期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 61, 期 21, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202116706
关键词
AgI-CuO; CO2 Electroreduction; Cu-0; Cu+ Sites; Iodine Ions Leaching; Tandem Catalysts
资金
- National Natural Science Foundation of China [22071069, 21805102, 21825103]
- Hubei Provincial Natural Science Foundation of China [2019CFA002]
- Foundation of Basic and Applied Basic Research of Guangdong Province [2019B1515120087]
- Natural Science Foundation of Anhui province [2008085QB81]
- Education Department of Anhui Province Foundation [KJ2019A0503]
- Analytical and Testing Center at Huazhong University of Science and Technology
In this study, the interaction and active origin of dual components in a tandem catalyst were investigated using multiple operando techniques. The results revealed that the leaching of iodine ions from AgI restricted the complete reduction of CuO, leading to the formation of stable active Cu-0/Cu+ species. This self-adaptive dual-optimization strategy resulted in excellent C2+ Faradaic efficiency of the catalyst.
Tandem catalysts can divide the reaction into distinct steps by local multiple sites and thus are attractive to trigger CO2RR to C2+ products. However, the evolution of catalysts generally exists during CO2RR, thus a closer investigation of the reconstitution, interplay, and active origin of dual components in tandem catalysts is warranted. Here, taking AgI-CuO as a conceptual tandem catalyst, we uncovered the interaction of two phases during the electrochemical reconstruction. Multiple operando techniques unraveled that in situ iodine ions leaching from AgI restrained the entire reduction of CuO to acquire stable active Cu-0/Cu+ species during the CO2RR. This way, the residual iodine species of the Ag matrix accelerated CO generation and iodine-induced Cu-0/Cu+ promotes C-C coupling. This self-adaptive dual-optimization endowed our catalysts with an excellent C2+ Faradaic efficiency of 68.9 %. Material operando changes in this work offer a new approach for manipulating active species towards enhancing C2+ products.
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