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化学进展 2022, Vol. 34 Issue (3): 533-546 DOI: 10.7536/PC210352 前一篇   后一篇

• 综述 •

过渡金属单原子电催化剂还原CO2制CO

沈树进, 韩成*(), 王兵, 王应德*()   

  1. 国防科技大学 空天科学学院 新型陶瓷纤维及其复合材料重点实验室 长沙 410073
  • 收稿日期:2021-04-01 修回日期:2021-07-10 出版日期:2021-07-29 发布日期:2021-07-29
  • 通讯作者: 韩成, 王应德
  • 基金资助:
    国家自然科学基金项目(51773226); 国家自然科学基金项目(61701514)
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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:2021-04-01 Revised:2021-07-10 Online:2021-07-29 Published:2021-07-29
  • Contact: Cheng Han, Yingde Wang
  • Supported by:
    National Natural Science Foundation of China(51773226); National Natural Science Foundation of China(61701514)

电催化二氧化碳还原(ECR)技术是实现“碳中和”目标的一种理想途径,而过渡金属单原子催化剂具有电子结构可调、原子利用率高和活性位点均一等特点,在ECR研究中具有显著优势。本文首先介绍了单原子电催化剂在还原CO2尤其是在选择性生成CO研究中的优势,然后综述了近年来Fe、Co、Ni及其他单原子电催化剂的反应位点调控策略与电催化选择性的调控机制,重点对质子耦合CO2还原生成CO的中间过程调控进行了归纳总结,并简要展望了发展方向,以期为推动单原子催化剂在ECR中规模化应用提供指导和参考。

关键词： 单原子催化剂, 二氧化碳还原, 电催化

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
()
图1 (a)颗粒尺寸与表面自由能和比活性的对应关系[44],(b)几何结构、电子结构与颗粒尺寸的对应关系[45]
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
图2 电催化还原CO2制CO反应路径示意图[46]
Fig.2 Schematic of the reaction steps of electrocatalytic CO2 to CO reduction[46]. Copyright 2017, Elsevier
表1 近期报道的单原子催化剂电催化还原CO2制CO的性能对比
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
图3 Ni-C/Ni-N-C催化剂[46]的(a)配位结构的示意图,(b)还原CO2制CO自由能图;(c)Ni-N4-C催化剂[60]的FECO;H-CPs[61]的(d)制备示意图,(e)与其他催化剂jCO对比图
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
图4 MePc催化剂[63]:(a)吸附*CO和*COOH的分波投影态密度;(b)还原CO2制CO自由能图。Co-N5/HNPCS[64]的(c)制备示意图;(d)LSV曲线。Co-Nx催化剂[68]的:(e)EXAFS 谱图;(f)还原CO2制CO自由能图;(g)不同电位下Co-N2、Co-N3和Co NPs的jtotal
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
图5 Fe-N-C催化剂[69]的(a)jCO和(b,c)Operando XAS表征;Fe1NC/SX-1000[71]中(d)载体尺寸变化示意图和(e)jCO, FECO与ESA的对应关系图;Fe-N/CNT@GNR中[56](f)Fe-N4位置示意图及(g)CNT到CNT@GNR的结构演变过程
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
图6 ZnN4/C催化剂[72]的(a)HAADF-STEM图和EXAFS谱图及(b)还原CO2制CO的自由能图;Bi SAs/NC[79]的(c)EDS mapping图和(d)还原CO2制CO的自由能图;Cu-Nx/GN[80]的(e)EXAFS谱图、(f)FECO和(g)还原CO2制CO的自由能图
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
图7 A-Ni-NG[92]中(a)Operando XANES谱图,(b)暴露在CO2气氛前(黑线),后(红线)的价带谱,以及CO2解吸后(蓝线)的价带谱,(c)CO2还原活性位点的结构演变,其中, E F 1和 E F 2是Ni-C O 2 δ -形成前后A-Ni-NG的费米能级,1πg和2πu是CO2分子轨道;(d)Ar、CO2气氛中Ni-TAPc的operando Raman光谱[93]
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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