4.8 Article

All-pH Stable Sandwich-Structured MoO2/MoS2/C Hollow Nanoreactors for Enhanced Electrochemical Hydrogen Evolution

期刊

ADVANCED FUNCTIONAL MATERIALS
卷 31, 期 27, 页码 -

出版社

WILEY-V C H VERLAG GMBH
DOI: 10.1002/adfm.202101715

关键词

all‐ pH stability; electrocatalytic hydrogen evolution; MoS; (2); nanoreactors; vacancies

资金

  1. National Natural Science Foundation of China [NSFC: 52002359, 21902157]
  2. Dalian National Laboratory for Clean Energy (DNL), CAS
  3. DNL Cooperation Fund, CAS [DNL180402]
  4. Key Program of Henan Province for Science and Technology [192102210018]

向作者/读者索取更多资源

A novel design of MoO2/MoS2/C hollow nanoreactors with high electrocatalytic efficiency for hydrogen evolution over all pH values is reported. The introduction of sulfur vacancies on MoO2 substrates and the design of defective carbon shells enhance the stability of the electrocatalysts in acidic and alkaline media, showing potential for durable hydrogen evolution. The vacancy engineering can regulate the band structures, electron density differences, total density of states, and adsorption-dissociation ability of H* and H2O over the entire pH range, providing insights for the rational development of practical pH-universal electrocatalysts.
Molybdenum sulfide has great potential for the electrocatalytic hydrogen evolution, but its structural instability in acidic media and high barriers in alkaline/neutral media limits its practical applications. Herein, the design of monodispersed sandwich-structured MoO2/MoS2/C hollow nanoreactors is reported with a triple layer conductor/catalyst/protector configuration for efficient electrochemical hydrogen evolution over all pH values. Metallic MoO2 substrates with ultrahigh pristine electroconductivity can promote the charge transfer while sulfur vacancies are introduced to activate the highly exposed (002) facets of MoS2. The optimized MoO2/MoS2/C nanoreactor exhibits overpotentials of 77, 91, and 97 mV (10 mA cm(-2)) and Tafel slopes of 41, 49, and 53 mV dec(-1) in acidic, alkaline, and neutral media, respectively, which are much better than most of the MoS2-based electrocatalysts. Moreover, defective carbon shells are in situ generated, preventing the electrocatalysts from corrosion in acidic and alkaline media; the structural stability is verified via in situ Raman and XRD characterizations. Based on the density functional theory calculations, vacancy engineering can regulate the band structures, electron density differences, total density of states, and the H* and H2O adsorption-dissociation ability over the entire pH range. The findings may shed light on the rational development of practical pH-universal electrocatalysts for durable hydrogen evolution.

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