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

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 EE_{cathodic half-cell} represent a 1.3× improvement relative to previously-published CO-to-n-propanol electroreduction reports.

Authors:

Wang, Xue  ^[1];

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• Search DOE PAGES for ORCID "0000-0002-6298-1858"

Wang, Ziyun  ^[1];

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• Search DOE PAGES for ORCID "0000-0002-2817-8367"

Zhuang, Tao-Tao ^[1]; Dinh, Cao-Thang  ^[1];

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• Search DOE PAGES for ORCID "0000-0001-9641-9815"

Li, Jun  ^[1];

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Nam, Dae-Hyun  ^[1];

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• Search DOE PAGES for ORCID "0000-0002-0871-1355"

Li, Fengwang  ^[1];

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• Search DOE PAGES for ORCID "0000-0003-1531-2966"

Huang, Chun-Wei ^[2]; Tan, Chih-Shan ^[1]; Chen, Zitao  ^[3];

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Chi, Miaofang  ^[3];

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Gabardo, Christine M.  ^[1];

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Seifitokaldani, Ali  ^[1];

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Todorović, Petar ^[1]; Proppe, Andrew  ^[1];

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Pang, Yuanjie ^[1]; Kirmani, Ahmad R. ^[4]; Wang, Yuhang  ^[1];

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Ip, Alexander H. ^[1]; Richter, Lee J. ^[4] more »; Scheffel, Benjamin ^[1]; Xu, Aoni ^[1]; Lo, Shen-Chuan ^[2]; Kelley, Shana O.  ^[1];

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• Search DOE PAGES for ORCID "0000-0003-3360-5359"

Sinton, David  ^[1];

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• Search DOE PAGES for ORCID "0000-0003-2714-6408"

Sargent, Edward H.  ^[1]

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• Search DOE PAGES for ORCID "0000-0003-0396-6495"

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+ Show Author Affiliations

1. Univ. of Toronto, ON (Canada)
2. Industrial Technology Research Inst., Hsinchu (Taiwan)
3. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)
4. National Inst. of Standards and Technology (NIST), Gaithersburg, MD (United States)

Publication Date:

Fri Nov 29 00:00:00 EST 2019

Research Org.:

Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS)

Sponsoring Org.:

Ontario Research Fund Research; Natural Sciences and Engineering Research Council of Canada (NSERC); CIFAR Bio-Inspired Solar Energy; University of Toronto Connaught; USDOE Office of Science (SC); Federal Economic Development Agency of Southern Ontario; Province of Ontario; IBM Canada Ltd.; Ontario Centres of Excellence; Mitacs; Canada Foundation for Innovation (CFI); Ontario Research Fund; Banting Postdoctoral Fellowships Program

OSTI Identifier:

1624214

Grant/Contract Number:  

AC02-06CH11357

Resource Type:

Accepted Manuscript

Journal Name:

Nature Communications

Additional Journal Information:

Journal Volume: 10; Journal Issue: 1; Journal ID: ISSN 2041-1723

Publisher:

Nature Publishing Group

Country of Publication:

United States

Language:

English

Subject:

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; science & technology - other topics; carbon capture and storage; electrocatalysis; materials for energy and catalysis; renewable energy