华东师范大学学报（自然科学版） >

2023 , Vol. 2023 >Issue 1: 149 - 159

DOI: https://doi.org/10.3969/j.issn.1000-5641.2023.01.015

CO2资源化利用

铜基催化剂在电还原二氧化碳领域的应用研究

  • 汤静 ,
  • 张子宁 ,
  • 郑翔
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  • 华东师范大学 化学与分子工程学院 上海市绿色化学与化工过程绿色化重点实验室, 上海　200062
汤　静, 女, 研究员, 博士生导师, 研究方向为纳米多孔材料和电催化. E-mail: jingtang@chem.ecnu.edu.cn

收稿日期: 2022-06-30

  录用日期: 2022-09-02

  网络出版日期: 2023-01-07

基金资助

国家自然科学基金 (22005099)

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Application of Cu-based catalysts in the electroreduction of carbon dioxide

  • Jing TANG ,
  • Zining ZHANG ,
  • Xiang ZHENG
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  • Shanghai Key Laboratory of Green Chemistry and Chemical Processes, School of Chemistry and Molecular Engineering, East China Normal University, Shanghai　200062, China

Received date: 2022-06-30

  Accepted date: 2022-09-02

  Online published: 2023-01-07

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摘要

为了实现碳达峰碳中和的国家战略, 利用可再生能源发电将二氧化碳电催化转化为化学品再利用, 这引起了科学界的广泛关注. 铜基催化剂可将二氧化碳电还原为高附加值的多碳产物, 但仍需研究其催化机理来提高催化产物的选择性和催化效率. 根据铜的状态可将铜基催化剂分为单原子铜基催化剂、定向晶面铜基催化剂、氧化态铜基催化剂和铜合金/复合催化剂. 本文简要介绍了以上4类铜基催化剂的常见制备方法、结构特点、电催化还原二氧化碳的效果和可能的催化机理.

关键词： 铜基催化剂; 电催化; 二氧化碳还原

本文引用格式

汤静 , 张子宁 , 郑翔 . 铜基催化剂在电还原二氧化碳领域的应用研究[J]. 华东师范大学学报（自然科学版）, 2023 , 2023(1) : 149 -159 . DOI: 10.3969/j.issn.1000-5641.2023.01.015

Abstract

To achieve the national strategy of carbon neutralization, the electroreduction of carbon dioxide into usable reagents via renewable energy has caused widespread concern in the scientific community. Cu-based electrocatalysts can reduce carbon dioxide to high value-added multi carbon products, but the catalytic mechanism still needs to be studied to improve its selectivity and efficiency. Depending on the state of the Cu, Cu-based catalysts can be divided into Cu alloy/composite catalysts, single-atom, oriented crystalline, and oxidized Cu-based catalysts. This paper introduced the common preparation methods, structural characteristics, effect of electro catalytic reduction of carbon dioxide, and possible catalytic mechanism of the four types of Cu-based catalysts mentioned above.

