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Selective CO2 Electrochemical Reduction Enabled by a Tricomponent Copolymer Modifier on a Copper Surface

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  • Jianchun Wang, California Institute of Technology
  • ,
  • Tao Cheng, California Institute of Technology
  • ,
  • Aidan Q. Fenwick, California Institute of Technology
  • ,
  • Turki N. Baroud, King Fahd University of Petroleum and Minerals
  • ,
  • Alonso Rosas-Hernández
  • Jeong Hoon Ko, California Institute of Technology
  • ,
  • Quan Gan, California Institute of Technology
  • ,
  • William A. Goddard III, California Institute of Technology
  • ,
  • Robert H. Grubbs, California Institute of Technology

Electrochemical CO2 reduction over Cu could provide value-added multicarbon hydrocarbons and alcohols. Despite recent breakthroughs, it remains a significant challenge to design a catalytic system with high product selectivity. Here we demonstrate that a high selectivity of ethylene (55%) and C2+ products (77%) could be achieved by a highly modular tricomponent copolymer modified Cu electrode, rivaling the best performance using other modified polycrystalline Cu foil catalysts. Such a copolymer can be conveniently prepared by a ring-opening metathesis polymerization, thereby offering a new degree of freedom for tuning the selectivity. Control experiments indicate all three components are essential for the selectivity enhancement. A surface characterization showed that the incorporation of a phenylpyridinium component increased the film robustness against delamination. It was also shown that its superior performance is not due to a morphology change of the Cu underneath. Molecular dynamics (MD) simulations indicate that a combination of increased local CO2 concentration, increased porosity for gas diffusion, and the local electric field effect together contribute to the increased ethylene and C2+ product selectivity.

TidsskriftJournal of the American Chemical Society
Sider (fra-til)2857-2865
Antal sider9
StatusUdgivet - feb. 2021
Eksternt udgivetJa

Bibliografisk note

Funding Information:
This study was supported by the King Fahd University of Petroleum and Minerals (R.H.G.) and the Joint Center for Artificial Photosynthesis, a Department of Energy (DOE) Energy Innovation Hub, supported through the Office of Science of the U.S. Department of Energy under Award Number DE-SC0004993.

Publisher Copyright:
© 2021 American Chemical Society

Copyright 2021 Elsevier B.V., All rights reserved.

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