3.2 5.

Perspective

Green Hydrogen Production

by Anion Exchange Membrane
Water Electrolysis: Status and
Future Perspectives

Daniela S. Falcão

https://doi.org/10.3390/en16020943
 energies
Perspective
Green Hydrogen Production by Anion Exchange Membrane
Water Electrolysis: Status and Future Perspectives
Daniela S. Falcão 1,2

1 CEFT—Transport Phenomena Research Centre, Faculty of Engineering, University of Porto,

Rua Dr. Roberto Frias, 4200-465 Porto, Portugal; [email protected]
2 ALiCE—Associate Laboratory in Chemical Engineering, Faculty of Engineering, University of Porto,
Rua Dr. Roberto Frias, 4200-465 Porto, Portugal

Abstract: Green hydrogen production, i.e., produced on a CO2 -neutral basis through the electrolysis
of water employing renewable electricity, has attracted increasing attention. The electricity required
is generated from Renewable Energy Sources (RES), for example, wind energy, hydropower, or solar
energy. Since neither the process of production nor the end products of H2 and O2 are harmful to the
environment, green hydrogen is climate neutral. Developing electrolysis technology is, therefore, a
research topic to follow. Anion Exchange Membrane (AEM) Water Electrolysis (WE) is an innovative
technology that couples the advantages of the more mature technologies of Proton Exchange Mem-
brane (PEM) and conventional alkaline electrolysis, with the potential to eliminate the drawbacks of
both. AEMWE technology is in an evolutionary stage and involves more investigation on several
research topics, such as membrane and catalyst development and stability, as well as alternative
feeding solutions that do not compromise the availability of fresh water. These topics are addressed
in this paper, mentioning the state-of-the-art materials, new promising ones, and providing future
research directions to improve AEMWE towards a most mature technology.

Keywords: green hydrogen; water electrolysis; anion exchange membrane; transition metal catalysts;
durability; feeding solution

Citation: Falcão, D.S. Green 1. Introduction

Hydrogen Production by Anion
Considering the world’s growing interest in producing green hydrogen, WE using
Exchange Membrane Water
RES appears as a promising solution. The two leading WE technologies to produce hy-
Electrolysis: Status and Future
Perspectives. Energies 2023, 16, 943.
drogen are conventional alkaline and PEM electrolysis, where the ions crossing the di-
https://doi.org/10.3390/en16020943
aphragm/membrane are hydroxide anions and hydrogen protons, respectively. The latter
presents two main advantages: great flexibility (On/Off cycling and transient operation)
Academic Editor: Jin-Soo Park and operation at high current densities. However, the high production cost related to the
Received: 16 December 2022 materials used (Platinum-Group Metals—PGM and titanium) is a limitation. Conventional
Revised: 5 January 2023 alkaline WE with liquid electrolytes are notable among others due to their larger maturity
Accepted: 8 January 2023 and higher commercial outreach [1]. In the conventional configuration, a thick diaphragm is
Published: 14 January 2023 necessary to separate the electrodes with a liquid electrolyte, resulting in moderate current
densities, lower hydrogen purity, and weak load cycling. Nevertheless, this technology
allows the use of non-noble metals, reducing production costs, and has a higher lifetime.
Recently, polymeric AEMs have been developed for electrochemical system applications [2].
Copyright: © 2023 by the author. They included advantages from both PEM and alkaline WE. The principal modification
Licensee MDPI, Basel, Switzerland. between conventional alkaline and AEMWE is the substitution of the diaphragm by an
This article is an open access article AEM, enabling the operation at higher current densities and preserving the opportunity of
distributed under the terms and
using non-noble metal catalysts. There is a research gap concerning the main components
conditions of the Creative Commons
and integrated AEMWE that can be assigned to the system complexity and the lack of
Attribution (CC BY) license (https://
standard evaluation criteria. For instance, most of the Hydrogen Evolution Reaction (HER)
creativecommons.org/licenses/by/
and Oxygen Evolution Reaction (OER) electrocatalysts described with excellent activity are
4.0/).

