Cationic-group-functionalized electrocatalysts enable stable acidic CO2 electrolysis

被引：155

作者：

Fan, Mengyang ^{[1
]}

Huang, Jianan Erick ^{[2
]}

Miao, Rui Kai ^{[1
]}

Mao, Yu ^{[3
]}

Ou, Pengfei ^{[2
,4
]}

Li, Feng ^{[1
]}

Li, Xiao-Yan ^{[2
]}

Cao, Yufei ^{[2
]}

Zhang, Zishuai ^{[5
]}

Zhang, Jinqiang ^{[1
,2
]}

Yan, Yu ^{[2
]}

Ozden, Adnan ^{[1
]}

Ni, Weiyan ^{[2
]}

Wang, Ying ^{[6
]}

Zhao, Yong ^{[1
]}

Chen, Zhu ^{[2
]}

Khatir, Behrooz ^{[1
]}

O'Brien, Colin P. ^{[1
]}

Xu, Yi ^{[1
]}

Xiao, Yurou Celine ^{[1
]}

Waterhouse, Geoffrey I. N. ^{[3
]}

Golovin, Kevin ^{[1
]}

Wang, Ziyun ^{[3
]}

Sargent, Edward H. ^{[2
,4
]}

Sinton, David ^{[1
]}

机构：

[1] Univ Toronto, Dept Mech & Ind Engn, Toronto, ON, Canada

[2] Univ Toronto, Dept Elect & Comp Engn, Toronto, ON, Canada

[3] Univ Auckland, Sch Chem Sci, Auckland, New Zealand

[4] Northwestern Univ, Dept Chem, Evanston, IL 60208 USA

[5] Univ British Columbia, Dept Chem, Vancouver, BC, Canada

[6] Chinese Univ Hong Kong S A R, Dept Chem, Hong Kong, Peoples R China

来源：

NATURE CATALYSIS | 2023年 / 6卷 / 09期

基金：

加拿大自然科学与工程研究理事会; 加拿大创新基金会;

关键词：

ELECTROCHEMICAL REDUCTION; ELECTROREDUCTION; MEMBRANES; SPECTROSCOPY; INTERFACES; CONVERSION; CATALYSIS; PRODUCTS; ALKALI; FUELS;

D O I：

10.1038/s41929-023-01003-5

中图分类号：

O64 [物理化学（理论化学）、化学物理学];

学科分类号：

070304 ; 081704 ;

摘要：

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%.

引用

页码：763 / 772

页数：10

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