Selective CO2 electrochemical reduction enabled by a tricomponent copolymer modifier on a copper surface

Jianchun Wang, Tao Cheng, Aidan Q. Fenwick, Turki N. Baroud, Alonso Rosas-Hernández, Jeong Hoon Ko, Quan Gan, William A. Goddard*, Robert H. Grubbs*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

97 Scopus citations

Abstract

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.

Original languageEnglish
Pages (from-to)2857-2865
Number of pages9
JournalJournal of the American Chemical Society
Volume143
Issue number7
DOIs
StatePublished - 24 Feb 2021

Bibliographical note

Publisher Copyright:
© 2021 American Chemical Society

ASJC Scopus subject areas

  • Catalysis
  • General Chemistry
  • Biochemistry
  • Colloid and Surface Chemistry

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