Enhanced multi-carbon alcohol electroproduction from CO via modulated hydrogen adsorption

Jun Li, Aoni Xu, Fengwang Li, Ziyun Wang, Chengqin Zou, Christine M. Gabardo, Yuhang Wang, Adnan Ozden, Yi Xu, Dae-Hyun Nam, Yanwei Lum, Joshua Wicks, Bin Chen, Zhiqiang Wang, Jiatang Chen, Yunzhou Wen, Taotao Zhuang, Mingchuan Luo, Xiwen Du, Tsun-Kong Sham, Bo Zhang, Edward H. Sargent () and David Sinton ()
Additional contact information
Jun Li: University of Toronto
Aoni Xu: University of Toronto
Fengwang Li: University of Toronto
Ziyun Wang: University of Toronto
Chengqin Zou: University of Toronto
Christine M. Gabardo: University of Toronto
Yuhang Wang: University of Toronto
Adnan Ozden: University of Toronto
Yi Xu: University of Toronto
Dae-Hyun Nam: University of Toronto
Yanwei Lum: University of Toronto
Joshua Wicks: University of Toronto
Bin Chen: University of Toronto
Zhiqiang Wang: University of Western Ontario
Jiatang Chen: University of Western Ontario
Yunzhou Wen: Fudan University
Taotao Zhuang: University of Toronto
Mingchuan Luo: University of Toronto
Xiwen Du: Tianjin University
Tsun-Kong Sham: University of Western Ontario
Bo Zhang: Fudan University
Edward H. Sargent: University of Toronto
David Sinton: University of Toronto

Nature Communications, 2020, vol. 11, issue 1, 1-8

Abstract: Abstract Multi-carbon alcohols such as ethanol are valued as fuels in view of their high energy density and ready transport. Unfortunately, the selectivity toward alcohols in CO2/CO electroreduction is diminished by ethylene production, especially when operating at high current densities (>100 mA cm−2). Here we report a metal doping approach to tune the adsorption of hydrogen at the copper surface and thereby promote alcohol production. Using density functional theory calculations, we screen a suite of transition metal dopants and find that incorporating Pd in Cu moderates hydrogen adsorption and assists the hydrogenation of C2 intermediates, providing a means to favour alcohol production and suppress ethylene. We synthesize a Pd-doped Cu catalyst that achieves a Faradaic efficiency of 40% toward alcohols and a partial current density of 277 mA cm−2 from CO electroreduction. The activity exceeds that of prior reports by a factor of 2.

Date: 2020
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DOI: 10.1038/s41467-020-17499-5

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