Available online at www.sciencedirect.
com Current Opinion in
ScienceDirect
Recent progress on electrochemical reduction of CO2
to methanol
Yanrong Liu1, Fangfang Li1, Xiangping Zhang2,3,4 and
Xiaoyan Ji1
Methanol is a future energy carrier because of its high volume-
specific energy density and a significant intermediate for many
bulk chemicals. Electrochemical reduction is a promising
method to fabricate methanol (CH3OH) from carbon dioxide
(CO2) where electrocatalyst, reactor configuration, and elec-
trode play an essential role. In this review, seven types of
electrocatalysts, that is, metal alloys, metal oxides, metal
chalcogenides and carbides, metal–organic complexes,
metal–free pyridine and metal–organic framework–based
electrocatalysts, as well as the effect of reactor configuration
and electrode were comprehensively summarized. Finally,
challenges and perspectives on developing electrocatalysts
were highlighted.
Addresses
1
Energy Engineering, Division of Energy Science, Luleå University of
Technology, 97187, Luleå, Sweden
2
CAS Key Laboratory of Green Process and Engineering, Beijing Key
Laboratory of Ionic Liquids Clean Process, State Key Laboratory of
Multiphase Complex Systems, Institute of Process Engineering, Chi-
nese Academy of Sciences, 100190, Beijing, PR China
3
Zhengzhou Institute of Emerging Industrial Technology, 450000,
Zhengzhou, PR China
4
Dalian National Laboratory for Clean Energy, Dalian, 116023, PR
China
Corresponding authors: Liu, Yanrong (Yanrong.liu@ltu.se); Ji,
Xiaoyan (xiaoyan.ji@ltu.se)
Current Opinion in Green and Sustainable Chemistry 2020,
23:10–17
This review comes from a themed issue on Green processes and
technologies
Edited by Xiangping Zhang
https://doi.org/10.1016/j.cogsc.2020.03.009
2452-2236/© 2020 Elsevier B.V. All rights reserved.
Introduction
CO2 generated from the excessive combustion of fossil
fuels is one of the significant contributors to undesired
climate change. The concentration of CO2 in the at-
mosphere is up to 410 ppm, which is 50% higher than
that of the industrial revolution [1]. In fact, CO2 is an
abundant C1 feedstock, and it can be converted into
various target products by plenty of strategies and
technologies, such as multienzymatic conversion [2],
thermal reduction [3], chemical conversion [4,5], and
photocatalytic [6e8] and electrochemical reduction
Current Opinion in Green and Sustainable Chemistry 2020, 23:10–17
Green and Sustainable Chemistry
(ECR) [9e11]. For multienzymatic conversion, the
inactivation of enzyme is the main reason restricting its
application. For the chemical, thermal, and photo-
catalytic conversions, only under harsh conditions or
using active reagents, the initial reduction barrier of
CO2 can be overcome.
Recently, ECR has been extensively studied owing to
the mild reaction conditions required. CO2 ECR has
obvious advantages in many aspects: (1) the reaction
process is flexible and controllable, (2) the electrolyte
can be recycled which will greatly reduce the con-
sumption of chemicals and the production of waste
liquids, (3) the reaction energy can be provided from
tide, wind, and solar power, and (4) the process of ECR
is green and clean without demand on the external hy-
drogenation source, being convenient for large-scale
applications [9,12].
It was reported that various target products can be ob-
tained from CO2 by ECR, for instance, CO, HCOOH,
CH4, CH3OH, C2H4, and so on. [13e16] Among them,
the conversion of CO2 into CH3OH is of great impor-
tance because CH3OH processes a high energy density
and is a significant precursor for manufacturing the bulk
chemicals such as plastics and silicone [17,18].
Several reviews have been published for CO2 ECR to
CH3OH. For example, Albo et al. [12] and Sun et al.
