TY - JOUR
T1 - Efficient upgrading of CO to C3 fuel using asymmetric C-C coupling active sites
AU - Wang, Xue
AU - Wang, Ziyun
AU - Zhuang, Tao-Tao
AU - Dinh, Cao-Thang
AU - Li, Jun
AU - Nam, Dae-Hyun
AU - Li, Fengwang
AU - Huang, Chun-Wei
AU - Tan, Chih-Shan
AU - Chen, Zitao
AU - Chi, Miaofang
AU - Gabardo, Christine M.
AU - Seifitokaldani, Ali
AU - Todorović, Petar
AU - Proppe, Andrew
AU - Pang, Yuanjie
AU - Kirmani, Ahmad R.
AU - Wang, Yuhang
AU - Ip, Alexander H.
AU - Richter, Lee J.
AU - Scheffel, Benjamin
AU - Xu, Aoni
AU - Lo, Shen-Chuan
AU - Kelley, Shana O.
AU - Sinton, David
AU - Sargent, Edward H.
PY - 2019
Y1 - 2019
N2 - 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.
AB - 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.
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U2 - 10.1038/s41467-019-13190-6
DO - 10.1038/s41467-019-13190-6
M3 - RGC 21 - Publication in refereed journal
C2 - 31780655
SN - 2041-1723
VL - 10
JO - Nature Communications
JF - Nature Communications
M1 - 5186
ER -