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Progress in Chemistry 2022, Vol. 34 Issue (3): 533-546 DOI: 10.7536/PC210352 Previous Articles   Next Articles

• Review •

Transition Metal Single-Atom Electrocatalysts for CO2 Reduction to CO

Shujin Shen, Cheng Han(), Bing Wang, Yingde Wang()   

  1. Science and Technology on Advanced Ceramic Fibers and Composites Laboratory, College of Aerospace Science and Engineering, National University of Defense Technology, Changsha 410073, China
  • Received: Revised: Online: Published:
  • Contact: Cheng Han, Yingde Wang
  • Supported by:
    National Natural Science Foundation of China(51773226); National Natural Science Foundation of China(61701514)
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Electrocatalytic carbon dioxide reduction (ECR) technology offers a potential strategy to achieve the goal of “carbon neutralization”. Transition metal single-atom catalysts have attracted much attention in ECR due to their adjustable electronic structure, high atom utilization and uniform active sites. This review firstly introduces the advantages of transition metal single-atom catalysts in CO2 reduction, especially in selective CO production. Then, the recent progress on controlling the active sites as well as the catalysis selectivity over Fe, Co, Ni and other single-atom electrocatalysts are reviewed, with special emphasis on the intermediate process control of proton coupled CO2 reduction to CO reaction path. Finally, the development direction of transition metal single-atom catalysts in ECR is briefly prospected to provide guidance and reference for promoting their large-scale application.

