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- Title
Efficient upgrading of CO to C<sub>3</sub> fuel using asymmetric C-C coupling active sites.
- Authors
Wang, Xue; Wang, Ziyun; Zhuang, Tao-Tao; Dinh, Cao-Thang; Li, Jun; Nam, Dae-Hyun; Li, Fengwang; Huang, Chun-Wei; Tan, Chih-Shan; Chen, Zitao; Chi, Miaofang; Gabardo, Christine M.; Seifitokaldani, Ali; Todorović, Petar; Proppe, Andrew; Pang, Yuanjie; Kirmani, Ahmad R.; Wang, Yuhang; Ip, Alexander H.; Richter, Lee J.
- 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. Catalysts for CO electroreduction have focused on Cu, and their main products have been C2 chemicals. Here authors use the concept of asymmetric active sites to develop a class of doped Cu catalysts for C-C coupling, delivering record selectivity to n-propanol.
- Subjects
NITROALDOL reactions; ELECTROLYTIC reduction; ENERGY conversion; ELECTROSYNTHESIS; CARBON-carbon bonds; ENERGY storage; ASYMMETRIC synthesis
- Publication
Nature Communications, 2019, Vol 10, Issue 1, pN.PAG
- ISSN
2041-1723
- Publication type
Article
- DOI
10.1038/s41467-019-13190-6