期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 58, 期 51, 页码 18676-18682出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201911470
关键词
atomic rearrangement; cobalt; electron configuration; hydrogen evolution reaction (HER); nanosheets
资金
- National Natural Science Foundation of China (NSFC) [21931001, 21922105, 21571089]
- Fundamental Research Funds for the Central Universities [lzujbky-2018-k08, lzujbky-2019-it10, lzujbky2018-it40, lzujbky-2017-it42]
- Special Fund Project of Guiding Scientific and Technological Innovation Development of Gansu Province [2019ZX-04]
- NSFC [21771156]
- Early Career Scheme (ECS) fund from the Research Grant Council (RGC) in Hong Kong [PolyU 253026/16P]
We report a novel modulation strategy by introducing transition metals into NiS2 nanosheets (NSs) to flexibly optimize the electronic configurations and atomic arrangement. The Co-NiS2 NSs exhibit excellent hydrogen evolution reaction (HER) performance with an overpotential of 80 mV at j=10 mA cm(-2) and long-term stability of 90 h in alkaline media. The turnover frequencies (TOFs) of 0.55 and 4.1 s(-1) at an overpotential of 100 and 200 mV also confirm their remarkable performance. DFT calculations reveal that the surface dopants abnormally sensitize surface Ni-3d bands in the long-range order towards higher electron-transfer activity, acting as the electron-depletion center. Meanwhile, the high lying surface S-sites possess substantially high selectivity for splitting the adsorbing H2O that guarantee the high HER performance within alkaline conditions. This work opens opportunities for enhancing water splitting by atomic-arrangement-assisted electronic modulation via a facile doping strategy.
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