Contents

1 Introduction

2 The advantages of single-atom electrocatalysts for CO2 reduction to CO

3 Single-atom electrocatalysts for CO2 reduction to CO

3.1 Ni single-atom electrocatalysts for CO2 reduction to CO

3.2 Co single-atom electrocatalysts for CO2 reduction to CO

3.3 Fe single-atom electrocatalysts for CO2 reduction to CO

3.4 Other single-atom electrocatalysts for CO2 reduction to CO

4 The mechanism research of electrocatalytic CO2 reduction to CO

5 Conclusion and outlook

Key words: single-atom catalysts, carbon dioxide reduction, electrocatalysis
Fig.1 (a) Correlation between particle size with surface free energy and specific activity[44], Copyright 2013, American Chemical Society; (b) Correlation between geometric structure and electronic structure with particle size[45]. Copyright 2018, The Royal Society of Chemistry
Fig.2 Schematic of the reaction steps of electrocatalytic CO2 to CO reduction[46]. Copyright 2017, Elsevier
Table 1 Electrocatalytic performance of recently reported single-atom catalysts for electrocatalytic CO2 to CO
Catalysts Active site structure Potential
/vs. RHE		 jCO
/mA·cm-2		 FECO Electrolyte Loading
/mg·cm-2		 ref
NiN-GS Ni-NxCy -0.70 V 4 93.2% 0.1 mol/L KHCO3 0.2 46
Ni-N4-C Ni-N4 -0.81 V 28.6 99% 0.5 mol/L KHCO3 0.2 59
H-CPs Ni-NxCy -1.0 V 48.66 97% 0.5 mol/L KHCO3 3.5 61
NiSA-Nx-C Ni-N2 -0.80 V ~15 98% 0.5 mol/L KHCO3 0.6 60
NiSA-Nx-C Ni-N3 -0.80 V ~7 ~90% 0.5 mol/L KHCO3 0.6 60
Ni-N3-V SAC Ni-N3 -0.80 V 48 94% 0.5 mol/L KHCO3 - 84
Ni-N4 Ni-N4 -0.8 V 10 ~78% 0.5 mol/L KHCO3 - 84
Ni-N3-C Ni-N3 -0.65 V ~7 95.6% 0.5 mol/L KHCO3 0.6 82
Ni-N4-C Ni-N4 -0.65 V ~4.5 89.2% 0.5 mol/L KHCO3 0.6 82
C-Zn1Ni4-ZIF-8 Ni-N4 -1.13 V 44.1 94% 0.5 mol/L KHCO3 0.088 43
A-Ni-NG Ni-N4 -0.61 V 31.5 97% 0.5 mol/L KHCO3 0.4 90
Ni-CNT-CC Ni-N4 -0.60 V 32.3 99% 0.5 mol/L KHCO3 0.5 91
NiSA/PCFM Ni-N4 -0.70 V 56.1 96% 0.5 mol/L KHCO3 1 82
CoPc Co-N4 -0.80 V ~10 99% 0.5 mol/L KHCO3 2 63
Co-N5/HNPCS Co-N5 -0.79 V 10.2 99.3% 0.2 mol/L NaHCO3 - 64
Co-N2 Co-N2 -0.63 V 18.1 94% 0.5 mol/L KHCO3 0.4 68
Co-N3 Co-N3 -0.63 V 2.5 ~68% 0.5 mol/L KHCO3 0.4 68
Co-N4 Co-N4 -0.63 V 0 0 0.5 mol/L KHCO3 0.4 68
Fe3+-N-C Fe-N4 -0.47 V 20.0 >90% 0.5 mol/L KHCO3 0.6 69
Fe1NC/S1-1000 Fe-N3 -0.50 V 6.4 96% 0.5 mol/L KHCO3 1 71
FeN/CNT@GNR Fe-N4 -0.76 V 22.7 96% 0.5 mol/L KHCO3 0.8 57
DNG-SAFe Fe-N4 -0.95 V 33 90% 0.1 mol/L KHCO3 1 85
Fe-N/CNT Fe-N4 -0.60 V ~5 95.5% 0.5 mol/L KHCO3 1 86
ZnNx/C Zn-N4 -0.43 V 4.8 95% 0.5 mol/L KHCO3 1 72
Bi SAs/NC Bi-N4 -0.50 V 4 97% 0.1 mol/L NaHCO3 - 79
Cu-N2/GN Cu-N2 -0.50 V 1.7 81% 0.1 mol/L KHCO3 0.5 80
Cu-N4/GN-800 Cu-N4 -0.50 V 0.74 62% 0.1 mol/L KHCO3 0.5 80
Mn-C3N4/CNT Mn-N3 -0.55 V 14.0 98.8% 0.5 mol/L KHCO3 1 81
Fig.3 (a) Different atomic configurations, (b) the corresponding free energy diagram of CO2 to CO conversion of Ni-C/Ni-N-C catalyst[46], Copyright 2017, Elsevier; (c) The FECO of Ni-N4-C catalyst[60]; (d) Schematic illustration and (e) jCO of H-CPs compared with those of others[61]. Copyright 2019, Elsevier
Fig.4 (a) Projected density of states for crucial structures from *CO and *COOH adsorption and (b) calculated free-energy diagram of MePc catalyst[63], Copyright 2018, Wiley-VCH; (c) Schematic illustration and (d) LSV curves of Co-N5/HNPCS[64], Copyright 2018, American Chemical Society; (e) The EXAFS, (f) the corresponding free energy diagram of CO2 to CO conversion, (g) jtotal of Co-N2, Co-N3 and Co NPs of Co-Nx catalysts[68]. Copyright 2018, Wiley-VCH
Fig.5 (a) jCO, (b,c) Operando XAS characterization of Fe3+-N-C and Fe2+-N-C catalysts[69], Copyright 2019, The American Association for the Advancement of Science; (d) Schematic illustration of the support size, (e) Correlation between FECO and ESA as well as jCO and ESA of Fe1NC/SX-1000[71], Copyright 2020, Wiley-VCH; (f) Schematic illustration of location sites of Fe-N4, (g) Structural evolution from CNTs to CNT@GNR[56]. Copyright 2020, American Chemical Society
Fig.6 (a) HAADF-STEM image and EXAFS, (b) free energy of ECR to CO of ZnN4/C catalyst[72], Copyright 2018, Wiley-VCH; (c) EDS mapping image, (d) free energy of ECR to CO of Bi SAs/NC[79], Copyright 2019, American Chemical Society; (e) EXAFS spectra, (f) FECO and (g) free energy of ECR to CO of Cu-Nx/GN[80]. Copyright 2020, Wiley-VCH
Fig.7 (a) Operando XANES, (b) valence band spectra of A-Ni-NG before (black line) and after (red line) CO2 gas exposure, and after desorption of CO2 (blue line) of A-Ni-NG, (c) proposed structural evolution of the active site in ECR. E F 1 and E F 2 are Fermi levels of A-Ni-NG before and after formation of Ni-C O 2 δ -, respectively. 1πg and 2πu are CO2 molecular orbitals[92], Copyright 2018, Springer Nature; (d) Operando Raman spectra of Ni-TAPc acquired in Ar or CO2 saturated KHCO3 solution[93]. Copyright 2019, Wiley-VCH
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