Cationic-group-functionalized electrocatalysts enable stable acidic CO2 electrolysis

Mengyang Fan, Jianan Erick Huang, Rui Kai Miao, Yu Mao, Pengfei Ou, Feng Li, Xiao Yan Li, Yufei Cao, Zishuai Zhang, Jinqiang Zhang, Yu Yan, Adnan Ozden, Weiyan Ni, Ying Wang, Yong Zhao, Zhu Chen, Behrooz Khatir, Colin P. O’Brien, Yi Xu, Yurou Celine XiaoGeoffrey I.N. Waterhouse, Kevin Golovin, Ziyun Wang*, Edward H. Sargent*, David Sinton*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

44 Scopus citations

Abstract

Acidic electrochemical CO2 reduction (CO2R) addresses CO2 loss and thus mitigates the energy penalties associated with CO2 recovery; however, acidic CO2R suffers low selectivity. One promising remedy—using a high concentration of alkali cations—steers CO2R towards multi-carbon (C2+) products, but these same alkali cations result in salt formation, limiting operating stability to <15 h. Here we present a copper catalyst functionalized with cationic groups (CG) that enables efficient CO2 activation in a stable manner. By replacing alkali cations with immobilized benzimidazolium CG within ionomer coatings, we achieve over 150 h of stable CO2R in acid. We find the water-management property of CG minimizes proton migration that enables operation at a modest voltage of 3.3 V with mildly alkaline local pH, leading to more energy-efficient CO2R with a C2+ Faradaic efficiency of 80 ± 3%. As a result, we report an energy efficiency of 28% for acidic CO2R towards C2+ products and a single-pass CO2 conversion efficiency exceeding 70%. [Figure not available: see fulltext.]

Original languageEnglish (US)
Pages (from-to)763-772
Number of pages10
JournalNature Catalysis
Volume6
Issue number9
DOIs
StatePublished - Sep 2023

ASJC Scopus subject areas

  • Catalysis
  • Bioengineering
  • Biochemistry
  • Process Chemistry and Technology

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