通过Operando拉曼光谱法监测过渡金属二硫属元素的析氢反应中间体,Advanced Functional Materials

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通过Operando拉曼光谱法监测过渡金属二硫属元素的析氢反应中间体
Advanced Functional Materials ( IF 18.5 ) Pub Date : 2020-07-09 , DOI: 10.1002/adfm.202003035
Shaohui Guo ₁ , Yaohua Li ₂ , Songwei Tang ₁ , Yuanyuan Zhang ₁ , Xuanhua Li ₁ , Ana Jorge Sobrido ₃ , Maria‐Magdalena Titirici ₄ , Bingqing Wei ₅

Affiliation

深入理解光催化过程中的水分解氢放出反应（HER）机理对于合理设计有效的光催化剂至关重要。尤其是，由多元混合结构促进的HER机制仍然极具挑战性和难以捉摸。本文中，采用原位光电化学/拉曼测量系统通过操作拉曼光谱和线性扫描伏安曲线监测在实际工作条件下杂化纳米结构的HER机理。作为概念验证，可调谐组成的过渡金属二硫化_二钼MoS ₂_x Se _2（1-_x_）纳米片用作模型光催化剂以揭示相应的光催化机理。光谱研究表明，氢原子可以通过在光催化过程中形成的中间物种吸附到活性硫和硒原子上。更重要的是，研究表明，反应性电子的数量与中间物种的拉曼强度之间存在指数关系，这可作为通过比较中间物种的拉曼强度直接评估HER在光催化剂中性能的指南。作为一种简单，直观且通用的分析方法，设计的拉曼操作测量方法提供了一种新工具，用于阐明现实和复杂环境中的催化反应机理。并战略性地改善H₂多元光催化剂的生产性能。

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Monitoring Hydrogen Evolution Reaction Intermediates of Transition Metal Dichalcogenides via Operando Raman Spectroscopy

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 MoS₂_xSe₂₍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 H₂ production performance of multielement photocatalysts.

更新日期：2020-08-26

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