Binding Site Diversity Promotes CO2 Electroreduction to Ethanol

Yuguang C. Li, Ziyun Wang, Tiange Yuan, Dae Hyun Nam, Mingchuan Luo, Joshua Wicks, Bin Chen, Jun Li, Fengwang Li, F. Pelayo García De Arquer, Ying Wang, Cao Thang Dinh, Oleksandr Voznyy, David Sinton, Edward H. Sargent*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

390 Scopus citations

Abstract

The electrochemical reduction of CO2 has seen many record-setting advances in C2 productivity in recent years. However, the selectivity for ethanol, a globally significant commodity chemical, is still low compared to the selectivity for products such as ethylene. Here we introduce diverse binding sites to a Cu catalyst, an approach that destabilizes the ethylene reaction intermediates and thereby promotes ethanol production. We develop a bimetallic Ag/Cu catalyst that implements the proposed design toward an improved ethanol catalyst. It achieves a record Faradaic efficiency of 41% toward ethanol at 250 mA/cm2 and -0.67 V vs RHE, leading to a cathodic-side (half-cell) energy efficiency of 24.7%. The new catalysts exhibit an in situ Raman spectrum, in the region associated with CO stretching, that is much broader than that of pure Cu controls, a finding we account for via the diversity of binding configurations. This physical picture, involving multisite binding, accounts for the enhanced ethanol production for bimetallic catalysts, and presents a framework to design multimetallic catalysts to control reaction paths in CO2 reductions toward desired products.

Original languageEnglish (US)
Pages (from-to)8584-8591
Number of pages8
JournalJournal of the American Chemical Society
Volume141
Issue number21
DOIs
StatePublished - May 29 2019

ASJC Scopus subject areas

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

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