Research Prospect of Single Atom Catalysts Towards Electrocatalytic Reduction of Carbon Dioxide

doi:10.19894/j.issn.1000-0518.210244

Chinese Journal of Applied Chemistry ›› 2022, Vol. 39 ›› Issue (6): 871-887.DOI: 10.19894/j.issn.1000-0518.210244

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Research Prospect of Single Atom Catalysts Towards Electrocatalytic Reduction of Carbon Dioxide

Chao ZHANG()

Aerospace Research Institute of Materials ＆ Processing Technology，Beijing 100076，China

Received:2021-05-18 Accepted:2021-10-13 Published:2022-06-01 Online:2022-06-27
Contact: Chao ZHANG
About author:zhchao@buaa.edu.cn
Supported by:
the National Natural Science Foundation of China(51472015)

Abstract

Abstract:

Electrocatalytic reduction of CO₂ can directly convert CO₂ and water into carbonous products by renewable electric energy under ambient conditions， which has a promising application prospect. However， its application is still limited by the sluggish cathode reaction. It is well-known that the size of the catalyst has a great influence on its activity. Reducing the metal catalyst to nanoscale particles can significantly increase the number of exposed active sites and its intrinsic activity， thus improve its catalytic performance. Furthermore， when the size of the catalyst is reduced to the level of single atom dispersion， the activity of the catalyst can be significantly improved. In recent years， single atom catalysts have become research hotspot in the field of electrocatalytic CO₂ reduction owing to their unique geometrical structures and electrical states. In this review， we summarize and review the research on the single atom catalysts towards electrocatalytic reduction of CO₂， and also analyze and discuss the difficulties and further research directions in the future.

Key words: Single atom catalysts, CO₂ reduction, Electrocatalysis, Active sites, Reaction intermediates

CLC Number:

O643.3

Chao ZHANG. Research Prospect of Single Atom Catalysts Towards Electrocatalytic Reduction of Carbon Dioxide[J]. Chinese Journal of Applied Chemistry, 2022, 39(6): 871-887.

Figures/Tables 17

Fig.1 The structure-activity relationship of various organic products produced by CO2 reduction reaction catalyzed by different SACs

Fig.2 Preparation process of CuSA/THCF：（a） Preparation of CuSA/THCF sample contains synthesis of ZIF precursors， electrospun and high-temperature treatment steps；（b） Digital photos of CuSA-THCF show the flexible of the sample［17］

Fig.3 Structural characterization of Cu single atoms：（a） XRD patterns；（b） High-resolution N1s spectral of CuSA/THCF；（c） High-resolution Cu2p spectral of CuSA/THCF show the unsaturated states of Cu atoms；（d） XANES spectral of CuSA/THCF， Cu foil and CuO；（e） EXAFS spectral of CuSA/THCF， Cu foil and CuO （f） EXAFS fitting results of CuSA/THCF confirm the existence of Cu-N4 coordinations ［17］

Fig.4 Characterization of NiSA/N-C：（a） Preparation process of NiSA/N-C；（b） TEM image of NiSA/N-C；（c） HAADF-STEM image of NiSA/N-C；（d） SAED patterns of NiSA/N-C；（e and f） HAADF-STEM images of NiSA/N-C with different magnifications with single atom Ni marked by red circles；（g） EDS results and the corresponding elemental mapping of Ni， N and C species［22］

Fig.5 Characterization of Ni/Fe-N-C：（a and b） High-resolution XPS N1s spectral （a） and XRD patterns （b） of Ni/Fe-N-C， Fe-N-C， Ni-N-C and N-C samples；（c） K-edge XANES spectral of Ni/Fe-N-C， Fe-N-C， Ni-N-C and N-C samples；（d） EXAFS spectral of Ni/Fe-N-C， Fe-N-C， Ni-N-C and N-C samples；（e） EXAFS fitting results of Ni/Fe-N-C sample show the presence of Ni-N and Ni-Fe coordination［22］

Fig.6 Characterization of Mo2TiC2T x -PtSA sample：（a） TEM image of Mo2TiC2T x -PtSA sample；（b） HAADF-STEM image of Mo2TiC2T x -PtSA sample；（c） HAADF-STEM images and their corresponding nanostructure fitting result confirm the existence of single atom Pt；（d） STEM-EDS images and corresponding elemental mapping results；（e） EXAFS spectra of Mo2TiC2T x -PtSA， Pt foil and PtO2 samples；（f） EXAFS spectra of Mo2TiC2T x -PtSA， Pt foil and PtO2 samples［25］

