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Molybdenum Carbide-Oxide Heterostructures: In Situ Surface Reconfiguration toward Efficient Electrocatalytic Hydrogen Evolution
Authors:Liuqing He  Wenbiao Zhang  Qijie Mo  Wenjie Huang  Prof. Dr. Lichun Yang  Prof. Dr. Qingsheng Gao
Affiliation:1. College of Chemistry and Materials Science, Jinan University, Guangzhou, 510632 China;2. School of Materials Science and Engineering, and Guangdong Provincial Key Laboratory of Advanced Energy Storage Materials, South China University of Technology, Guangzhou, 510640 China
Abstract:Heterostructured Mo2C-MoOx on carbon cloth (Mo2C-MoOx/CC), as a model of easily oxidized electrocatalysts under ambient conditions, is investigated to uncover surface reconfiguration during the hydrogen evolution reaction (HER). Raman spectroscopy combined with electrochemical tests demonstrates that the MoVI oxides on the surface are in situ reduced to MoIV, accomplishing promoted HER in acidic condition. As indicated by density functional theoretical calculations, the in situ reduced surface with terminal Mo=O moieties can effectively bring the negative ΔGH* on bare Mo2C close to a thermodynamic neutral value, addressing difficult H* desorption toward fast HER kinetics. The optimized Mo2C-MoOx/CC only requires a low overpotential (η10) of 60 mV at −10 mA cm−2 in 1.0 m HClO4, outperforming Mo2C/CC and most non-precious electrocatalysts. In situ surface reconfiguration are shown on W2C-WOx, highlighting the significance to boost various metal-carbides and to identify active sites.
Keywords:Heterogrenzflächen  Wasserstoffentwicklung  In-situ-Rekonfiguration  Molybdäncarbide  Oberflächensauerstoff
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