Energies 2023, 16, 943. https://doi.org/10.3390/en16020943 https://www.mdpi.com/journal/energies

Energies 2023, 16, 943 2 of 8

tested at room temperature, for a small period, at low voltages, but these conditions do not
correspond to real applications [3]. To be a competitive technology, by 2050, AEMWEs must
operate at current densities above 2 Acm−2 with a voltage below 2 V [4]. Accelerated Stress
Tests (ASTs) are decisive for determining the targeted lifetime of AEMWEs. Developments
regarding the key electrolyzer components, such as the membrane, electrocatalyst, and
their effects on electrolysis performance, have been reported in the literature [5]. The Mem-
brane Electrode Assembly (MEA) is the main component that determines the performance
of the electrolyzer, comprising the AEM, ionomer, anode, cathode catalyst layers, and
Gas Diffusion Layers (GDLs). Although some membranes are commercially offered, they
have two important weaknesses: the mobility of anions through the AEM is considerably
lower than the mobility of protons through a PEM, and they do not demonstrate good
chemical and/or mechanical stability. The alkaline media brings the advantage of using a
wider variety of cheaper materials for AEMWE components compared to PEMWE. The
feeding-water quality plays a vital role in the electrocatalytic activity and significantly
affects the performance of the AEMWE. However, the use of impure water brings a great
research opportunity considering the shortage of drinking water, but technical barriers for
impure-water splitting need to be overcome [6].
There are several reviews available in the literature concerning AEMWE technology from
a global perspective [2–4,7–10] or addressing specific topics such as membranes [5,11,12] or
electrocatalysts [13], which could be useful to readers who desire to deepen their knowledge
of the topic.
In this perspective paper, four research lines considered hot topics were selected: mem-
brane and catalyst development, and durability and feeding solutions options, including
the interesting possibility of using wastewater.

2. Hot Topics
2.1. Membrane Development
The AEM, comprising an anion exchange cationic group linked to a polymer back-
bone, is a key constituent that determines the AEMWEs’ performance and lifetime. The
mechanical and thermal stability is related to the polymer backbone chemistry, whereas the
ionic conductivity is influenced by the cationic functional groups. The chemical stability is
influenced by both the polymer backbone and the functional groups [7]. There are several
AEMs commercially available, and others developed “in-house”, reported in the literature.
The polymer backbone is frequently a polysulfone, crosslinked polystyrene with divinyl
benzene (DVB), or polyaromatics [7]. For example, poly(fluorenyl aryl piperidinium)-,
polycarbazole-, and polyphenylene-based AEMs were tested in cells attaining current
densities as 2.3, 2.57, and 5.3 Acm−2 , respectively, measured at 1.8 V, presenting good
durability [4]. The cationic functional groups are generally quaternary ammonium (QA) or
imidazolium (IM). Some suppliers commercialize AEMs, such as: Tokuyama (A201) (dis-
continued production), Fumatech (FumasepR), Ionomer (AemionTM ), Dioxide Materials
(Sustainion® ), and Orion Polymer (OrionTM ). There are research-based membranes, e.g.,
Versogen (PiperION) and Xergy (XION™ Ion Exchange Membranes), which are promising
alternatives to overtake commercial membranes. Nevertheless, they are offered on the
market, although they are costly due to their small production scale and are not cost-
competitive with commercial ones. In addition, more studies regarding durability under
severe conditions are needed [4].
Liu et al. [14] tested the performance of an AEMWE at 60 ◦ C with different commercial
membranes: Sustainion® 37-50, Fumasep FAS-50, Fumasep FAPQ, Neosepta ACM, AMI
7001, Nafion® 115, and Celazole® PBI. Better results were found using Sustainion® 37-
50 membranes, operating at 1 Acm−2 at about 1.9 V for 2000 h. The other membranes
presented a high area-specific resistance (ASR) or a higher degradation rate under the
tested conditions.
Henkensmeier et al. [11] published a very interesting paper, giving an overview of
the commercial AEMs (Fumatech Fumasep® FAA3, Tokuyama A201, Ionomer Aemion™,
Energies 2023, 16, 943 3 of 8

