Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 59, Issue 12, Pages 4814-4821Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201916538
Keywords
carbon dioxide reduction; electrochemistry; hierarchical structures; interfaces; tin oxide
Categories
Funding
- National Key R&D Program of China [2017YFA0700102]
- National Natural Science Foundation of China [21573222, 91545202, 21802124, 91845103]
- Dalian National Laboratory for Clean Energy [DNL180404]
- Dalian Institute of Chemical Physics [DICP DMTO201702]
- Dalian Outstanding Young Scientist Foundation [2017RJ03]
- Strategic Priority Research Program of the Chinese Academy of Sciences [XDB17020200]
- CAS Youth Innovation Promotion [2015145]
- China Postdoctoral Science Foundation [2018M630307, 2019T120220]
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The electrochemical CO2 reduction reaction (CO2RR) to give C-1 (formate and CO) products is one of the most techno-economically achievable strategies for alleviating CO2 emissions. Now, it is demonstrated that the SnOx shell in Sn2.7Cu catalyst with a hierarchical Sn-Cu core can be reconstructed in situ under cathodic potentials of CO2RR. The resulting Sn2.7Cu catalyst achieves a high current density of 406.7 +/- 14.4 mA cm(-2) with C-1 Faradaic efficiency of 98.0 +/- 0.9 % at -0.70 V vs. RHE, and remains stable at 243.1 +/- 19.2 mA cm(-2) with a C-1 Faradaic efficiency of 99.0 +/- 0.5 % for 40 h at -0.55 V vs. RHE. DFT calculations indicate that the reconstructed Sn/SnOx interface facilitates formic acid production by optimizing binding of the reaction intermediate HCOO* while promotes Faradaic efficiency of C-1 products by suppressing the competitive hydrogen evolution reaction, resulting in high Faradaic efficiency, current density, and stability of CO2RR at low overpotentials.
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