期刊
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
卷 142, 期 13, 页码 6400-6408出版社
AMER CHEMICAL SOC
DOI: 10.1021/jacs.0c01699
关键词
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资金
- National Natural Science Foundation of China [21521001, 21431006, 21225315, 21321002, 91645202, 21975237, 51702312]
- Users with Excellence and Scientific Research Grant of Hefei Science Center of CAS [2015HSCUE007]
- Key Research Program of Frontier Sciences, CAS [QYZDJ-SSW-SLH036]
- National Basic Research Program of China [2014CB931800, 2018YFA0702001]
- Chinese Academy of Sciences [KGZD-EW-T05, XDA090301001]
- Strategic Priority Research Program of the Chinese Academy of Sciences [XDA21000000]
- Fundamental Research Funds for the Central Universities [WK2060190045, WK2340000076]
- Recruitment Program of Global Youth Experts
Selective and efficient catalytic conversion of carbon dioxide (CO2) into value-added fuels and feedstocks provides an ideal avenue to high-density renewable energy storage. An impediment to enabling deep CO2 reduction to oxygenates and hydrocarbons (e.g., C2+ compounds) is the difficulty of coupling carbon-carbon bonds efficiently. Copper in the +1 oxidation state has been thought to be active for catalyzing C2+ formation, whereas it is prone to being reduced to Cu-0 at cathodic potentials. Here we report that catalysts with nanocavities can confine carbon intermediates formed in situ, which in turn covers the local catalyst surface and thereby stabilizes Cu+ species. Experimental measurements on multihollow cuprous oxide catalyst exhibit a C2+ Faradaic efficiency of 75.2 +/- 2.7% at a C2+ partial current density of 267 +/- 13 mA cm(-2) and a large C2+-to-C-1 ratio of similar to 7.2. Operando Raman spectra, in conjunction with X-ray absorption studies, confirm that Cu+ species in the as-designed catalyst are well retained during CO2 reduction, which leads to the marked C2+ selectivity at a large conversion rate.
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