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

Xue Wang, Ziyun Wang, Tao Tao Zhuang, Cao Thang Dinh, Jun Li, Dae Hyun Nam, Fengwang Li, Chun Wei Huang, Chih Shan Tan, Zitao Chen, Miaofang Chi, Christine M. Gabardo, Ali Seifitokaldani, Petar Todorović, Andrew Proppe, Yuanjie Pang, Ahmad R. Kirmani, Yuhang Wang, Alexander H. Ip, Lee J. RichterBenjamin Scheffel, Aoni Xu, Shen Chuan Lo, Shana O. Kelley, David Sinton, Edward H. Sargent*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

175 Scopus citations

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.

Original languageEnglish
Article number5186
JournalNature Communications
Volume10
Issue number1
DOIs
StatePublished - 1 Dec 2019

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