Molybdenum Carbide-Oxide Heterostructures: In Situ Surface Reconfiguration toward Efficient Electrocatalytic Hydrogen Evolution.,Angewandte Chemie International Edition

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Molybdenum Carbide-Oxide Heterostructures: In Situ Surface Reconfiguration toward Efficient Electrocatalytic Hydrogen Evolution.
Angewandte Chemie International Edition ( IF 16.1 ) Pub Date : 2019-12-27 , DOI: 10.1002/anie.201914752
Liuqing He ₁ , Wenbiao Zhang ₁ , Qijie Mo ₁ , Wenjie Huang ₂ , Lichun Yang ₂ , Qingsheng Gao ₁

Affiliation

Heterostructured Mo2 C-MoOx on carbon cloth (Mo2 C-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 Mo2 C close to a thermodynamic neutral value, addressing difficult H* desorption toward fast HER kinetics. The optimized Mo2 C-MoOx /CC only requires a low overpotential (η10 ) of 60 mV at -10 mA cm-2 in 1.0 m HClO4 , outperforming Mo2 C/CC and most non-precious electrocatalysts. In situ surface reconfiguration are shown on W2 C-WOx , highlighting the significance to boost various metal-carbides and to identify active sites.

中文翻译：

碳化钼-氧化物异质结构：向高效电催化氢放出的原位表面重构。

研究了碳布上的异结构Mo2 C-MoOx（Mo2 C-MoOx / CC）作为环境条件下易氧化的电催化剂的模型，以揭示析氢反应（HER）过程中的表面重构。拉曼光谱结合电化学测试表明，表面上的MoVI氧化物被原位还原为MoIV，从而在酸性条件下完成了HER的促进反应。如密度泛函理论计算所表明的那样，带有末端Mo = O部分的原位还原表面可以有效地使裸Mo2 C上的负ΔGH*接近热力学中性值，从而解决了H *向快速HER动力学解吸的难题。经过优化的Mo2 C-MoOx / CC在1.0 m HClO4中在-10 mA cm-2下仅需60 mV的低过电势（η10），优于Mo2 C / CC和大多数非贵金属电催化剂。

更新日期：2020-01-24

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