Chinese Journal of Catalysis ›› 2021, Vol. 42 ›› Issue (6): 920-937.DOI: 10.1016/S1872-2067(20)63718-4
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Jing Dua,†, Yuan-Yuan Mad,†, Huaqiao Tana,*(), Zhen-Hui Kangb,c,#(), Yangguang Lia,$()
Received:
2020-07-22
Accepted:
2020-09-03
Online:
2021-06-18
Published:
2021-01-30
Contact:
Huaqiao Tan,Zhen-Hui Kang,Yangguang Li
About author:
$E-mail: liyg658@nenu.edu.cn†These authors contributed equally.
Supported by:
Jing Du, Yuan-Yuan Ma, Huaqiao Tan, Zhen-Hui Kang, Yangguang Li. Progress of electrochemical CO2 reduction reactions over polyoxometalate-based materials[J]. Chinese Journal of Catalysis, 2021, 42(6): 920-937.
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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(20)63718-4
Possible half-reactions in electrochemical CO2RRs | Electrode potentials (V vs. SHE) |
---|---|
CO2 (g) + e- → *COO- | -1.90 |
CO2 (g) + 2H+ + 2e- → CO (g) + H2O (l) | -0.52 |
CO2 (g) + 8H+ + 8e- → CH4 (g) + 2H2O (l) | -0.24 |
2CO2 (g) + 12H+ + 12e- → C2H4 (g) + 4H2O (l) | -0.34 |
CO2 (g) + 2H+ + 2e- → HCOOH (l) | -0.61 |
CO2 (g) + 4H+ + 4e- → HCHO (l) + H2O (l) | -0.51 |
CO2 (g) + 6H+ (l) + 6e- → CH3OH (l) + H2O (l) | -0.38 |
2H+ + 2e- → H2 (g) | -0.42 |
Table 1 Electrochemical potentials of reactions that may occur during electrocatalytic CO2 reduction in aqueous solutions.
Possible half-reactions in electrochemical CO2RRs | Electrode potentials (V vs. SHE) |
---|---|
CO2 (g) + e- → *COO- | -1.90 |
CO2 (g) + 2H+ + 2e- → CO (g) + H2O (l) | -0.52 |
CO2 (g) + 8H+ + 8e- → CH4 (g) + 2H2O (l) | -0.24 |
2CO2 (g) + 12H+ + 12e- → C2H4 (g) + 4H2O (l) | -0.34 |
CO2 (g) + 2H+ + 2e- → HCOOH (l) | -0.61 |
CO2 (g) + 4H+ + 4e- → HCHO (l) + H2O (l) | -0.51 |
CO2 (g) + 6H+ (l) + 6e- → CH3OH (l) + H2O (l) | -0.38 |
2H+ + 2e- → H2 (g) | -0.42 |
Fig. 1. Kinetic volcano plot for CO evolution at a 0.35 V overpotential from the (211) step of TMs. The TMs fall along a trendline that does not pass over the top of the volcano. However, the noble metals occupy near-optimum positions along this trend line. The speci?c CO evolution current for the ChCODH II and MbCODH enzyme models is comparable or better than those of the noble metals. Reprinted with the permission of Ref. [75]. Copyright 2013, American Chemical Society.
Fig. 2. (a) Visible spectra of tetraheptylammonium salts of (I) α-[SiW11O39Co(OH2)]6-, (II) α-[SiW11O39Co(_)]6-, and (III) a-[SiW11O39Co(CO2)]6- in toluene. (b) Infrared spectrum of the tetraheptylammonium salt of α-[SiW11O39Co(CO2)]6- in CCl4. The two peaks marked with arrows appear after the CO2 is bubbled, and are assigned to vibrations of CO2 complexed to cobalt. (c) Difference spectrum between α-[SiW11O39Co(CO2)]6- and α-[SiW11O39Co(_)]6-. The peak at 2335 cm-1 originates from the CO2 gas dissolved in the solvent. (d) 13C NMR spectra of 0.1 M α-[SiW11O39Co(CO2)]6- in toluene at temperatures from -40 °C to + 35 °C. (e-h) Proposed hypothetical bonding modes for CO2 with cobalt in α-[SiW11O39Co(CO2)]6-, stabilized by hydrogen bonding utilizing both hydrogen atoms from water. Reprinted with the permission of Ref. [88]. Copyright 1998, American Chemical Society (ACS).
