Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 144, Issue 1, Pages 259-269Publisher
AMER CHEMICAL SOC
DOI: 10.1021/jacs.1c09508
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Funding
- National Basic Research Program of China [2018YFA0702001]
- National Natural Science Foundation of China [21975237, 22175162]
- Anhui Provincial Research and Development Program [202004a05020073]
- USTC Research Funds of the Double First-Class Initiative [YD2340002007]
- Fundamental Research Funds for the Central Universities [WK2340000101]
- Recruitment Program of Global Youth Experts
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The study demonstrates that oxide-derived copper crystals enclosed by Cu(100)/Cu(111) interfaces can efficiently reduce CO2 to multicarbon products with high Faradaic efficiency. Combining experimental and computational studies reveals that these interfaces have a favorable local electronic structure that enhances catalytic activity.
The electrosynthesis of valuable multicarbon chemicals using carbon dioxide (CO2) as a feedstock has substantially progressed recently but still faces considerable challenges. A major difficulty lines in the sluggish kinetics of forming carbon-carbon (C-C) bonds, especially in neutral media. We report here that oxide-derived copper crystals enclosed by six {100} and eight {111} facets can reduce CO2 to multicarbon products with a high Faradaic efficiency of 74.9 +/- 1.7% at a commercially relevant current density of 300 mA cm(-2) in 1 M KHCO3 (pH similar to 8.4). By combining the experimental and computational studies, we uncovered that Cu(100)/Cu(111) interfaces offer a favorable local electronic structure that enhances *CO adsorption and lowers C-C coupling activation energy barriers, performing superior to Cu(100) and Cu(111) surfaces, respectively. On this catalyst, no obvious degradation was observed at 300 mA cm(-2) over 50 h of continuous operation.
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