Constraining CO coverage on copper promotes high-efficiency ethylene electroproduction

Jun Li, Ziyun Wang, Christopher McCallum, Yi Xu, Fengwang Li, Yuhang Wang, Christine M. Gabardo, Cao Thang Dinh, Tao Tao Zhuang, Liang Wang, Jane Y. Howe, Yang Ren, Edward H. Sargent, David Sinton*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

115 Scopus citations

Abstract

The availability of inexpensive industrial CO gas streams motivates efficient electrocatalytic upgrading of CO to higher-value feedstocks such as ethylene. However, the electrosynthesis of ethylene by the CO reduction reaction (CORR) has suffered from low selectivity and energy efficiency. Here we find that the recent strategy of increasing performance through use of highly alkaline electrolyte—which is very effective in CO2RR—fails in CORR and drives the reaction to acetate. We then observe that ethylene selectivity increases when we constrain (decrease) CO availability. Using density functional theory, we show how CO coverage on copper influences the reaction pathways of ethylene versus oxygenate: lower CO coverage stabilizes the ethylene-relevant intermediates whereas higher CO coverage favours oxygenate formation. We then control local CO availability experimentally by tuning the CO concentration and reaction rate; we achieve ethylene Faradaic efficiencies of 72% and a partial current density of >800 mA cm−2. The overall system provides a half-cell energy efficiency of 44% for ethylene production.

Original languageEnglish (US)
Pages (from-to)1124-1131
Number of pages8
JournalNature Catalysis
Volume2
Issue number12
DOIs
StatePublished - Dec 1 2019

ASJC Scopus subject areas

  • Catalysis
  • Bioengineering
  • Biochemistry
  • Process Chemistry and Technology

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