Fig. 3. Synthesis of the organometallic derivative [α-H2PW11O39{RhIIICp*(OH2)}]3- (the POM skeleton is displayed in polyhedral representation). Reprinted with the permission of Ref. [98]. Copyright 2019 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.
Fig. 4. (a) Structural representation of Mn(III), Ni(II), and Zn(II) μ-(meso-5,10,15,20-tetra(pirydil)porphyrin)tetrakis{bis(bipyridine)chloride ruthenium(II)}; Linear sweep voltammogram of bare ITO electrode (b), [MnIIITRP]5+/[SiW12O40]4- multilayer modi?ed electrode (c) [ZnIITRP]4+/[SiW12O40]4- multilayer modi?ed electrode (d) and [NiIITRP]4+/[SiW12O40]4- multilayer modi?ed electrode the in presence (solid line) and absence (dash line) of CO2 and 0.1 M NaClO4 solution at 5 mV s-1 (e). Reprinted with the permission of Ref. [100]. Copyright 2013 Elsevier Ltd.
Electrode | Products and TOF (s-1) | ||
---|---|---|---|
CO | HCOOH | CH3OH | |
[MnIIITRP]5-/[SiW12O40]4-/ITO | N.D.a | 0.48 b | 0.023 |
[ZnIITRP]5-/[SiW12O40]4-/ITO | 0.0037 | N.D. a | 8.2 |
[NiIITRP]5-/[SiW12O40]4-/ITO | 0.24 | 0.083 | N.D. a |
Table 2 Electrocatalytic CO2RR activity and products of [MTRP]/[SiW12O40]/ITO electrodes.
Electrode | Products and TOF (s-1) | ||
---|---|---|---|
CO | HCOOH | CH3OH | |
[MnIIITRP]5-/[SiW12O40]4-/ITO | N.D.a | 0.48 b | 0.023 |
[ZnIITRP]5-/[SiW12O40]4-/ITO | 0.0037 | N.D. a | 8.2 |
[NiIITRP]5-/[SiW12O40]4-/ITO | 0.24 | 0.083 | N.D. a |
Fig. 5. (a) Schematic illustration of the structures of M-PMOFs (M = Co, Fe, Ni, Zn). M-PMOFs consist of 4-connection TCPP linkers and zigzag POM chains; (b) Linear sweep voltammetry (LSV) curves of M-PMOFs; (c) Faradaic ef?ciencies for CO; (d) Durability test of Co-PMOF at a potential of -0.8 V vs. RHE. Reprinted with the permission of Ref. [37]. Copyright 2018, Springer Nature.
Fig. 6. (a) Schematic diagram of the reaction mechanism induced by POM-MnL; (b) TEM image of SiW12-MnL/KB (inset: HR-TEM image of SiW12-MnL/KB, scale bar: 5 nm); (c) The CV curves for MnL/KB, CsSiW12/KB, and SiW12-MnL/KB in 0.5 mol L-1 N2-saturated KHCO3 at a 0.05 V s-1 scan rate; (d) The LSV curves of SiW12-MnL/KB and MnL/KB in 0.5 M N2-(black curve) or CO2-(red curve) saturated KHCO3 electrolyte; (e) The FE for CO at di?erent potentials for MnL/KB and SiW12-MnL/KB (the line is drawn only to guide the eye); (f) The FEs for CO and H2 at the overpotential of the highest FE for CO of MnL/KB and POM-MnL/KB. Reprinted with the permission of Ref. [101]. Copyright 2020, Royal Society of Chemistry (RSC).
Fig. 7. Square reaction scheme representing the interaction between the reduced forms of [α-SiW12O40]4- and CO2 during electrochemical reduction. [α-SiW12O40]4- is represented as SiW4- for convenience. Reprinted with the permission of Ref. [102]. Copyright 2016 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim.
Fig. 8. The Faradaic e?ciencies of products of In cathode in SiW9V3 (a) and SiW11Mn (b) electrolyte. (c) XPS spectra of In 3d for the indium electrode before and after electrolysis with 1 and 12 h. (d) XPS spectra of W 4f for the indium electrode after 1 h electrolysis. (e) The FTIR spectroscopy characterization for the 2 mM SiW9V3-0.1 M Na2SO4 electrolyte during electrolysis, in which the peak at 2071 cm-1 corresponds to the adsorbed CO*. (f) Current density with electrolysis time at different potential for 1 h; The inset is the current density with electrolysis time at -1.15 V vs. Ag/AgCl for 12 h. Reprinted with the permission of Refs. [103,104]. Copyright 2020 Elsevier Ltd.