[19] provided a comprehensive summary of different
types of electrocatalysts, electrolytes, electrochemical
cells, possible reaction mechanisms, and reaction con-
ditions (i.e. pH, temperature, pressure); Zhang et al. [9]
reviewed the electrocatalysts and selectivities of
methanol , while Al-Rowaili et al. [10] introduced the
challenges and future prospects of metaleorganic
framework (MOF) and non-MOF electrocatalysts in
2018. There are mainly three key points in CO2 ECR,
that is, electrocatalyst, electrolyte, and electrochemical
cell. The developments in the electrolytes (e.g. aqueous
solution, organic solvent, ionic liquid) and electro-
chemical cells (e.g. H-type, continuous-flow) are still
very limited. On the contrary, the electrocatalyst, which
can significantly enhance the CH3OH selectivity and
restrain the hydrogen evolution reaction (HER), has
attracted more and more attention. Therefore, in this
review, the newly developed electrocatalysts for CO2
ECR to CH3OH were mainly reviewed, followed by a
www.sciencedirect.com

brief discussion of the reactor configuration/electrode
effect to avoid the repetition of the published reviews.
Electrocatalysts for CO2 ECR to CH3OH
ECR of CO2 to CH3OH can be performed under the
ambient conditions through sixeelectron pathways, in
which the formation of CH3OH undergoes CO [20] or
HCOO
[21] as intermediates (Figure 1). Thermody-
namically, the CO2 reduction potential is 20 mV positive
than that of HER [12], and thus the competition be-
tween CO2 reduction and HER results in low CH3OH
selectivity. In addition, CH3OH formation requires 6e
,
being kinetically slow [10]. Electrocatalyst plays a sig-
nificant role to enhance CH3OH selectivity and sup-
press HER.
Canfield and Frese [22] firstly reported CH3OH as a
direct product on III-V semiconductor electrode. Since
then, metal alloys, inorganic, and organicemetal com-
pounds, as well as the pyridine-based electrocatalysts
have gained a lot of interests attributed to their
remarkable selectivity. Recently, metal-free compounds
were rapidly developed as they can avoid metal utiliza-
tion and improve catalytic activity, as well as the high
selectivity of MOF electrocatalysts. The recent devel-
opment on CO2 ECR to CH3OH is summarized in
Table 1 and discussed in the following sections with
different types of electrocatalysts. In addition, NHE,
RHE, and SHE are represent normal hydrogen elec-
trode, reversible hydrogen electrode, and standard
hydrogen electrode, respectively.
Metal alloys
Poor selectivity and activity of metals limit their prac-
tical applications for CO2 ECR to CH3OH [9]. Metal
Figure 1
Proposed pathways of CO2 ECR to CH3OH. ECR, electrochemical reduction.
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Recent progress on electrochemical Liu et al. 11
alloys can adjust the binding ability of active in-
termediates and thus are promising to enhance the re-
action selectivity and kinetics. A aerogel electrocatalyst
with high porosity was synthesized by Lu et al. [23]
When [BMIM][BF4] and H2O with a molar ratio of 1:3
were selected as electrolytes, the Faradaic efficiency
(FE) and current density of CH3OH can be up to 80%
and 31.8 mA/cm2, respectively, over the Pd83Cu17
aerogel which attributed to the valence states, ratios,
and strong interaction of Pd and Cu. Zhang et al. [24]
investigated this process using electrocatalyst of Cu/
tetrahexahedral Pd nanocrystals (Cu/THH Pd NCs),
indicating that the alcohol selectivity can be controlled
by the monolayers (MLs) of Cu in the electrocatalyst,
and 0.8 ML Cu shows the highest CH3OH selectivity
compared with 1 ML Cu and 1.2 ML Cu. A Zn/Ag foam
electrocatalyst was prepared by Low et al. [25] The
active sites in this electrocatalyst are the strained sub-
micron Zn dendrites, resulting in a FE of 10.5% for
producing CH3OH.
Metal oxides
Metal oxide electrocatalysts have the merits of high
selectivity and high energy efficiency. Cuprous oxide/
polypyrrole particles with octahedral and icosahedra
structure (Cu2O(OL-MH)/Ppy) can achieve a ultrahigh
CH3OH activity and selectivity with FE of 93  1.2%
and 1.61  0.02 mmol/(cm2$s) formation rate at
0.85 V
[26]. The N atoms in the Ppy shell worked as the CO2
active sites, leading to high stability. Albo and Irabien
[18] loaded the electrocatalyst of Cu2O on the gas
diffusion electrode and achieved a FE of 42.3% for
CH3OH formation, founding that Cuþ can significantly
affect the selectivity and activity toward CH3OH.