Key words： Cu-based catalysts; electrocatalysis; carbon dioxide reduction

参考文献

1 FALKOWSKI P, SCHOLES R J, BOYLE E, et al. The global carbon cycle: A test of our knowledge of earth as a system. Science, 2000, 290 (5490): 291- 296.
2 OBAMA B. The irreversible momentum of clean energy. Science, 2017, 355 (6321): 126- 129.
3 GAO D F, ARAN-AIS R M, JEON H S, et al. Rational catalyst and electrolyte design for CO2 electroreduction towards multicarbon products . Nature Catalysis, 2019, 2 (3): 198- 210.
4 HANDOKO A D, WEI F X, JENNDY, et al. Understanding heterogeneous electrocatalytic carbon dioxide reduction through operando techniques. Nature Catalysis, 2018, 1 (12): 922- 934.
5 WAKERLEY D, LAMAISON S, OZANAM F, et al. Bio-inspired hydrophobicity promotes CO2 reduction on a Cu surface . Nature Materials, 2019, 18 (11): 1222- 1227.
6 ZHENG W Z, YANG J, CHEN H Q, et al. Atomically defined undercoordinated active sites for highly efficient CO2 electroreduction . Advanced Functional Materials, 2019, 30 (4): 1- 10.
7 XU C C, ZHI X, VASILEFF A, et al. Highly selective two-electron electrocatalytic CO2 reduction on single-atom Cu catalysts[J]. Small Structures, 2020, 2(1): 1-7.
8 YANG F Q, MAO X Y, MA M F, et al. Scalable strategy to fabricate single Cu atoms coordinated carbons for efficient electroreduction of CO2 to CO . Carbon, 2020, 168, 528- 535.
9 CHEN S H, WANG B Q, ZHU J X, et al. Lewis acid site-promoted single-atomic Cu catalyzes electrochemical CO2 methanation . Nano Letters, 2021, 21 (17): 7325- 7331.
10 JIAO J Q, LIN R, LIU S J, et al. Copper atom-pair catalyst anchored on alloy nanowires for selective and efficient electrochemical reduction of CO2. Nature Chemistry, 2019, 11 (3): 222- 228.
11 XU H P, REBOLLAR D, HE H Y, et al. Highly selective electrocatalytic CO2 reduction to ethanol by metallic clusters dynamically formed from atomically dispersed copper . Nature Energy, 2020, 5 (8): 623- 632.
12 FU S J, LIU X, RAN J R, et al. CO2 reduction by single copper atom supported on g-C3N4 with asymmetrical active sites . Applied Surface Science, 2021, 540, 1- 7.
13 LI S, GUAN A X, YANG C, et al. Dual-atomic Cu sites for electrocatalytic CO reduction to C2+ products . ACS Materials Letters, 2021, 3 (12): 1729- 1737.
14 TAKAHASHI I, KOGA O, HOSHI N, et al. Electrochemical reduction of CO2 at copper single crystal Cu(S)-[n(111)×(111)] and Cu(S)-[n(110)×(100)] electrodes . Journal of Electroanalytical Chemistry, 2002, 533 (1/2): 135- 143.
15 SCHOUTEN K J P, QIN Z S, GALLENT E P, et al. Two pathways for the formation of ethylene in CO2 reduction on single-crystal copper electrodes . Journal of the American Chemical Society, 2012, 134 (24): 9864- 9867.
16 HAHN C, HATSUKADE T, KIM Y G, et al. Engineering Cu surfaces for the electrocatalytic conversion of CO2: Controlling selectivity toward oxygenates and hydrocarbons . Proceedings of the National Academy of Sciences of the United States of America, 2017, 114 (23): 5918- 5923.
17 GREGORIO G L, BURDYNY T, LOIUDICE A, et al. Facet-dependent selectivity of Cu catalysts in electrochemical CO2 reduction at commercially viable current densities . ACS Catalysis, 2020, 10 (9): 4854- 4862.
18 RESKE R, MIRTRY H, BEHAFARID F, et al. Particle size effects in the catalytic electroreduction of CO2 on Cu nanoparticles . Journal of the American Chemical Society, 2014, 136 (19): 6978- 86.
19 GAO Y G, WU Q, LIANG, X Z, et al. Cu2O nanoparticles with both (100) and (111) facets for enhancing the selectivity and activity of CO2 electroreduction to ethylene . Advanced Science, 2020, 7 (6): 1- 7.
20 ZHONG D Z, ZHAO Z J, ZHAO Q, et al. Coupling of Cu (100) and (110) facets promotes carbon dioxide conversion to hydrocarbons and alcohols. Angewandte Chemie-International Edition, 2021, 60 (9): 4879- 4885.
21 LI H, YU P P, LEI R B, et al. Facet-selective deposition of ultrathin Al2O3 on copper nanocrystals for highly stable CO2 electroreduction to ethylene . Angewandte Chemie-International Edition, 2021, 60 (47): 24838- 24843.
