Unveiling the in-situ hydrogen intercalation in Mo2COx for promoting the alkaline hydrogen evolution reaction

IF 20.2 1区化学 Q1 CHEMISTRY, PHYSICAL Applied Catalysis B: Environmental Pub Date : 2023-09-05 DOI:10.1016/j.apcatb.2023.122739

Hong Chuan Fu, Xiao Hui Chen, Bo Yang, Yuan Hao Luo, Ting Li, Xiao Hu Wang, Qing Zhang, Xiao Lin Li, Nian Bing Li, Hong Qun Luo

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引用次数: 1

Abstract

Dimolybdenum carbide (Mo₂C) is an efficient electrocatalyst for the hydrogen evolution reaction (HER). However, Mo₂C tends to undergo surface chemical reconstruction under reaction conditions, which presents difficulties for optimization and characterization. Here, we report an HER activated Mo₂CO_x–Ni(OH)₂ catalyst and demonstrate that structural transformations including the surface oxidation of Mo₂C and the in-situ hydrogen intercalation of Mo₂CO_x govern the promoted HER performance. The electrochemically induced hydrogen intercalation from Mo₂CO_x to H_xMo₂CO_x was identified by in-situ cyclic voltammetry characterization, and the significant role of hydrogen intercalation in surface-mediated HER pathway has been revealed by in-situ electrochemical impedance characterization. Density functional theory calculations indicate that hydrogen intercalation enables the HER by addressing sluggish water dissociation toward fast kinetics. Overall, this work underscores the importance of tracking the structure dynamic alteration of Mo₂C-based material under the reaction conditions.

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揭示了Mo2COx中原位插氢促进碱性析氢反应的机理

碳化二钼(Mo2C)是一种高效的析氢反应电催化剂。然而，在反应条件下，Mo2C容易发生表面化学重构，这给优化和表征带来了困难。本文报道了一种HER活化的Mo2COx - ni (OH)2催化剂，并证明了Mo2C的表面氧化和Mo2COx的原位插氢等结构转变控制了HER性能的提升。通过原位循环伏安法表征确定了电化学诱导的氢从Mo2COx插入到HxMo2COx，并通过原位电化学阻抗表征揭示了氢插入在表面介导的HER途径中的重要作用。密度泛函理论计算表明，插入氢通过解决缓慢的水解离向快速动力学方向发展，使HER成为可能。总之，这项工作强调了在反应条件下追踪mo2c基材料结构动态变化的重要性。

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来源期刊

Applied Catalysis B: Environmental 环境科学-工程：化工

CiteScore

38.60

自引率

6.30%

发文量

1117

审稿时长

24 days

期刊介绍： Applied Catalysis B: Environment and Energy (formerly Applied Catalysis B: Environmental) is a journal that focuses on the transition towards cleaner and more sustainable energy sources. The journal's publications cover a wide range of topics, including: 1.Catalytic elimination of environmental pollutants such as nitrogen oxides, carbon monoxide, sulfur compounds, chlorinated and other organic compounds, and soot emitted from stationary or mobile sources. 2.Basic understanding of catalysts used in environmental pollution abatement, particularly in industrial processes. 3.All aspects of preparation, characterization, activation, deactivation, and regeneration of novel and commercially applicable environmental catalysts. 4.New catalytic routes and processes for the production of clean energy, such as hydrogen generation via catalytic fuel processing, and new catalysts and electrocatalysts for fuel cells. 5.Catalytic reactions that convert wastes into useful products. 6.Clean manufacturing techniques that replace toxic chemicals with environmentally friendly catalysts. 7.Scientific aspects of photocatalytic processes and a basic understanding of photocatalysts as applied to environmental problems. 8.New catalytic combustion technologies and catalysts. 9.New catalytic non-enzymatic transformations of biomass components. The journal is abstracted and indexed in API Abstracts, Research Alert, Chemical Abstracts, Web of Science, Theoretical Chemical Engineering Abstracts, Engineering, Technology & Applied Sciences, and others.