Dioxide Materials Sustainion® , and membranes commercialized by Orion Polymer, Cohoes,

NY, USA), and reviewed their properties and performances in AEMWE. The authors con-
cluded that all materials (membrane, ionomer, catalyst, cell design, etc.) must be optimized
together. Consequently, it is difficult to precisely rank the commercial membranes by ana-
lyzing the available literature data, limiting an experimental rank to a system. As an overall
tendency, however, the membranes FAA3 and A201 presented a lower ion conductivity
than the novel membranes Aemion and Sustainion® .
Fortin et al. [15] tested Aemion™ AEMs (all-hydrocarbon) with several ion-exchange
capacities and thicknesses. The authors reported that better results were obtained using the
AEM AF1-HNN8-50, with a thickness of 50 µm, achieving current densities of 2 Acm−2 at
a potential of 1.82 V using 1 M KOH at 60 ◦ C.
Kang et al. [16] used an AEM without an aryl-ether backbone structure (Orion-TM1TM ).
The authors reported that this membrane contains quaternary ammonium as a functional
group and polyphenylene as the backbone, presenting a high ionic conductivity and sta-
bility, performing better and being more durable than the conventional AEM (FAA-3).
Additionally, it showed high efficiency using pure water as a feed solution. The opti-
mized TM1-MEA attained a current density of 2.75 Acm−2 at 1.9 V with great stability of
55 mV h−1 , benefiting from the superior structural advantages of the Orion-TM1™ mem-
brane. The aryl-ether-free structure and hydrophobic properties inhibited decomposition
by ether hydrolysis and prevented the attack of hydrophilic hydroxide ions.
Lv et al. [9] developed a quaternary ammonium poly (n-methyl-piperidine-co-p-
terphenyl) (QAPPT) and Ni-Fe layered double hydroxide (LDH) composite membrane. The
QAPPT/3% Ni-Fe LDH composite membrane exhibited a great performance of 1 Acm−2
at the voltage of 1.824 V at 60 ◦ C, superior to most of the ones reported in the literature.
Moreover, a long-term stability test was conducted at 500 mAcm−2 for more than 87 h,
achieving a reasonable performance.
As explained in the introduction, the MEA, comprising not only the membrane but
also ionomer, anode, and cathode catalyst layers and GDLs, needs to be optimized. A
recent review [9] explained the most common methods used to produce MEAs, catalyst-
coated membrane (CCM), and catalyst-coated substrate (CCS) methods. The commonly
implemented hot-press method used in PEM cells was not a good option in AEMWEs
because i) the degree of mechanical force and high temperature induces irreversible dam-
age to the membrane due to the use of metallic GDLs, and ii) hydrocarbon ionomers
do not have an accessible glass transition (cannot be effectively fused by hot-pressing).
This may lead to performance losses and degradation generated by insufficient contact
and/or gradual delamination between the membrane/catalyst layer interface. Catalyst–
ionomer interaction and loading content optimization are crucial for the advances in
AEMWEs [17]. Engineered MEAs must be developed, aiming for effective contact between
membrane/catalyst/ionomer/GDL.

2.2. Non-PGM Catalyst Development

Theoretically, due to a high pH environment, AEMWE can permit the substitution of
PGM electrocatalysts with Earth-abundant first-row transition metals (e.g., Mn, Fe, Ni, Cu,
and Mo) to catalyze OER and HER reactions. Currently, IrO2 , Ni, Ni-Fe alloys, graphene,
Pb2 Ru2 O6.5 , and Cu0.7 CO2.3 O4 are used as OER catalysts, while Pt black, CuCoOx, Ni-
Mo, Ni/CeO2 -La2 O3 /C, Ni, and graphene could be used as HER catalysts [2]. Ir and
Pt could be replaced by Fe, Ni, Mn, Cu, and Mo, considerably decreasing the prices of
the global system. PGM-free electrocatalysts are already used to catalyze OER, with Ni-
based electrocatalysts, which are currently state-of-the-art. However, for the HER, the
state-of-the-art electrocatalysts are still based on precious metals [4].
Sulaiman et al. [13] wrote a complete review paper with an overview of the latest
electrocatalysts for HER and OER. The authors reported that transition metal catalysts with
very good electrocatalytic properties can play a role in improving AEMWE performance.
For instance, the NiMo-NH3 /NH2 for HER coupled with a Fe-NiMo-NH3 /NH2 for OER
Energies 2023, 16, 943 4 of 8

