost reduction may be
the baseline LCOSNG values have been collected in Table S9 of the associated with the increase in the technological maturity of the two
Supplementary Material. solutions, especially for the three-reactors chemical looping process.
The three main parameters affecting the LCOSNG are represented by Electricity consumption represents one the main cost items of the
the capital costs, the discount rates, and the capacity factor. Differently OPEX, and a ± 50 % variation of results in the LCOSNG ranging between
from the other parameters, the capacity factor has a non-linear effect on 2.08 €/kg – 2.44 €/kg for G-SNG and 1.68 €/kg – 1.85 €/kg for CL-SNG.
the final costs, providing a larger percentage variation (+17 % in G-SNG A reduction in electricity costs can occur when a renewable energy plant
and + 15 in CL-SNG) with respect to the baseline in the worst-case fully dedicated to the chemical plant is installed or, more commonly, if
scenario, i.e. the capacity factor is reduced to 0.65. Improving the certified green electricity is supplied from the grid. On the contrary, a

13
O. Palone et al. Energy Conversion and Management 324 (2025) 119294

Table 12 the accepted value (3.5 % in vol), though this threshold is expected
Comparison of LCOSNG from technologies proposed in the literature aiming at to increase in the forthcoming years.
SNG production. 2) The configuration based on chemical looping presents a levelized
Technology LCOSNG [€/kg] Reference cost of substitute natural gas of 1.76 €/kg with respect to 2.26 €/kg
Updraft Gasification 2.08–––2.44 This work
for the updraft gasification pathway. This difference is due to the
Chemical Looping Hydrogen Production 1.68–––1.85 This work higher capital cost of the updraft gasification plant, which involves
Green Electrolysis + CO2 purchase1 3.2–––4.0 [50] more process units such as: the tar reformer, the air separation unit,
Green Electrolysis + CO2 purchase2 1.6–––2.6 [51] the water gas shift section, and the pressure swing adsorption. On the
Green electrolysis + CO2 purchase3 1.3–––1.9 [52]
contrary, the chemical looping pathway is characterized by intrinsic
Green Electrolysis + CO2 capture 1.82 [53]
Biomass gasification + H2 purchase4 1.25–––2.8 [54] separation of the gas species and high purity H2 production. How­
NG market price 0.8 – 1.5 [55] ever, chemical looping application to process solid wastes should be
1 experimentally investigated to confirm the assumptions, from both
Batteries electric storage is also considered, which increases the cost of
electricity supply.
the process (e.g. tar production) and economic (capacity factor)
2
Electricity cost of 14.3 €/MWh (Qatar). point of view.
3
Assumed a very low water electrolysis stack cost of 270 $/kW and 400 $/kW 3) Energy and environmental analysis results are in contrast with the
for alkaline and polymeric membrane electrolysis, respectively, as well as an economic results. The updraft gasification plant shows an outlet SNG
interest rate of 4.5%. flow rate of 16.3 t/h with respect to 13.7 t/h of the chemical looping
4
Discount rate of 5% and biomass price changing from 0 to 20 €/GJ. plant. This results in higher synthetic methane production efficiency
(42 % vs 34 %), lower energy intensity (125 vs 141 GJ/tSNG), and
variation in the MSW pre-treatment cost has a more limited effect on the higher SNG/MSW mass ratio (16 % vs 14 %). However, the hydrogen
LCOSNG. A reduction in MSW costs can be induced by changes in power production and consequently the SNG flow rate can be improved by
consumption related to the pre-treatment phase or, more likely, by optimizing the oxygen carrier composition and the thermodynamic
government incentives for waste treatment, especially in countries fac­ conditions in the steam reactor.
ing serious disposal issues. 4) Sensitivity analyses have been performed on: the cost of electricity,
municipal solid waste pretreatment costs, the total capital cost, the
3.3.2. Comparison with alternative technologies discount rate, and the plant capacity factor. The economic com­
Considering the challenges of a future reduction in the discount rate petitivity of the chemical looping configuration has been confirmed.
and capital costs of the two plants, the cost of MSW and electricity The future reduction in the electricity cost by renewable energy
