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首页> 外文期刊>Advanced Functional Materials >Monitoring Hydrogen Evolution Reaction Intermediates of Transition Metal Dichalcogenides via Operando Raman Spectroscopy
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Monitoring Hydrogen Evolution Reaction Intermediates of Transition Metal Dichalcogenides via Operando Raman Spectroscopy

机译：通过操作公司拉曼光谱监测过渡金属二甲甲基甲基化物的氢进化反应中间体

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摘要

A deeper understanding of the water-splitting hydrogen evolution reaction (HER) mechanism during photocatalytic processes is crucial for the rational design of efficient photocatalysts. In particular, the HER mechanism promoted by multielement hybrid structures remains extremely challenging and elusive. Herein, an in situ photoelectrochemical/Raman measurement system is employed to monitor the HER mechanism of hybrid nanostructures under realistic working conditions via operando Raman spectra and linear-sweep voltammetry curves. As a proof of concept, tunable composition transition metal dichalcogenides MoS(2)(x)Se(2(1-)(x)())nanosheets are used as a model photocatalyst to unveil the corresponding photocatalytic mechanism. The spectroscopic studies reveal that hydrogen atoms can be adsorbed to active sulfur and selenium atoms via intermediate species formed during the photocatalytic process. More importantly, the studies demonstrate that an exponential relationship exists between the number of reactive electrons and the Raman intensity of intermediate species, which can serve as a guideline to directly evaluate the HER performance in photocatalysts by comparing the Raman intensities of the intermediate species. As a simple, intuitive, and general analytical method, the designed operando Raman measurement approach provides a new tool for elucidating catalytic reaction mechanisms in a realistic and complex environment; and strategically improving H(2)production performance of multielement photocatalysts.
机译：在光催化过程中对水分裂氢进化反应（她）机理的更深入了解，对于有效光催化剂的合理设计至关重要。特别是，由多元化杂交结构促进的她的机制仍然非常具有挑战性和难以捉摸。这里，采用原位光电化学/拉曼测量系统来监测通过Operando拉曼光谱和线性扫描伏安法曲线在现实工作条件下的杂化纳米结构的机理。作为概念的证据，可调谐组合物过渡金属二甲硅藻剂MOS（2）（x）Se（2（1 - ）（x）（x））纳米晶片用作模型光催化剂，以推出相应的光催化机制。光谱研究表明，通过在光催化过程中形成的中间物质可以吸附到活性硫和硒原子中的氢原子。更重要的是，研究表明，在反应电子和中间物种的拉曼强度之间存在指数关系，其可以作为直接评估光催化剂在光催化剂中的性能的指导。作为一种简单，直观和一般的分析方法，设计的操作寿测定方法提供了一种用于阐明催化反应机制在现实和复杂的环境中的新工具;并策略性地改善H（2）多元素光催化剂的生产性能。

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  • 来源
    《Advanced Functional Materials》 |2020年第35期|2003035.1-2003035.9|共9页
  • 作者

    Guo Shaohui; Li Yaohua; Tang Songwei; Zhang Yuanyuan; Li Xuanhua; Sobrido Ana Jorge; Titirici Maria-Magdalena; Wei Bingqing;

  • 作者单位

    Northwestern Polytech Univ Sch Mat Sci & Engn Ctr Nano Energy Mat State Key Lab Solidificat Proc Xian 710072 Shaanxi Peoples R China;

    Taiyuan Satellite Launch Ctr Yinchuan Branch Yinchuan 750000 Ningxia Peoples R China;

    Northwestern Polytech Univ Sch Mat Sci & Engn Ctr Nano Energy Mat State Key Lab Solidificat Proc Xian 710072 Shaanxi Peoples R China;

    Northwestern Polytech Univ Sch Mat Sci & Engn Ctr Nano Energy Mat State Key Lab Solidificat Proc Xian 710072 Shaanxi Peoples R China;

    Northwestern Polytech Univ Sch Mat Sci & Engn Ctr Nano Energy Mat State Key Lab Solidificat Proc Xian 710072 Shaanxi Peoples R China;

    Queen Mary Univ London Sch Engn & Mat Sci Fac Sci & Engn Mile End Rd London E1 4NS England;

    Imperial Coll London Dept Chem Engn South Kensington Campus London SW7 2AZ England;

    Univ Delaware Dept Mech Engn Newark DE 19716 USA;

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  • 正文语种 eng
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  • 关键词

    multielement photocatalysts; operando Raman spectroscopy; photocatalytic reaction intermediates; transition metal dichalcogenides;

    机译：多元首光催化剂;手术用raman光谱;光催化反应中间体;过渡金属二硫代甲基化物;

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