reached 1 Acm−2 at 1.57 V. Li et al. [3] illustrated that OER kinetics can be influenced by
a higher catalyst loading at the anode, and a lower utilization rate, particularly when the
concentration of hydroxyl ions in the electrolyte has diminished, and active sites on the
catalyst have been blocked by the inevitable high pressure of gas evolved in the MEA. The
authors also stated that Ni-Mo alloyed materials, Co3 O4 nanocrystals, Fe, and Ni-Fe alloys
are good candidates to improve OER performance; however, stability through a period of
one thousand hours needs to be confirmed. Sulaiman et al. [13] reported that bifunctional
(the same for HER and OER reactions) catalysts should be investigated, making a simpler
electrode system. For OER, many of the reported studies demonstrated high activity and
efficiency of transition metal-based catalysts, predominantly NiFe-based, however, the
majority still present high overpotentials beyond 200 mV, at 10 mAcm−2 [13]. The high
overpotentials are associated with the slow and difficult OER mechanism [3]. Considering
HER electrocatalysts, the use of transition metals is still challenging because most of these
catalysts are not as active as Pt/C. HER is also slower in alkaline media than in acid
media [18]. Consequently, to decrease the overpotential and improve the activity of HER
transition metal catalysts, there is a need to understand their reaction mechanism related to
the adsorption of water molecules and bond breaking. One possible approach, reported
by Li et al. [3], is the addition of heteroatoms, such as N-doping, possibly lowering the
adsorption-free energy, facilitating HER. In addition, their stability and efficiency must be
confirmed for real-world applications.

2.3. Durability
Most existing AEMWE components, especially membranes and catalysts, are not
robust enough considering industrial targets due to chemical and mechanical degradation.
This scenario is prone to change with intensive research and a few promising alternatives.
The causes of AEMWE performance losses include membrane degradation. It is well-
known that the hydroxide anions attack the positively charged cations in the AEM, neutral-
izing them [4]. This leads to a loss of anion-exchange functional groups and, consequently,
a decrease in OH− conductivity generating higher ohmic resistances [19]. Additionally,
continued thermal and chemical degradation of ionomers could reduce the connection to
the catalysts, decreasing the reaction rate [13]. The ionomer ionic conductivity is better
using a high number of ion-exchange groups, but this situation intensifies the water uptake
originating the ionomer dissolution at higher temperatures. The catalyst activity may also
become worse through catalyst dissolution, particle coalescence (catalyst agglomeration),
Ostwald ripening, support corrosion, and adsorption of ionomer moieties [7].
Motealleh et al. [20] demonstrated a good performance, considering industrial pa-
rameters using Sustainion® membranes. Durability tests exhibited a stable performance
of 1 A.cm−2 at 1.85 V with a degradation rate below 1 mV/h over 10,000 h, leading to
an estimated lifetime of about 20 years. Moreover, the authors reported that it is possible
to increase the mechanical stability of a Sustainion® membrane through the addition of
zirconia to the polymer matrix.
Henkensmeier et al. [11] determined that stability is intrinsically related to the system.
The authors pointed out that a reliable prediction of membranes’ lifetime is necessary.
Since durability tests usually need up to 10,000 h, it is necessary to develop ASTs, as was
performed for PEM Fuel Cells. Durability tests using ASTs to determine components’ aging
are crucial to attaining the industrial standard requirements. Overall, despite stability
being recognized as a bottleneck, there is weak knowledge about the lifetime of optimized
systems.
Bearing in mind catalyst stability, they must have a lifetime of more than 1000 h and
keep their efficiency when operating at high current densities and under repeated on-off
cycles from RES [13].
Energies 2023, 16, 943 5 of 8

