空位工程介导的中空结构 ZnO/ZnS S 型异质结用于高效光催化制取 H2

IF 15.7 1区 化学 Q1 CHEMISTRY, APPLIED Chinese Journal of Catalysis Pub Date : 2024-09-01 DOI:10.1016/S1872-2067(24)60099-9
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摘要

设计具有空位工程的阶梯型(S-scheme)异质结光催化剂是实现高效光催化产生 H2 活性的可靠方法。本文通过离子交换和煅烧处理,合理地构建了具有 O 和 Zn 空位(VO,Zn-ZnO/ZnS)的中空 ZnO/ZnS S 型异质结。在这种光催化系统中,中空结构结合双空位的引入,使其具有足够的光吸收能力。此外,O 空位和 Zn 空位分别作为光诱导电子和空穴的捕获位点,有利于促进光诱导载流子分离。同时,S 型电荷转移机制不仅能提高光诱导载流子的分离和转移效率,还能保持较强的氧化还原能力。正如预期的那样,优化的 VO、Zn-ZnO/ZnS 异质结的光催化 H2 产率高达 160.91 mmol g-1 h-1,分别是纯 ZnO 和 ZnS 的约 643.6 倍和 214.5 倍。同时,实验结果和密度泛函理论计算表明,光诱导载流子转移途径遵循 S 型异质结机制,O 和 Zn 空位的引入降低了表面反应势垒。这项工作为太阳能到燃料的能量转换提供了一种在 S 型异质结中进行空位工程的创新策略。
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Vacancy engineering mediated hollow structured ZnO/ZnS S-scheme heterojunction for highly efficient photocatalytic H2 production

Designing a step-scheme (S-scheme) heterojunction photocatalyst with vacancy engineering is a reliable approach to achieve highly efficient photocatalytic H2 production activity. Herein, a hollow ZnO/ZnS S-scheme heterojunction with O and Zn vacancies (VO, Zn-ZnO/ZnS) is rationally constructed via ion-exchange and calcination treatments. In such a photocatalytic system, the hollow structure combined with the introduction of dual vacancies endows the adequate light absorption. Moreover, the O and Zn vacancies serve as the trapping sites for photo-induced electrons and holes, respectively, which are beneficial for promoting the photo-induced carrier separation. Meanwhile, the S-scheme charge transfer mechanism can not only improve the separation and transfer efficiencies of photo-induced carrier but also retain the strong redox capacity. As expected, the optimized VO, Zn-ZnO/ZnS heterojunction exhibits a superior photocatalytic H2 production rate of 160.91 mmol g–1 h–1, approximately 643.6 times and 214.5 times with respect to that obtained on pure ZnO and ZnS, respectively. Simultaneously, the experimental results and density functional theory calculations disclose that the photo-induced carrier transfer pathway follows the S‐scheme heterojunction mechanism and the introduction of O and Zn vacancies reduces the surface reaction barrier. This work provides an innovative strategy of vacancy engineering in S-scheme heterojunction for solar‐to‐fuel energy conversion.

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来源期刊
Chinese Journal of Catalysis
Chinese Journal of Catalysis 工程技术-工程:化工
CiteScore
25.80
自引率
10.30%
发文量
235
审稿时长
1.2 months
期刊介绍: The journal covers a broad scope, encompassing new trends in catalysis for applications in energy production, environmental protection, and the preparation of materials, petroleum chemicals, and fine chemicals. It explores the scientific foundation for preparing and activating catalysts of commercial interest, emphasizing representative models.The focus includes spectroscopic methods for structural characterization, especially in situ techniques, as well as new theoretical methods with practical impact in catalysis and catalytic reactions.The journal delves into the relationship between homogeneous and heterogeneous catalysis and includes theoretical studies on the structure and reactivity of catalysts.Additionally, contributions on photocatalysis, biocatalysis, surface science, and catalysis-related chemical kinetics are welcomed.
期刊最新文献
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