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

Tsz Woon Benedict Lo, Yi Xie, Pengfei Qu, Wang Xue, Zhangyou Xu, Yuguang C. Li, Ziyun Wang, Jianan Erick Huang, Joshua Wicks, Christopher McCallum, Ning Wang, Yuhang Wang, Tianxiang Chen, David Sinton, Jimmy C. Yu, Ying Wang, Edward H. Sargent

Research output: Journal article publicationJournal articleAcademic researchpeer-review

214 Citations (Scopus)

Abstract

Renewable electricity-powered CO 2 reduction to multi-carbon (C 2+) products offers a promising route to realization of low-carbon-footprint fuels and chemicals. However, a major fraction of input CO 2 (>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 CO 2 on Cu-based catalysts to weaken H* binding. Using density functional theory studies, we found Pd–Cu promising for selective C 2+ production over C 1, with the lowest ∆G OCCOH* and ∆G OCCOH* - ∆G CHO*. We synthesized Pd–Cu catalysts and report a crossover-free system (liquid product crossover <0.05%) with a Faradaic efficiency of 89 ± 4% for CO 2 to C 2+ at 500 mA cm −2, simultaneous with single-pass CO 2 utilization of 60 ± 2% to C 2+. [Figure not available: see fulltext.]

Original languageEnglish
Pages (from-to)564-570
Number of pages7
JournalNature Catalysis
Volume5
Issue number6
DOIs
Publication statusPublished - 9 Jun 2022

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