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

Mingchuan Luo, Ziyun Wang, Yuguang C. Li, Jun Li, Fengwang Li, Yanwei Lum, Dae-Hyun Nam, Bin Chen, Joshua Wicks, Aoni Xu, Taotao Zhuang, Wan Ru Leow, Xue Wang, Cao-Thang Dinh, Ying Wang, Yuhang Wang, David Sinton and Edward H. Sargent ()
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Mingchuan Luo: University of Toronto
Ziyun Wang: University of Toronto
Yuguang C. Li: University of Toronto
Jun Li: University of Toronto
Fengwang Li: University of Toronto
Yanwei Lum: University of Toronto
Dae-Hyun Nam: University of Toronto
Bin Chen: University of Toronto
Joshua Wicks: University of Toronto
Aoni Xu: University of Toronto
Taotao Zhuang: University of Toronto
Wan Ru Leow: University of Toronto
Xue Wang: University of Toronto
Cao-Thang Dinh: University of Toronto
Ying Wang: University of Toronto
Yuhang Wang: University of Toronto
David Sinton: University of Toronto
Edward H. Sargent: University of Toronto

Nature Communications, 2019, vol. 10, issue 1, 1-7

Abstract: Abstract 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, a key intermediate whose fate determines branching to ethanol versus ethylene.

Date: 2019
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DOI: 10.1038/s41467-019-13833-8

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