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Efficient upgrading of CO to C3 fuel using asymmetric C-C coupling active sites

Published

Author(s)

Lee J. Richter, Ahmad R. Kirmani, Xue Wang, Wang Ziyuan, Dinh Cao-Thang, Li Jun, Nam Dae-Hyun, Li Fengwang, Huang Chun-Wei, Tan Chih-Shan, Chen Zitao, Chi Miaofang, Gabardo M. Christine, Seiifitokaldani Ali, Todorovic Petar, Proppe Andrew, Pang Yuanjie, wang yuhang, Ip H. Alexander, Shen-Chuan Lo, shana O. kelley, David Sinton, Edward H. Sargent, Tao-Tao Zhuang, Benjamin Scheffel

Abstract

The electroreduction of C1 feedgas to high-energy-density fuels provides an attractive avenue to the storage of renewable electricity. Much progress has been made to improve selectivity to C1 and C2 products, however, the selectivity to desirable high-energy-density C3 products remains relatively low. We reason that C3 electrosynthesis relies on a higher-order reaction pathway that requires the formation of multiple carbon-carbon (C-C) bonds, and thus pursue a strategy explicitly designed to couple C2 with C1 intermediates. We develop an approach wherein neighboring copper atoms having distinct electronic structures interact with two adsorbates to catalyze an asymmetric reaction. We achieve a record n-propanol Faradaic efficiency (FE) of (33 ± 1)% with a conversion rate of (4.5 ± 0.1) mA cm−2, and a record n-propanol cathodic energy conversion efficiency (EEcathodic half-cell) of 21%. The FE and EEcathodic half-cell represent a 1.3× improvement relative to previously-published CO-to-n-propanol electroreduction reports.
Citation
Nature Communications
Volume
10

Keywords

electrochemstry, catalysis, carbon monoxide, electroredcution, quantum chemistry
Created November 29, 2019, Updated April 14, 2020