Fig. 9. (a) SEM images of Ag-PMo nanocomposite-modi?ed ITO glasses; (b) TEM images of Ag-PMo nanocomposites, inset: Schematic diagram of Ag-PMo catalytic CO2 reduction; (c) Comparison of cyclic voltammograms obtained at an Ag-PMo nanocomposite-modi?ed GC electrode in DMF (0.1 M [n-Bu4N]PF6) with 0.5% (v/v) added H2O under a CO2 (black line) or a N2b(red line) atmosphere (Scan rate: 100 mV s-1); (d) Potentiostatic i-t curves obtained at an Ag-PMo nanocomposite modified GC electrode in DMF (0.1 M [n-Bu4N]PF6) with 0.5% (v/v) added water under CO2 or N2 atmospheres. Applied potential: -1.9 V vs. Fc0/+. Reprinted with the permission of Ref. [105]. Copyright 2018, American Chemical Society.
Fig. 10. (a) SEM image of the film deposited on an FTO electrode in aqueous 0.25 M HNO3 solutions containing 1.0 mM Bi(NO3)3; (b) Atomic force microscopy (AFM) image and height profile of Bi-PMo nanosheets; (c) Raman spectra of Bi-PMo nanosheets before (black) and after electrolysis (red), and H3PMo12O40 (blue); (d,e) High-resolution XPS spectra recorded for Mo 3d and Bi 4f regions of the Bi-PMo nanosheets; (f) Cyclic voltammograms obtained for Bi-PMo nanosheet (solid lines) and Bi nano-dendrite (dash lines) modified GC electrodes in CO2-(black) or N2-(red) saturated 0.5 M NaHCO3 aqueous solutions, scan rate: 0.1 V s-1; (g) Faradaic efficiencies for formate produced on Bi-PMo nanosheets (black) and Bi nano-dendrites (red) at various applied potentials in CO2-saturated 0.5 M NaHCO3 solutions; (h) Long term stability study of Bi-PMo nanosheets during controlled potential electrolysis at -0.86 V vs. RHE in a CO2-saturated 0.5 M NaHCO3 solution; (i) Tafel plots obtained for Bi-PMo nanosheets (black) and Bi nano-dendrites (red). Reprinted with the permission of Ref. [106]. Copyright 2019 Wiley‐VCH Verlag GmbH & Co. KGaA, Weinheim.
Electrocatalyst | Electrolyte | Potential | Principal product | FE (%) | TON | Ref. |
---|---|---|---|---|---|---|
(TOA)6[α-SiW11O39Co(_)] | CH2Cl2 | -1.5 V vs. Hg2Cl2/Hg | CO | 18 | — | [ |
(TBA)3[H2PW11O39{RhIIICp* (OH2)}] | CH3CN | -1.8 V vs. Hg2Cl2/Hg | HCOOH | 4.5 | 0.8 | [ |
[Cp*RhIII(bpy)Cl]+ | CH3CN | -1.8 V vs. Hg2Cl2/Hg | HCOOH | 60 | 18 | [ |
[Mn(III)TRP]5+/[SiW12O40]4-/ITO | 0.1 M NaClO4 | -0.8 V vs. Ag/AgCl | HCOOH | — | 1.06 × 104 | [ |
[Zn(II)TRP]4+/[SiW12O40]4-/ITO | 0.1 M NaClO4 | -0.8 V vs. Ag/AgCl | Methanol | — | 1.76 × 105 | [ |
[Ni(II)TRP]5+/[SiW12O40]4-/ITO | 0.1 M NaClO4 | -0.8 V vs. Ag/AgCl | CO | — | 3.85 × 103 | [ |
[Ni(II)TRP]5+ | DMF | -0.8 V vs. SHE | CO | — | — | [ |
Co-PMOF | 0.5 M KHCO3 | -0.8 V vs. RHE | CO | 98.7 | 7693 | [ |
Fe-PMOF | 0.5 M KHCO3 | -0.8 V vs. RHE | CO | 28.8 | — | [ |