2.4. Feeding Solutions

In AEMWE, deionized water, ultrapure water, 1 wt.% K2 CO3 , and 1 M KOH have
all been used as reactants [3]. Hydroxide solutions are used as an alternative to pure
water to feed AEMWE to increase the ionic conductivity of the AEM because resistance
losses decrease almost linearly (in a limited range of concentrations) when increasing
electrolyte concentration [21]. However, higher hydroxide concentration conducts in
elevated corrosion rates, reducing the lifetime of AEMWEs [7]. Better performances have
been reported using 1 M KOH [2]. The predicted hydrogen demand in the distant renewable
future is 2.3 Gt per year [22]. Considering the reaction stoichiometry, for every kg of
hydrogen produced, 9 kg of water must be consumed. Therefore, 2.3 Gt of hydrogen
requires 20.5 Gt, or 20.5 billion m3 of water [23]. Although in other sectors, i.e., agriculture,
more water is used than necessary for the most ambitious scenario for hydrogen, the scarcity
of freshwater limits its use. As mentioned before, the feeding condition significantly impacts
on the electrocatalytic activity and, consequently, AEMWE performance.
The use of demineralized water is the most preferred option to make AEM electrolysis
a competitive technology. Nevertheless, using pure water carries critical new challenges. Ni
is currently the standard material for electrode construction in AEM electrolysis. However,
under anodic polarization, it is stable only at a pH higher than 9, conditioning the use
of a pure water feed without performance degradation. Another problem with using
deionized water, also occurring using hydroxide solutions, is the negative influence of CO2
on performance. Parrondo et al. [24] described that this phenomenon was due to dissolved
carbonate and bicarbonate anions that diminish the ionic conductivity of the membrane
and catalytic layer binders.
The use of impure water in AEMWE is also an important research topic. Even if most
pollutants in wastewater are successfully removed by the current wastewater treatment
processes, small quantities of impurities (residual organics and ions) remain in the treated
water. No studies show how the impurities affect water electrolyzer performance and
durability, despite studies reporting how impurities affect either the membrane or electrode.
There is a need to understand more fully the impact of water impurities present in wastew-
ater on the performance and durability of AEMWE. For example, despite the fact that
most cationic impurities have undesirable effects during electrolysis, cationic Fe impurities
seem to be essential to stabilize OER activity in alkaline conditions with Earth-abundant
catalysts [6]. Zou et al. [25] reported that Fe cations intensely improve OER activity when
incorporated substitutionally into Ni or Co (oxy)hydroxides, acting as possible OER active
sites. However, pure Fe (oxy)hydroxide is not a good catalyst for OER, and its effect still
needs to be better understood. Cation poisoning can be avoided by adjusting the water flow
rate and current density to minimize co-ion transport or through engineering approaches.
It is also important to understand the relationships between the morphology, composition,
and phase of the catalyst material and its durability in impure water AEM electrolysis.
Analysis of Chemical Oxygen Demand (COD), Total Organic Carbon (TOC), and several
metals (i.e., zinc, copper, iron) present in treated wastewater will be necessary to identify
its composition. If CO2 (previously identified as a detrimental compound) is present, it
must be removed before using the wastewater. It is also possible that supplementary water
treatments will be needed to eliminate specific impurities affecting AEMWE performance
and durability. For example, precipitation or adsorption treatments could be able to remove
undesirable metals.
Another possible solution is the use of seawater to feed AEMWEs. However, this latter
approach leads to a side reaction, competitive with OER: the chloride oxidation reaction
(ClER). Park et al. [26] thoroughly explained this competition and how to avoid/minimize
it. The authors suggested that to achieve high OER selectivity, seawater electrolysis should
be performed below 1.72 VRHE under alkaline conditions, and a more active electrocatalyst
for the OER is essential to attain highly efficient seawater electrolysis in an overvoltage
range of less than 490 mV.
Few studies reported the use of other feeding solutions than hydroxide solutions.
Energies 2023, 16, 943 6 of 8