represent two promising parameters for reducing LCOSNG and sources penetration, possible incentives on municipal solid waste
achieving competitiveness with other decarbonization technologies. processing, and selling of byproducts (e.g. high purity N2 in chemical
Table 12 shows the LCOSNG range according to a ± 50 % variation looping plant) are addressed as the most likely solutions to enhance
in the electricity cost and the values of other SNG production configu­ the economic competitivity with alternative pathways presented in
rations presented in the literature. For an electricity cost range of the literature and with fossil NG.
50–140 €/MWh, the LCOSNG ranges between 2.08–––2.44 €/kg for G-
SNG and between 1.68–––1.85 €/kg for CL-SNG. The cost ranges indi­ CRediT authorship contribution statement
cated in the literature for alternative technologies are on average below
the values hereby calculated for the G-SNG scenario and above those of Orlando Palone: Writing – review & editing, Writing – original
the CL-SNG scenario. However, literature values often start from opti­ draft, Software, Methodology, Formal analysis, Conceptualization. Luca
mistic assumptions relating to the capital cost of the technologies, such Cedola: Supervision, Conceptualization. Franco Rispoli: Supervision,
as the electrolysers stack cost, the electricity supply cost, and the dis­ Funding acquisition. Domenico Borello: Writing – review & editing,
count rates (see Table 12). Supervision, Funding acquisition, Conceptualization.
Cost competitivity with fossil NG can be achieved by combining:
government incentives on the reconversion of MSW into fuels (especially Declaration of competing interest
in countries facing waste disposal challenges), low cost electricity sup­
ply, CO2 taxation, efficient synergies with other industrial processes, The authors declare the following financial interests/personal re­
process efficiency and availability maximization. Fossil NG price is in lationships which may be considered as potential competing interests:
the range between 0.8 €/kg (industrial) − 1.5 €/kg (household) [55] and Domenico Borello reports equipment, drugs, or supplies was provided by
is expected to increase in the following years. Moreover, in the chemical Italian National Agency for New Technologies, Energy and Sustainable
looping configuration further treatment and selling of high-purity N2 Economic Development (ENEA). Domenico Borello reports financial
from the AR could represent an additional and substantial source reve­ support was provided by Italian Ministry of University and Research
nue, as first proposed in the process scheme investigated in Ref. [56]. (MUR). If there are other authors, they declare that they have no known
competing financial interests or personal relationships that could have
4. Conclusions appeared to influence the work reported in this paper.

A comparative techno-economic analysis has been carried out on two Acknowledgements

process configurations for substitute natural gas production from
municipal solid waste thermochemical processing. The technological The authors acknowledge the support by Italian Ministry of Uni­
solutions hereby considered are based on the following main steps: (a) versity and Research (MUR) as part of the European Union program
syngas production from either updraft gasification or chemical looping NextGenerationEU, PNRR - M4C2 - ECS_00000024 “Rome Technopole”.
hydrogen production, (b) syngas purification, (c) catalytic methanation. Additionally, the authors acknowledge support by the European Union –
The following main points can be drawn from the comparative analysis: NextGeneration EU from the Italian Ministry of Environment and Energy
Security POR H2 AdP MASE/ENEA with involvement of CNR and RSE,
1) In both configurations, the substitute natural gas quality respects the PNRR - Mission 2, Component 2, Investment 3.5 «Ricerca e Sviluppo di
Wobbe Index, Gas Gravity, and Higher Heating Value ranges indi­ Tecnologie per la Filiera dell’Idrogeno». Finally, the authors would like
cated by the Italian legislation. The H2 content is significantly above to thank MSc Luca del Sole, MSc Davide Catoni and BSc Federico Iorio
for their contributions to this work.

14
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