期刊
ACS NANO
卷 13, 期 10, 页码 11733-11740出版社
AMER CHEMICAL SOC
DOI: 10.1021/acsnano.9b05714
关键词
molybdenum disulfide; alkaline hydrogen evolution reaction; heteroatom doping; structure-performance relationship; water dissociation kinetics
类别
资金
- National Key R&D Program of China [2017YFA0303500]
- NSFC [U1932201, 11574280, 11605201]
- China Postdoctoral Science Foundation [2018M630709]
- Anhui Provincial Natural Science Foundation [1908085QB51]
- Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education)
- Nankai University (111 project) [B12015]
Molybdenum disulfide (MoS2) has attracted much attention as a promising alternative to Pt-based catalysts for highly efficient hydrogen generation. However, it suffers sluggish kinetics for driving the hydrogen evolution reaction (HER) process because of inert basal planes, especially in alkaline solution. Here, we show a combination of heteroatom doping and phase transformation strategies to engineer the inplane structure of MoS2, that trigger their catalytic activities. Systematic characterizations are performed with advanced aberration-corrected microscopy and X-ray techniques, indicating that an as-designed MoS2 catalyst has a distorted zigzag-chain superlattice in metallic phase, while its in-plane structure was engineered via the incorporation of cobalt and oxygen species. The optimal Co, O dual-doped metallic phase molybdenum disulfide (1T-MoS2) electrocatalyst shows a significantly enhanced HER activity with a low overpotential of 113 mV at 10 mA cm(-2) and corresponding small Tafel slope of 50 mV dec(-1), accompanied by the robust stability in alkaline media. The calculated turnover frequency is higher than 6.65 H-2 s(-1) at an overpotential of 200 mV. More in-depth insights from the first-principle calculations illustrate that the water dissociation as a rate-determining step was largely accelerated by the in-plane Co-O-Mo species and fast electron transfer of the catalyst. Benefiting from ingenious design and fine identifications, this work provides a fundamental understanding of the relationships among heteroatom doping, phase transformation, and performance for MoS2-based catalysts.
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