期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 -, 期 -, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202308091
关键词
Electrocatalyst; Nanostructures; Sub-Nanoreactor; Universal Strategy; Water Splitting
A universal sub-nanoreactor strategy was developed for synthesizing yolk-shell MoS2 supported single atom electrocatalysts with dual-anchored microenvironment, which showed robust hydrogen-evolution reaction performance. The optimized C-Co-MoS2 catalyst exhibited the lowest overpotential and significantly improved activity compared to previously reported MoS2-based electrocatalysts. Theoretical calculations and in situ characterizations revealed the active center and durability of the catalyst. This work provides a universal pathway for designing efficient electrocatalysts for electro-refinery.
The coordination structure determines the electrocatalytic performances of single atom catalysts (SACs), while it remains a challenge to precisely regulate their spatial location and coordination environment. Herein, we report a universal sub-nanoreactor strategy for synthesis of yolk-shell MoS2 supported single atom electrocatalysts with dual-anchored microenvironment of vacancy-enriched MoS2 and intercalation carbon toward robust hydrogen-evolution reaction. Theoretical calculations reveal that the E-Lock and E-Channel are conducive to stabilize and activate metal single atoms. A group of SACs is subsequently produced with the assistance of sulfur vacancy and intercalation carbon in the yolk-shell sub-nanoreactor. The optimized C-Co-MoS2 yields the lowest overpotential (& eta;(10)=17 mV) compared with previously reported MoS2-based electrocatalysts to date, and also affords a 5-9 fold improvement in activity even comparing with those as-prepared single-anchored analogues. Theoretical results and in situ characterizations unveil its active center and durability. This work provides a universal pathway to design efficient catalysts for electro-refinery.
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