Dopant-tuned stabilization of intermediates promotes electrosynthesis of valuable C3 products

Tao-Tao Zhuang, Dae-Hyun Nam, Ziyun Wang, Hui-Hui Li, Christine M. Gabardo, Yi Li, Zhi-Qin Liang, Jun Li, Xiao-Jing Liu, Bin Chen, Wan Ru Leow, Rui Wu, Xue Wang, Fengwang Li, Yanwei Lum, Joshua Wicks, Colin P. O’Brien, Tao Peng, Alexander H. Ip, Tsun-Kong Sham, Shu-Hong Yu, David Sinton and Edward H. Sargent ()
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Tao-Tao Zhuang: University of Toronto
Dae-Hyun Nam: University of Toronto
Ziyun Wang: University of Toronto
Hui-Hui Li: University of Toronto
Christine M. Gabardo: University of Toronto
Yi Li: University of Science and Technology of China
Zhi-Qin Liang: University of Toronto
Jun Li: University of Toronto
Xiao-Jing Liu: University of Science and Technology of China
Bin Chen: University of Toronto
Wan Ru Leow: University of Toronto
Rui Wu: University of Science and Technology of China
Xue Wang: University of Toronto
Fengwang Li: University of Toronto
Yanwei Lum: University of Toronto
Joshua Wicks: University of Toronto
Colin P. O’Brien: University of Toronto
Tao Peng: University of Toronto
Alexander H. Ip: University of Toronto
Tsun-Kong Sham: University of Western Ontario
Shu-Hong Yu: University of Science and Technology of China
David Sinton: University of Toronto
Edward H. Sargent: University of Toronto

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

Abstract: Abstract The upgrading of CO2/CO feedstocks to higher-value chemicals via energy-efficient electrochemical processes enables carbon utilization and renewable energy storage. Substantial progress has been made to improve performance at the cathodic side; whereas less progress has been made on improving anodic electro-oxidation reactions to generate value. Here we report the efficient electroproduction of value-added multi-carbon dimethyl carbonate (DMC) from CO and methanol via oxidative carbonylation. We find that, compared to pure palladium controls, boron-doped palladium (Pd-B) tunes the binding strength of intermediates along this reaction pathway and favors DMC formation. We implement this doping strategy and report the selective electrosynthesis of DMC experimentally. We achieve a DMC Faradaic efficiency of 83 ± 5%, fully a 3x increase in performance compared to the corresponding pure Pd electrocatalyst.

Date: 2019
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DOI: 10.1038/s41467-019-12788-0

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