Fig.7 Electrocatalytic CO2 reduction properties of Cu-CeO2-4%：（a） CV curves of Cu-CeO2， CeO2 and Cu samples；（b） Faradaic efficiencies of various CO2 reduction products catalysis by Cu-CeO2-4% under different potentials［26］

Fig.8 In situ high-temperature-shockwave synthesis of HT-SAs：（a） The schematic diagram shows the HT-SA synthesis and dispersion process；（b） Temperature evolution during the shockwave synthesis and a detailed heating/cooling pattern；（c） A ten-pulse shock heating pattern demonstrates the uniform temperature in each cycle with a high-temperature on state and a low temperature off state［27］

Fig.9 Preparation of Fe SAs/GO involves two steps： 1） Absorbed GO on the surface of Fe foam and formed Fe—O bonds with Fe atoms on the surface； 2） By mechanical force， GO is separated from the foam Fe surface. Using the principle that the strength of Fe—O is greater than the strength of Fe—Fe metal bond， single atomic Fe is formed［28］

Fig.10 Characterization of single atom Co catalyst：（a） EXAFS spectra of Co-N2， Co-N3 and Co-N4 samples；（b） XANES spectra of Co-N2， Co-N3 and Co-N4 samples［33］

Fig.11 In situ catalytic mechanism illustration of Ni-TAPc catalyst：（a and b） Raman spectra of Ni-TAPc collected on an Au electrode at various potentials （vs.RHE） in 0.5 mol/L KHCO3 aqueous solution at room temperature under an atmosphere of （c） Ar （1.01×105 Pa） and （d） CO2 （1.01×105 Pa）；（c） Reaction pathway of CO2 reduction to CO on the Ni SAC［37］

Fig.12 Characterization of single atom Ni decorated N-doped graphene：（a） SEM image of A-Ni-NG；（b） TEM image of A-Ni-NG；（c） XRD patterns of Ni-NG， A-Ni-NSG and Ni-NG；（d） HAADF-STEM image of A-Ni-NG；（e） Elemental contents of A-Ni-NG， inset： high-resolution XPS N1s spectra；（f） High-resolution Ni2p spectra of different samples［47］

Fig.13 Electrocatalytic CO2 reduction results of A-Ni-NG：（a） LSV curves of different samples in 0.5 mol/L KHCO3 electrolyte at the rotation rate of 1600 r/min；（b） CO product Faradaic efficiencies of different samples under different potentials；（c） Comparations of TOF results of A-Ni-NG catalyst with a series of reported catalysts；（d） Total reduction current densities and CO product current densities of A-Ni-NG for 100 h long-term tests［47］

Fig.14 （a） Free energy profiles （at -0.78 V（vs.RHE）） for CO2 activation on Cu， Cu@Cu2O and APC of Cu10-Cu1x+ on Pd10Te3 nanowires；（b） Configurations of physisorbed CO2 and chemisorbed CO2 on Cu-APC［51］

Fig.15 Characterization of AD-Sn/N-1000 sample：（a） Bright-field STEM image of AD-Sn/N-1000 sample；（b－d） Dark-field STEM image of AD-Sn/N-1000 sample；（e） Elemental mapping images of AD-Sn/N-1000 sample；（f） High-resolution XPS Sn3d spectral of AD-Sn/N-1000 and Sn-CF1000［53］

Fig.16 Electrocatalytic properties of AD-Sn/N-C1000 sample：（a） Current densities curves of AD-Sn/N-C1000 and Sn-CF1000 samples in 0.1 mol/L KHCO3 electrolyte；（b） Faradaic efficiencies of AD-Sn/N-C1000 and Sn-CF1000 samples at different potentials；（c） Long-term test of AD-Sn/N-C1000 at -0.6 V vs.RHE；（d） Tafel slopes of CO product current densities of AD-Sn/N-C1000 and Sn-CF1000 samples［53］

Fig.17 XPS and XAFS spectra of Cu-CeO2 sample：（a） XPS Ce3d spectra of Cu-CeO2-4% sample；（b） XPS Cu2p3/2 spectra of Cu-CeO2-4% sample；（c） XANES spectra of Cu-CeO2， Cu foil， CuO and Cu2O samples；（d） EXAFS spectra of Cu-CeO2， Cu foil， CuO and Cu2O samples［26］

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Research Prospect of Single Atom Catalysts Towards Electrocatalytic Reduction of Carbon Dioxide

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