Moreover, nano Cu2O has a higher stability and
Current Opinion in Green and Sustainable Chemistry
Current Opinion in Green and Sustainable Chemistry 2020, 23:10–17
12 Green processes and technologies

Table 1

Summary of CO2 ECR to CH3OH.

Electrocatalyst Electrolyte Potential (V) Formation rates Current density Faradaic Ref.
(mmol/(m2$s) (mA/cm2) efficiency (%)

Pd83Cu17 aerogel [Bmim][BF4]:H2O (1:3) −2.1 (vs. Ag/Ag+) 43.9 31.8 80 [23]
Cu0.8 ML/THH Pd NCs 0.1 M NaHCO3 −0.46 (vs. RHE) – – 19.5 [24]
PD-Zn/Ag foam 0.1 M KHCO3 −1.38 (vs. RHE) 4.9 −2.7 10.5 [25]
Cu2O(OL-MH)/Ppy 0.5 M KHCO3 −0.85 (vs. RHE) – – 93 ± 1.2 [26]
Pd/SnO2 0.1 M NaHCO3 −0.24 (vs. RHE) – – 54.8 ± 2 [27]
Cu/Cu2O KHCO3 −2.0 (vs. SHE) 46 7.8 47.5 [28]
Cu2O 0.5 M KHCO3 −0.70 (vs. RHE) 73.1 10 42.3 [18]
Cu2O-MWCNTs 0.5 M NaHCO3 −0.11 (vs. RHE) 49.3 7.5 38 [29]
Cu2O/ZnO 10 mM 2-mPy+0.5 M KHCO3 −0.26 (vs. Ag/AgCl) 2.91 1 25.6 [30]
CuO/Cu2O 0.1 M KHCO3 −0.5 (vs. RHE) – – 24 [31]
Ag–Co3O4 –CeO2-LGC 0.1 M KHCO3 −0.85 (vs. RHE) 51.8 12.8 23.4 [32]
Cu/TiO2-NG 0.2 M KI −0.20 (vs. RHE) 0.21 0.061 19.5 [33]
Cu2O/ZnO 0.5 M KHCO3 −0.68 (vs. RHE) 31.7 10.64 17.7 [34]
Cu/TiO2 0.5 M NaHCO3 −2.0 (vs. RHE) 103.7 120 5 [35]
Cu1$63Se (1/3) 30% [Bmim][PF6] −2.1 (vs. Ag/Ag+) 556.3 41.5 77.6 [36]
/MeCN/H2O (5%)
Mo–Bi BMC 0.5 M [Bmim][BF4]/MeCN −0.7 (vs. SHE) 148.8 12.1 71.2 [37]
Fe2P2S6 0.5 M KHCO3 −0.2 (vs. RHE) – – 65.2 [38]
FeS2/NiS 0.5 M KHCO3 −0.6 (vs. RHE) 34.3 3.1 64 [39]
Pt@adenine-rGO 0.1 M KNO3 −0.3 (vs. Ag/AgCl) 7.3 0.5 85 [40]
CoPc-CNT 0.1 M KHCO3 −0.94 (vs. RHE) 80.6 10.6 44 [41]
Pt@histamine-rGO 0.1 M KNO3 −0.3 (vs. Ag/AgCl) – – 37 [42]
Cu/Bi-MOF 0.5 M KHCO3 −0.21 (vs. RHE) 29.7 20 8.6 [43]
Pd/PANI-CuPANI 0.5 M H2SO4 −0.9 (vs. RHE) – – 10 [44]
[Cu3(m6-C9H3O6)2]n 0.5 M KHCO3 −0.28 (vs. RHE) 5.62 10 5.6 [45]
Pd/PANI 0.5 M H2SO4 −0.9 (vs. RHE) – – 5.4 [46]
CuZnDTA 0.5 M KHCO3 −0.63 (vs. RHE) 3.4 10 3.4 [45]
Co(CO3)0$5(OH)$0.11H2O 0.1 M NaHCO3 −0.34 (vs. RHE) 9.2 0.59 97 [47]
[Fe(PP3)(MeCN)2](BF4)2 MeCN + diethylamine (10 v%) −1.25 (vs. NHE) 71 6 68.5 [48]
BP 0.1 M KHCO3 −0.5 (vs. RHE) – – 92 [49]
BBD 1 M NH3 aqueous solution −0.64 (vs. RHE) – – 24.3 [50]
Pyridine (Py) 10 mM Py+0.5 M KCl – – – 39 [51]
2-pyridinethiol@Pt–Au 0.1 M KNO3 −0.2 (vs. Ag/AgCl) – – 39 [52]
[PYD]@Cu –Pt 0.5 M KCl −0.04 (vs. RHE) 140.6 22 37 [53]
[PYD]@Pd 0.5 M KCl −0.04 (vs. RHE) 314.4 ~52 35 [54]
Pyridoxine (PN) 10 mM PN+0.1 M KCl −0.55 (vs. 3 M Ag/AgCl) – – 5 [55]

selectivity compared with Cu for CH3OH production
[28]. Malik et al. [29] synthesized a Cu-based electro-
catalyst with Cu2O incorporated in multi-walled carbon
nanotubes (MWCNTs), showing an optimum FE of
