High carbon utilization in CO2 reduction to multi-carbon products in acidic media

Yi Xie, Pengfei Ou, Xue Wang, Zhanyou Xu, Yuguang C. Li, Ziyun Wang, Jianan Erick Huang, Joshua Wicks, Christopher McCallum, Ning Wang, Yuhang Wang, Tianxiang Chen, Benedict T.W. Lo, David Sinton, Jimmy C. Yu, Ying Wang*, Edward H. Sargent

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

12 Scopus citations

Abstract

Renewable electricity-powered CO2 reduction to multi-carbon (C2+) products offers a promising route to realization of low-carbon-footprint fuels and chemicals. However, a major fraction of input CO2 (>85%) is consumed by the electrolyte through reactions with hydroxide to form carbonate/bicarbonate in both alkaline and neutral reactors. Acidic conditions offer a solution to overcoming this limitation, but also promote the hydrogen evolution reaction. Here we report a design strategy that suppresses hydrogen evolution reaction activity by maximizing the co-adsorption of CO and CO2 on Cu-based catalysts to weaken H* binding. Using density functional theory studies, we found Pd–Cu promising for selective C2+ production over C1, with the lowest ∆GOCCOH* and ∆GOCCOH* - ∆GCHO*. We synthesized Pd–Cu catalysts and report a crossover-free system (liquid product crossover <0.05%) with a Faradaic efficiency of 89 ± 4% for CO2 to C2+ at 500 mA cm−2, simultaneous with single-pass CO2 utilization of 60 ± 2% to C2+. [Figure not available: see fulltext.]

Original languageEnglish (US)
Pages (from-to)564-570
Number of pages7
JournalNature Catalysis
Volume5
Issue number6
DOIs
StatePublished - Jun 2022

ASJC Scopus subject areas

  • Catalysis
  • Bioengineering
  • Biochemistry
  • Process Chemistry and Technology

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