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Modulating ultrafast carrier dynamics behavior via vacancy engineering of ReSe2 with Se vacancy for efficient electrochemical activity
Chemical Engineering Journal ( IF 15.1 ) Pub Date : 2024-03-26 , DOI: 10.1016/j.cej.2024.150724
Ming-Kun Jiang , Yu-Xin Liu , Shan-Shan Kan , Shi-Xuan Deng , Zhe-Kun Ren , Xiao-Meng Jiang , Cheng-Bao Yao

Vacancy engineering is powerful for manipulating material properties. Selenium vacancies (V) exert significantly impact on the physicochemical properties of rhenium diselenide (ReSe), triggering applications in catalysis and photoelectric devices. However, the effects on electronic structure, carrier lifetime, and electrochemical activity are inadequately explored and poorly elucidated. Herein, hydrothermal-controlled growth of ReSe with V is synthesized by different strategies. The ethanol-assisted hydrothermal method can adjust V concentration of ReSe on carbon paper by time parameters. Mediated excitonic effects were characterized in the transient absorption spectroscopy and photoluminescence of V-regulated ReSe. The defect level produces unique defect emission peak, and the V-mediated exciton dynamics problem was discussed. The transient absorption result shows that high V concentration can optimize carrier lifetime, carrier separation efficiency, and electron utilization. The electrocatalytic hydrogen evolution reaction of ReSe catalyst revealed the electrochemical activity regulation by V concentration, which provides ideas for enhancing catalyst performance. Density functional theory result confirms the role of selenium vacancies in the regulation of the electronic structure of ReSe. This work proffers an optimal solution strategy for hydrothermal preparation of ReSe, and demonstrates the feasibility of regulating electrochemical activity by vacancy engineering. The excellent performance is beneficial for water cracking and physical devices.

中文翻译:

通过带有 Se 空位的 ReSe2 空位工程来调节超快载流子动力学行为,以实现高效的电化学活性

空位工程对于操纵材料特性非常有用。硒空位 (V) 对二硒化铼 (ReSe) 的物理化学性质产生显着影响,从而引发了在催化和光电器件中的应用。然而,其对电子结构、载流子寿命和电化学活性的影响尚未得到充分探索和阐明。在此,通过不同的策略合成了 ReSe 与 V 的水热控制生长。乙醇辅助水热法可以通过时间参数调节碳纸上ReSe的V浓度。通过 V 调节 ReSe 的瞬态吸收光谱和光致发光来表征介导的激子效应。缺陷能级产生独特的缺陷发射峰,并讨论了V介导的激子动力学问题。瞬态吸收结果表明,高 V 浓度可以优化载流子寿命、载流子分离效率和电子利用率。 ReSe催化剂的电催化析氢反应揭示了V浓度对电化学活性的调节,为提高催化剂性能提供了思路。密度泛函理论结果证实了硒空位在ReSe电子结构调控中的作用。这项工作为水热制备ReSe提供了一种优化的解决策略,并证明了通过空位工程调节电化学活性的可行性。优异的性能有利于水裂解和物理装置。
更新日期:2024-03-26
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