38%. The combination of Cu2O and MWCNTs is benefit
for improving stability of catalyst. Daiyan et al. [31]
prepared a CuO/Cu2O electrocatalyst on Cu foam (3D
heterostructure) and the formed Cuþ/Cu2þ on the Cu
foam electrode enhanced the activity of electrocatalyst.
Several reports indicate that Cu2O/ZnO electrocatalyst
provides good selectivity and activity [30,34,56]. The
nitrogen-doped electrocatalyst of Cu/TiO2-NG [33] and
Cu-supported TiO2 nanotubes [35] showed excellent
performances to produce CH3OH, due to TiO2 can
enhance the CO2 capture, reaction stability, and elec-
trocatalyst surface area. Zhang et al. [27] prepared a 2D
hierarchical Pd/SnO2 with an outstanding selectivity of
54.8  2% for CH3OH. The high selectivity was
attributed to the built up of PdeOeSn interfaces. For
CH3OH production on AgeCo3O4eCeO2, low graphi-
tized carbon, 23.4% FE and 7.5 mA/cm2 current density
were obtained, due to the multi active sites of AgeOe
Ce [32]. These results indicate that introducing oxida-
tion states in metallic electrocatalysts can enhance the
selectivity and activity of CO2 ECR to CH3OH.
Metal chalcogenides and carbides
Metal chalcogenides and carbides were found being
remarkable electrocatalysts for CO2 ECR. Different
compositions of [BMIM][PF6]/CH3CN/H2O were
developed as electrolytes to conduct CO2 ECR with a
series copper electrocatalysts [36]. The results showed
that the catalyst size and structure can significantly
affect the reaction. Among the prepared electro-
catalysts, Cu1$63Se (1/3) nanocatalyst displayed the
highest current density and FE with values of 41.5 mA/

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cm2 and 77.6%, respectively, followed by Cu2Se, Cu2S,
CuSe, CuS, Cu2O, CuO, and Cu. Sun et al. [37] re-
ported a MoeBi bimetallic chalcogenide (MoeBi BMC)
electrocatalyst, which can produce CH3OH with a
maximum FE of 71.2% due to the remarkable interac-
tion of Mo and Bi. A 2D nano structure electrocatalyst of
Fe2P2S6 with a CH3OH FE of 65.2% was investigated by
Ji et al. [38] This research indicates that the Fe atom is
the active site for CH3OH production. The FeS2/NiS
prepared by the traditional hydrothermal method
performed high FE of 64% at
0.6 V, due to that the
formed active sites between FeS2 and NiS can signifi-
cantly restrain HER and facilitate CO2 ECR [39].
Sebastián et al. [57] investigated CO2 ECR over PtRu/C
and Ru/C electrocatalysts, showing that CH3OH can be
effectively produced on PtRu/C compared with Ru/C.
The studies of metal chalcogenides and carbides shed a
new insight into designing of low-cost catalysts.
