Engineering the In-Plane Structure of Metallic Phase Molybdenum Disulfide via Co and O Dopants toward Efficient Alkaline Hydrogen Evolution

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 so...

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Bibliographic Details
Published in:ACS nano 2019-10, Vol.13 (10), p.11733-11740
Main Authors: Cao, Dengfeng, Ye, Ke, Moses, Oyawale Adetunji, Xu, Wenjie, Liu, Daobin, Song, Pin, Wu, Chuanqiang, Wang, Changda, Ding, Shiqing, Chen, Shuangming, Ge, Binghui, Jiang, Jun, Song, Li
Format: Article
Language:English
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Summary: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 in-plane 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 H2 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.
ISSN:1936-0851
1936-086X
DOI:10.1021/acsnano.9b05714