Hydroxide promotes carbon dioxide electroreduction to ethanol on copper via tuning of adsorbed hydrogen

被引：298

作者：

Luo, Mingchuan ^{[1
]}

Wang, Ziyun ^{[1
]}

Li, Yuguang C. ^{[1
]}

Li, Jun ^{[1
]}

Li, Fengwang ^{[1
]}

Lum, Yanwei ^{[1
]}

Nam, Dae-Hyun ^{[1
]}

Chen, Bin ^{[1
]}

Wicks, Joshua ^{[1
]}

Xu, Aoni ^{[1
]}

Zhuang, Taotao ^{[1
]}

Leow, Wan Ru ^{[1
]}

Wang, Xue ^{[1
]}

Dinh, Cao-Thang ^{[1
]}

Wang, Ying ^{[1
]}

Wang, Yuhang ^{[1
]}

Sinton, David ^{[2
]}

Sargent, Edward H. ^{[1
]}

机构：

[1] Univ Toronto, Dept Elect & Comp Engn, Toronto, ON M5S 1A4, Canada

[2] Univ Toronto, Dept Mech & Ind Engn, Toronto, ON M5S 3G8, Canada

来源：

NATURE COMMUNICATIONS | 2019年 / 10卷 / 1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：

INITIO MOLECULAR-DYNAMICS; TOTAL-ENERGY CALCULATIONS; CO2; REDUCTION; ELECTROCHEMICAL REDUCTION; SELECTIVITY; EFFICIENCY; EVOLUTION;

D O I：

10.1038/s41467-019-13833-8

中图分类号：

O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];

学科分类号：

07 ; 0710 ; 09 ;

摘要：

Producing liquid fuels such as ethanol from CO2, H2O, and renewable electricity offers a route to store sustainable energy. The search for efficient electrocatalysts for the CO2 reduction reaction relies on tuning the adsorption strength of carbonaceous intermediates. Here, we report a complementary approach in which we utilize hydroxide and oxide doping of a catalyst surface to tune the adsorbed hydrogen on Cu. Density functional theory studies indicate that this doping accelerates water dissociation and changes the hydrogen adsorption energy on Cu. We synthesize and investigate a suite of metal-hydroxide-interface-doped-Cu catalysts, and find that the most efficient, Ce(OH)(x)-doped-Cu, exhibits an ethanol Faradaic efficiency of 43% and a partial current density of 128 mA cm(-2). Mechanistic studies, wherein we combine investigation of hydrogen evolution performance with the results of operando Raman spectroscopy, show that adsorbed hydrogen hydrogenates surface (HCCOH)-H-star, a key intermediate whose fate determines branching to ethanol versus ethylene.

引用

页数：7

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