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Universal Sub-Nanoreactor Strategy for Synthesis of Yolk-Shell MoS2 Supported Single Atom Electrocatalysts toward Robust Hydrogen Evolution Reaction
Authors:Feilong Gong  Yuheng Liu  Yang Zhao  Prof Wei Liu  Prof Guang Zeng  Prof Guoqing Wang  Prof Yonghui Zhang  Lihua Gong  Prof Jian Liu
Institution:1. Key Laboratory of Surface and Interface Science and Technology of Henan Province, College of Material and Chemical Engineering, Zhengzhou University of Light Industry, Zhengzhou, Henan, 450001 P. R. China

Contribution: Conceptualization (equal), Formal analysis (equal), Funding acquisition (lead), ​Investigation (lead), Visualization (equal), Writing - original draft (lead);2. Key Laboratory of Surface and Interface Science and Technology of Henan Province, College of Material and Chemical Engineering, Zhengzhou University of Light Industry, Zhengzhou, Henan, 450001 P. R. China

Contribution: Data curation (lead), Formal analysis (equal), ​Investigation (equal), Validation (equal), Visualization (equal);3. State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, Liaoning, 116023 P. R. China

Contribution: Data curation (equal), Formal analysis (equal), Resources (equal), Validation (equal), Visualization (equal);4. State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, Liaoning, 116023 P. R. China

Contribution: Data curation (equal), Formal analysis (equal), ​Investigation (equal);5. Key Laboratory of Surface and Interface Science and Technology of Henan Province, College of Material and Chemical Engineering, Zhengzhou University of Light Industry, Zhengzhou, Henan, 450001 P. R. China

Contribution: Data curation (equal), Methodology (equal), Software (equal), Validation (equal);6. Key Laboratory of Surface and Interface Science and Technology of Henan Province, College of Material and Chemical Engineering, Zhengzhou University of Light Industry, Zhengzhou, Henan, 450001 P. R. China;7. State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, Liaoning, 116023 P. R. China

Abstract: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 (η10=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.
Keywords:Electrocatalyst  Nanostructures  Sub-Nanoreactor  Universal Strategy  Water Splitting
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