Metal–organic complexes
Metaleorganic complexes have been performed for
ECR of CO2 because of their unique coordinative
structures and active center [58]. Typically, CH3OH is
the only target product by combining the Pt@Adenine-
rGO electrocatalyst and the glass carbon electrode with
a FE and current density of 85% and 0.5 mA/cm2,
respectively [40]. In addition, this kind of electro-
catalyst has a higher FE than that of Pt@histamine-rGO
(37%) [42]. Pd/polyaniline (PANI) displayed high
overpotential for HER, improving the selectivity of
CH3OH [46]. When Cu/PANI mixed with Pd/PANI
(molar ratio 1:1), FE increased from 5.4 to 10%, attrib-
uting to the synergistic effects between metals and
PANI [44]. Albo et al. [45] investigated the ECR per-
formance using different Cu-based metaleorganic
porous electrocatalysts, including [Cu3(m6-C9H3O6)2]n
[Cu3(m3-C5H4N5)2]n [Cu(m-C2H2N2S2)]n, and
[Cu0$6Zn0.4 (m-C2H2N2S2)]n. Among them [Cu3(m6-
C9H3O6)2]n and [Cu0$6Zn0.4(m-C2H2N2S2)]n showed
stable electrocatalytic performances. A molecular elec-
trocatalyst was developed by dispersing cobalt phtha-
locyanine (CoPc) on carbon nanotubes (CNTs) [41].
The result illustrated that the CH3OH FE (44%) and
current density (10.6 mA/cm2) were significantly
increased compared with the CoPc electrocatalyst. The
additional CNTs enhanced the activity of CoPc and the
electron transfer velocity.
Metal-free electrocatalysts
Ultrahigh FE has been obtained over the metal-based
electrocatalysts, for example, Co(CO3)0$5(OH)$
0.11H2O afforded a FE of 97% [47], while 68.5% for
[Fe(PP3) (MeCN)2](BF4)2 [48]. However, the rela-
tively costly price and release of metal ions during the
processes make it necessary to develop metal-free al-
ternatives. Recently, Mou et al. [49] found that the
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Recent progress on electrochemical Liu et al. 13
synergy of B and P in the boron phosphide nano-
particles promoted the binding and activating of CO2,
resulting in an outstanding FE (92.0%) for CH3OH
at
0.5 V. Owing to the high durability and wide po-
tential window, N/B codoped [59] and B-doped dia-
mond [50] were used for CO2 ECR, which could realize
the CH3OH formation with FEs of <20 and 24.3%,
respectively. The investigation of metal-free electro-
catalysts proposed a new idea for designing cheaper
electrocatalyst.
Pyridine electrocatalysts
In 1994, Seshadri et al. [60] found pyridine (Py) is an
effective homogeneous electrocatalyst for ECR of CO2
to CH3OH with FE of 30%. Since then, several publi-
cations over the Py-based electrocatalysts were reported
[61e66]. Recently, Cole et al. [51] investigated the
substituent effects in the Py-based electrocatalysts and
found that the performance of CO2 ECR generally
increased with increasing basicity and LUMO energy of
pyridinium, and also the steric effects played an
important role in catalytic behavior. In addition, pH can
greatly affect CH3OH formation [30]. The aqueous
solutions of pyridoxine [55] and 6.7-dimethyl-4-
hydroxy-2-mercaptopteridine [67e69] containing pyri-
dinyl were also developed with good selectivity for
CH3OH. However, it is difficult to separate and recycle
Py from electrolytes, and thus immobilizing homoge-
neous Py on heterogeneous supports has been proposed.
Based on this, Yang et al. [53] [54] performed CO2
reduction over the organically doped palladium and alloy
electrocatalysts with Py derivatives ([PYD]@Pd and
[PYD]@CuePt), showing high stability and reusability.
PteAu self-assembled monolayer electrode with intro-
ducing 2-pyridinethiol (2-pyridinethiol@PteAu)
displayed an outstanding performance with FE of 39%
at
0.2 V [52]. Generally, 6 molecules of 2-pyridinethiol
and 6e
participated in the reaction to form CH3OH on
the surfaces of Pt and Au, exhibiting the possibility to
realize the developing low-cost Py-based
electrocatalysts.
