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Tailoring the Surface and Interface Structures of Copper-Based Catalysts for Electrochemical Reduction of CO2 to Ethylene and Ethanol

期刊

SMALL
卷 18, 期 18, 页码 -

出版社

WILEY-V C H VERLAG GMBH
DOI: 10.1002/smll.202107450

关键词

Cu-based catalysts; electrochemical reduction of CO; (2); ethanol; ethylene; surface and interface structures

资金

  1. National Natural Science Foundation of China (NSFC) [22075201and 21872101]
  2. JST-ERATO Materials Space-Tectonics Project [JPMJER2003]

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This paper systematically discusses the effects of surface and interface structures in Cu-based catalysts for the electrochemical CO2 reduction to valuable ethylene and ethanol. The key steps for ethylene production are C-C coupling, which can be enhanced by tuning the surface structures of the catalyst, and for ethanol production, it is the controllable hydrodeoxygenation of C-2 intermediates, which can be achieved by tuning the stability of oxygenate intermediates through the metallic cluster induced special atomic configuration and bimetallic synergy induced the double active sites on the catalyst surface. The structure-performance relationships provide guidance for the design of Cu-based catalysts for highly efficient reduction of CO2.
Electrochemical CO2 reduction to valuable ethylene and ethanol offers a promising strategy to lower CO2 emissions while storing renewable electricity. Cu-based catalysts have shown the potential for CO2-to-ethylene/ethanol conversion, but still suffer from low activity and selectivity. Herein, the effects of surface and interface structures in Cu-based catalysts for CO2-to-ethylene/ethanol production are systematically discussed. Both reactions involve three crucial steps: formation of CO intermediate, C-C coupling, and hydrodeoxygenation of C-2 intermediates. For ethylene, the key step is C-C coupling, which can be enhanced by tailoring the surface structures of catalyst such as step sites on facets, Cu-0/Cu delta+ species and nanopores, as well as the optimized molecule-catalyst and electrolyte-catalyst interfaces further promoting the higher ethylene production. While the controllable hydrodeoxygenation of C-2 intermediate is important for ethanol, which can be achieved by tuning the stability of oxygenate intermediates through the metallic cluster induced special atomic configuration and bimetallic synergy induced the double active sites on catalyst surface. Additionally, constraining CO coverage by the complex-catalyst interface and stabilizing C-O bond by N-doped carbon/Cu interface can also enhance the ethanol selectivity. The structure-performance relationships will provide the guidance for the design of Cu-based catalysts for highly efficient reduction of CO2.

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