Park et al. [26] tested an AEMWE using a Ni-doped FeOOH catalyst, tested in 1.0 M
KOH + seawater, demonstrating a current density of 729 mA cm−2 and an energy con-
version efficiency of 76.35%. Compared to reported AEM electrolyzers operated in 1.0 M
KOH, the Ni-doped FeOOH operated in 1.0 M KOH + seawater still exhibited a higher
performance.
Lindquist et al. [27] performed a study with an AEMWE made of commercially
available materials, operating near 1.9 V at 1 A cm−2 in pure water. This study highlights
that improving hydroxide conductivity, mass transport, and long-term ionomer stability
are crucial for developing pure-water AEM electrolyzers.

3. Conclusions and Perspectives

AEMWE is a technology with tremendous potential for development, being the ma-
jor challenge to overcome their high alkaline degradation. The main conclusions and
perspectives are summarized below for each of the hot topics addressed.
Membranes:
Commercial membranes are available, differing in chemistry and thickness, that may
contribute to system improvement and accelerate the research pathway. In particular,
Sustainion® membranes constitute a promising option due to their good performance and
durability. Different combinations using diverse anion exchange cationic groups linked to
different polymer backbones must be investigated to develop more conductive, stable, and
durable membranes. Moreover, all the AEMWE components should be optimized together,
and experimental characterization recurring to IV curves, EIS, CV, and in situ/ex situ
catalysts’ characterization should be performed for a deeper understanding of components’
interactions and the contribution of each component for performance losses and durability.
Catalysts:
Transition metal catalysts are already used with good results in OER, although few
studies have been conducted reporting their use for HER. An interesting option leading to
a simpler MEA construction is the use of bifunctional electrodes presenting good perfor-
mances, considering both OER and HER reactions. Consequently, it is essential to further
investigate the reaction mechanisms to a deep knowledge of the internal properties of
these catalyst materials facilitating the development of more efficient catalysts (with lower
overpotentials). Regarding the catalysts, deposition in the membrane (CCM approach)
is preferable to guarantee better adhesion and to permit the use of lower catalyst load-
ings. Nevertheless, further optimization is essential considering ink composition and
guaranteeing an appropriate electrode–membrane contact during assemblage.
Durability:
The biggest concern when developing new materials, catalysts, and membranes,
besides their performance, is undoubtedly their durability. Some materials appear to be
promising options, but once tested under real operating conditions, they demonstrated
poor durability. ASTs protocols, mimetizing the dynamic RES operating conditions, must
be widely implemented, allowing a quick durability assessment of the materials.
Feeding solutions:
The most used feeding solution is a hydroxide solution due to an improvement
in AEMWE conductivity and, consequently, in performance. However, considering the
shortage of fresh water, the desired options are seawater or treated wastewater. These
options remain an ambitious scenario since AEMWE components quickly deteriorate
with contaminants presented in impure waters, and/or the performance is lower due to
competitive reactions occurring in the electrodes. More efforts in developing more robust
and less susceptible to feed-water impurities AEMWE systems are mandatory to improve
their lifetimes and reduce the overall cost.
Energies 2023, 16, 943 7 of 8

Funding: This work is financially supported by national funds through the FCT/MCTES (PID-
DAC), under the project PTDC/EQU-EQU/1707/2020. This work was also financially supported by
LA/P/0045/2020 (ALiCE), UIDB/00532/2020 and UIDP/00532/2020 (CEFT), funded by national
funds through FCT/MCTES (PIDDAC).
Conflicts of Interest: The author declares no conflict of interest. The funders had no role in the design
of the study; in the collection, analyses, or interpretation of data; in the writing of the manuscript, or
in the decision to publish the results.

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