Ni-PMOF | 0.5 M KHCO3 | -0.8 V vs. RHE | CO | 18.5 | — | [ |
Zn-PMOF | 0.5 M KHCO3 | -0.8 V vs. RHE | CO | 0.95 | — | [ |
Co-TMCP | 0.5 M KHCO3 | -0.9 V vs. RHE | CO | ~50 | — | [ |
MOF-525(Co) | 0.5 M KHCO3 | -0.8 V vs. RHE | CO | 47.9 | — | [ |
CoPPC/CNT | 0.5 M KHCO3 | -0.58 V vs. RHE | CO | ~90 | — | [ |
SiW12-MnL/KB | 0.5 M KHCO3 | -0.72 V vs. RHE | CO | 95 | — | [ |
PW12-MnL/KB | 0.5 M KHCO3 | -0.72 V vs. RHE | CO | 80 | — | [ |
PMo12-MnL/KB | 0.5 M KHCO3 | -0.52 V vs. RHE | CO | 65 | — | [ |
MnL/KB | 0.5 M KHCO3 | -0.72 V vs. RHE | CO | 65 | — | [ |
[Mn(L)(CO)3Br (MnL) | CH3CN | -1.7 V vs. Ag/Ag+ | CO | 85 | 34 | [ |
AgNC@BSA | 1 mM [Bu4N]4[α-SiW12 O40] in DMF | -2.32 V vs. Fc0/+ | CO | 75.6 | — | [ |
Ag-PMo | DMF | -1.9 vs. Fc0/+ | CO | 90 ± 5 | — | [ |
Ag/N-doped graphene/carbon foam | 0.1 M KHCO3 | -0.6 V vs. RHE | Ethanol | 85.2 | — | [ |
Ag QDDCs | 0.5 M KHCO3 | -0.3 V vs. RHE | CO | 95 | — | [ |
Indium sheet | 2 mM SiW9V3 + 0.1 M Na2SO4 | -1.15 vs. Ag/AgCl | CH3COOH | 96.5 | — | [ |
Indium sheet | 2 mM SiW11Mn+ 0.1 M Na2SO4 | -1.0 V vs. RHE | CH3COOH | 72.1 | — | [ |
In2O3-rGO | 0.1 M KHCO3 | -1.2 V vs. RHE | HCOOH | 84.6 | — | [ |
Sulfur-doped indium | 0.5 M KHCO3 | -0.98 V vs. RHE | HCOOH | 93 | — | [ |
Bi-PMo nanosheets | 0.5 M KHCO3 | -0.86 V vs. RHE | CH3COOH | 93 | — | [ |
Bi nano-dendrites | 0.5 M KHCO3 | -0.96 V vs. RHE | CH3COOH | 81 | — | [ |
Bi nanoflakes | 0.1 M KHCO3 | -0.6 V vs. RHE | HCOOH | ~100 | — | [ |
Table 3 Performance of major POM-based electrocatalysts and other representative electrocatalysts used in electrocatalytic CO2RRs.
Electrocatalyst | Electrolyte | Potential | Principal product | FE (%) | TON | Ref. |
---|---|---|---|---|---|---|
(TOA)6[α-SiW11O39Co(_)] | CH2Cl2 | -1.5 V vs. Hg2Cl2/Hg | CO | 18 | — | [ |
(TBA)3[H2PW11O39{RhIIICp* (OH2)}] | CH3CN | -1.8 V vs. Hg2Cl2/Hg | HCOOH | 4.5 | 0.8 | [ |
[Cp*RhIII(bpy)Cl]+ | CH3CN | -1.8 V vs. Hg2Cl2/Hg | HCOOH | 60 | 18 | [ |
[Mn(III)TRP]5+/[SiW12O40]4-/ITO | 0.1 M NaClO4 | -0.8 V vs. Ag/AgCl | HCOOH | — | 1.06 × 104 | [ |
[Zn(II)TRP]4+/[SiW12O40]4-/ITO | 0.1 M NaClO4 | -0.8 V vs. Ag/AgCl | Methanol | — | 1.76 × 105 | [ |
[Ni(II)TRP]5+/[SiW12O40]4-/ITO | 0.1 M NaClO4 | -0.8 V vs. Ag/AgCl | CO | — | 3.85 × 103 | [ |
[Ni(II)TRP]5+ | DMF | -0.8 V vs. SHE | CO | — | — | [ |
Co-PMOF | 0.5 M KHCO3 | -0.8 V vs. RHE | CO | 98.7 | 7693 | [ |
Fe-PMOF | 0.5 M KHCO3 | -0.8 V vs. RHE | CO | 28.8 | — | [ |
Ni-PMOF | 0.5 M KHCO3 | -0.8 V vs. RHE | CO | 18.5 | — | [ |
Zn-PMOF | 0.5 M KHCO3 | -0.8 V vs. RHE | CO | 0.95 | — | [ |
Co-TMCP | 0.5 M KHCO3 | -0.9 V vs. RHE | CO | ~50 | — | [ |
MOF-525(Co) | 0.5 M KHCO3 | -0.8 V vs. RHE | CO | 47.9 | — | [ |
