期刊
SMALL
卷 18, 期 39, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/smll.202203173
关键词
hydrogen evolution reaction; MoS; (2) basal plane; oxygen evolution reaction; sulfur vacancies; transition metal doping
类别
资金
- National Natural Science Foundation of China [51972030, U2004210, 21875080, 51572100]
- Innovative Research Group Project of the Natural Science Foundation of Hubei Province [2019CFA020]
- Major Project of Technology Innovation of Hubei Province [2018AAA011]
- Special Projects for Local Science and Technology Development Guided by the Chinese Central Government [2019ZYYD024]
- HUST Key Interdisciplinary Team Project [2016JCTD101]
- City University of Hong Kong Strategic Research Grant [7005505]
Activation of the basal planes of MoS2 using sulfur vacancies and transition metal doping can achieve efficient hydrogen and oxygen evolution reactions. This approach can be extended to other TMDs for high-efficiency electrocatalysis.
2D transition metal disulfides (TMDs) are promising and cost-effective alternatives to noble-metal-based catalysts for hydrogen production. Activation of the inert basal plane of TMDs is crucial to improving the catalytic efficiency. Herein, introduction of in-plane sulfur vacancies (S-v) and 3d transition metal dopants in concert activates the basal planes of MoS2 (M-S-v-MoS2) to achieve high activities in the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER). Acetate introducing mild wet chemical etching removes surface S atoms facilitating subsequent cation exchange between the exposed Mo atoms and targeted metal ions in solution. Density-functional theory calculation demonstrates that the exposed 3d transition metal dopants in MoS2 basal planes serve as multifunctional active centers, which not only reduce Delta G(H*) but also accelerate water oxidation. As a result, the optimal Ni-S-v-MoS2 and Co-S-v-MoS2 electrocatalysts show excellent stability and alkaline HER and OER characteristics such as low overpotentials of 101 and 190 mV at 10 mA cm(-2), respectively. The results reveal a strategy to activate the inert MoS2 basal planes by defect and doping co-engineering and the technique can be extended to other types of TMDs for high-efficiency electrocatalysis beyond water splitting.
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