Molybdenum Carbide-Oxide Heterostructures: In Situ Surface Reconfiguration toward Efficient Electrocatalytic Hydrogen Evolution

Molybdenum Carbide-Oxide Heterostructures: In Situ Surface Reconfiguration toward Efficient Electrocatalytic Hydrogen Evolution
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碳化钼-氧化物异质结构:原位表面重构以实现高效电催化析氢

DOI:
10.1002/anie.201914752
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发表时间:
2020-01-24
影响因子:
16.6
通讯作者:
Gao, Qingsheng
Gao, Qingsheng
中科院分区:
化学1区
文献类型:
--
作者:
He, Liuqing;Zhang, Wenbiao;Gao, Qingsheng

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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 Mo-VI oxides on the surface are in situ reduced to Mo-IV, 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 Delta G(H*) 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 (eta(10)) 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.