MOF electrocatalyst
MOF is a promising electrocatalyst for CO2 ECR due to
high surface area and unique structure. However, the
drawbacks of low conductivity and low thermal and
chemical stability in aqueous solution make the chal-
lenges for MOF application [70]. Albo et al. [43]
designed and synthesized a high reaction stability
(>5 h) and large surface area (1197e1559 m2/g)
Cu(II)eBi(III)-basedeMOF electrocatalyst for CO2
ECR to CH3OH , founding that the selectivity of
CH3OH can be adjusted by CueBi loading. Owing to
the synergic effect of CueBi (12%)-based MOF, 8.6%
FE and current density (20 mA/cm2) were achieved for
CH3OH formation.
Current Opinion in Green and Sustainable Chemistry 2020, 23:10–17
14 Green processes and technologies
Reactor configuration/electrode effect
Beyond the electrocatalyst, reactor configuration and
electrode also play an important role in CO2 ECR to
CH3OH. A mathematical model with a 20.2% deviation
compared with the experimental result for CO2 ECR to
CH3OH in a microfluidic flow cell was developed by
Kotb et al. [71] The result indicates that the CO2 mass
transfer to the cathode is the main factor in the effect of
reaction rate, increasing electrolyte flowrate and using
more conductive membranes will enhance the CO2 ECR
to CH3OH. Vennekötter et al. [72] developed a gas
diffusion electrode into a designed zero-gap assembly
membrane reactor cell. It was found that the designed
electrode and the cell can eliminate ohmic loss and
enhance the reaction efficiently. In addition, the pH
deviation between two reactor cells and the interface
between the cathode and membrane also need to be
considered to improve the CO2 ECR. Yang et al. [73]
prepared a single-atom Cu carbon membrane electrode
with the abundant through-hole structure. The formed
through-hole structure promotes to produce the effi-
cient Cu single-atom for CO2 ECR to CH3OH. High
stability of more than 50 h with a current density
of
93 mA/cm2 and 44% FE for CH3OH formation were
achieved when using this membrane as the electrode. A
biomembrane electrode of Cuechitosanepoly(vinyl)
alcohol (PVA) with high alkali resistance was fabricated
[74]. This electrode has the merits of remarkable hy-
drophilic, high conductive, good mechanical, and envi-
ronment friendly properties. A 68.05% FE of CH3OH
was acquired because of the overlayer membrane
structure of the electrode.
Challenges and perspectives
Research studies have been conducted intensively on
electrocatalysts and the effect of reactor configuration/
electrode for CO2 ECR to CH3OH. Although a large
number of developed electrocatalysts have been
applied to accelerate the production of CH3OH and
achieved a high selectively (e.g. metal oxides and
metal-free electrocatalysts), however, the large over-
potential, low current density, and stability make it
difficult to satisfy the commercial applications. More-
over, fundamental theoretical study, efficient electrode,
and large-scale integrated reactor development are still
limited. The future research efforts may focus on (1)
developing new complex electrocatalysts (e.g. hybrid
metal, metal oxides) and electrocatalyst assemblies
(e.g. 2D/3D nano materials) to increase the CO2
reduction active sites; (2) exploration of new low-cost
metal-free electrocatalysts; (3) designing more stable
electrocatalysts with more desirable active sites, which
are of importance to accelerate the CO2 reduction and
the CH3OH selectivity; (4) designing high stability and
conductivity MOF electrocatalysts; and (5) develop-
ment of the large-scale integrated reactor, including
high efficient buffered system, high conductivity
Current Opinion in Green and Sustainable Chemistry 2020, 23:10–17
membrane material, and large surface area electrode
(e.g. gas diffusion electrode, single-atom membrane,
and bioconductive membrane electrodes). To under-
stand CO2 ECR steps, the rate determining factors and
complete pathways, as well as theoretical calculations
need to be further developed.
Conflict of interest statement
Nothing declared.
Acknowledgments
This work is financially supported by Carl Tryggers Stiftelse foundation
(No. 18:175). F.L. and X.J. thank the financial support from the Swedish
Energy Agency (No. P47500-1). X.J. also thanks the financial support from
the K. C. Wang Education Foundation (No. GJTD-2018-04). X.Z. thanks
the financial supports from the National Natural Science Foundation of
China (No. 21838010) and the DNL Cooperation Fund, CAS (No. DNL
180406).
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