CoPPC/CNT | 0.5 M KHCO3 | -0.58 V vs. RHE | CO | ~90 | — | [ |
SiW12-MnL/KB | 0.5 M KHCO3 | -0.72 V vs. RHE | CO | 95 | — | [ |
PW12-MnL/KB | 0.5 M KHCO3 | -0.72 V vs. RHE | CO | 80 | — | [ |
PMo12-MnL/KB | 0.5 M KHCO3 | -0.52 V vs. RHE | CO | 65 | — | [ |
MnL/KB | 0.5 M KHCO3 | -0.72 V vs. RHE | CO | 65 | — | [ |
[Mn(L)(CO)3Br (MnL) | CH3CN | -1.7 V vs. Ag/Ag+ | CO | 85 | 34 | [ |
AgNC@BSA | 1 mM [Bu4N]4[α-SiW12 O40] in DMF | -2.32 V vs. Fc0/+ | CO | 75.6 | — | [ |
Ag-PMo | DMF | -1.9 vs. Fc0/+ | CO | 90 ± 5 | — | [ |
Ag/N-doped graphene/carbon foam | 0.1 M KHCO3 | -0.6 V vs. RHE | Ethanol | 85.2 | — | [ |
Ag QDDCs | 0.5 M KHCO3 | -0.3 V vs. RHE | CO | 95 | — | [ |
Indium sheet | 2 mM SiW9V3 + 0.1 M Na2SO4 | -1.15 vs. Ag/AgCl | CH3COOH | 96.5 | — | [ |
Indium sheet | 2 mM SiW11Mn+ 0.1 M Na2SO4 | -1.0 V vs. RHE | CH3COOH | 72.1 | — | [ |
In2O3-rGO | 0.1 M KHCO3 | -1.2 V vs. RHE | HCOOH | 84.6 | — | [ |
Sulfur-doped indium | 0.5 M KHCO3 | -0.98 V vs. RHE | HCOOH | 93 | — | [ |
Bi-PMo nanosheets | 0.5 M KHCO3 | -0.86 V vs. RHE | CH3COOH | 93 | — | [ |
Bi nano-dendrites | 0.5 M KHCO3 | -0.96 V vs. RHE | CH3COOH | 81 | — | [ |
Bi nanoflakes | 0.1 M KHCO3 | -0.6 V vs. RHE | HCOOH | ~100 | — | [ |
Fig. 11. The DFT calculation and proposed reaction mechanism. (a) The free energy diagrams of CO2 reduction to CO for POM (orange), Co-TCPP (green), and Co-PMOF (pink). The rate-determining step and the corresponding free energy of each material are indicated (Note that an asterisk represents a surface-active site for reaction); (b) Comparison of the free energy of each elementary reaction (ΔG1, ΔG2, and ΔG3 represent the free energy of *COOH formation, *CO formation, and CO desorption, respectively) during CO2RRs for Co-PMOF, Fe-PMOF, Ni-PMOF, and Zn-PMOF, respectively; (c,d) Proposed mechanism scheme for the CO2RRs on Co-PMOF (POMs as electron-donors, porphyrins as charge transfer ligands, and TMs as electron-acceptors). Reprinted with the permission of Ref. [37]. Copyright 2018, Springer Nature.
Fig. 12. (a) Computed frontier orbitals (compositions and energies) for MnL, SiW12-MnL, PW12-MnL, and PMo12-MnL (the green lines represent the unoccupied molecular orbitals (MO) contributed by MnL in POM-MnL); (b) The electronic con?gurations for the di?erent reduction degree states of SiW12-MnL, PW12-MnL, and PMo12-MnL; (c) The transient photovoltage curves of powder POM-MnL and MnL; (d) Potential energy surfaces for H+ and CO2 addition to the respective active CO2 and H adducts. Reprinted with the permission of Ref. [101]. Copyright 2020, Royal Society of Chemistry (RSC).
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