22 YANG P P, ZHANG X L, GAO F Y, et al. Protecting copper oxidation state via intermediate confinement for selective CO2 electroreduction to C2+ fuels . Journal of the American Chemical Society, 2020, 142 (13): 6400- 6408.
23 JUNG H, LEE S Y, LEE C W, et al. Electrochemical fragmentation of Cu2O nanoparticles enhancing selective C-C coupling from CO2 reduction reaction . Journal of the American Chemical Society, 2019, 141 (11): 4624- 4633.
24 GAO Y G, YU S Q, ZHOU P, et al. Promoting electrocatalytic reduction of CO2 to C2H4 production by inhibiting C2H5OH desorption from Cu2O/C composite . Small, 2022, 18 (9): 2105212- 2105222.
25 LIU W, ZHAI P B, LI A W, et al. Electrochemical CO2 reduction to ethylene by ultrathin CuO nanoplate arrays . Nature Communications, 2022, 13 (1): 1877- 1889.
26 ZHANG J F, WANG Y, LI Z Y, et al. Grain boundary-derived Cu(+)/Cu(0) interfaces in CuO nanosheets for low overpotential carbon dioxide electroreduction to ethylene. Advanced Science, 2022, 2200454- 2200465.
27 ZHOU Y J, QI H H, WU J, et al. Amino modified carbon dots with electron sink effect increase interface charge transfer rate of Cu‐based electrocatalyst to enhance the CO2 conversion selectivity to C2H4. Advanced Functional Materials, 2022, 32 (22): 2113335- 2113347.
28 ZHANG W, HUANG C Q, XIAO Q, et al. Atypical oxygen-bearing copper boosts ethylene selectivity toward electrocatalytic CO2 reduction . Journal of the American Chemical Society, 2020, 142 (26): 11417- 11427.
29 QIU X F, ZHU H L, HUANG J R, et al. Highly selective CO2 electroreduction to C2H4 using a metal-organic framework with dual active sites . Journal of the American Chemical Society, 2021, 143 (19): 7242- 7246.
30 LYU Z H, ZHU S Q, XIE M H, et al. Controlling the surface oxidation of Cu nanowires improves their catalytic selectivity and stability toward C2+ products in CO2 reduction . Angewandte Chemie-International Edition, 2021, 60 (4): 1909- 1915.
31 YU J L, WANG J, MA Y B, et al. Recent progresses in electrochemical carbon dioxide reduction on copper-based catalysts toward multicarbon products. Advanced Functional Materials, 2021, 31 (37): 2102151- 2102179.
32 XIONG L K, ZHANG X, YUAN H, et al. Breaking the linear scaling relationship by compositional and structural crafting of ternary Cu-Au/Ag nanoframes for electrocatalytic ethylene production. Angewandte Chemie-International Edition, 2021, 60 (5): 2508- 2518.
33 YAN Y B, ZHAO Z P, ZHAO J, et al. Atomic-thin hexagonal CuCo nanocrystals with d-band tuning for CO2 reduction . Journal of Materials Chemistry A, 2021, 9 (12): 7496- 7502.
34 ZHONG Y Z, KONG X D, SONG Z M, et al. Adjusting local CO confinement in porous-shell Ag@Cu catalysts for enhancing C-C coupling toward CO2 eletroreduction . Nano Letters, 2022, 22 (6): 2554- 2560.
35 JIA S Q, ZHU Q G, WU H H, et al. Efficient electrocatalytic reduction of carbon dioxide to ethylene on copper-antimony bimetallic alloy catalyst. Chinese Journal of Catalysis, 2020, 41 (7): 1091- 1098.
36 SONG H, TAN Y C, KIM B, et al. Tunable product selectivity in electrochemical CO2 reduction on well-mixed Ni-Cu alloys . ACS Applied Materials & Interfaces, 2021, 13 (46): 55272- 55280.
37 ZHANG Y F, ZHAO Y, WANG C Y, et al. Zn-Doped Cu(100) facet with efficient catalytic ability for the CO2 electroreduction to ethylene . Physical Chemistry Chemical Physics, 2019, 21 (38): 21341- 21348.
38 YIN Z Y, YU C, ZHAO Z L, et al. Cu3N nanocubes for selective electrochemical reduction of CO2 to ethylene . Nano Letters, 2019, 19 (12): 8658- 8663.
39 SONG Y F, JUNQUEIRA J R C, SIKDAR N, et al. B-Cu-Zn gas diffusion electrodes for CO2 electroreduction to C2+ products at high current densities . Angewandte Chemie-International Edition, 2021, 60 (16): 9135- 9141.
40 MA W C, XIE S J, LIU T T, et al. Electrocatalytic reduction of CO2 to ethylene and ethanol through hydrogen-assisted C-C coupling over fluorine-modified copper . Nature Catalysis, 2020, 3 (6): 478- 487.
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