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Synergistic Effect of the Surface Vacancy Defects for Promoting Photocatalytic Stability and Activity of ZnS Nanoparticles
ACS Catalysis ( IF 11.3 ) Pub Date : 2021-10-17 , DOI: 10.1021/acscatal.1c03476
Bin Xiao 1 , Tianping Lv 1 , Jianhong Zhao 1 , Qian Rong 1 , Hong Zhang 2 , Haitang Wei 1 , Jingcheng He 1 , Jin Zhang 1 , Yumin Zhang 1 , Yong Peng 2 , Qingju Liu 1
Affiliation  

High activity, high stability, and low cost have always been the pursuit of photocatalyst design and development. Herein, a simple method is used to integrate abundant anion vacancies (VS) and cation vacancies (VZn) on the surface of ZnS (M–ZnS), deriving VS and VZn pairs (vacancy pairs), isolated Zn atoms (Zniso), and isolated S atoms (Siso). Abundant surface vacancy defects fully expose and activate the surface atoms, regulate the band structure, and significantly improve the separation of photogenerated carriers. M–ZnS is endowed with high activity, and the average hydrogen production rate of the optimal sample increases to 576.07 μmol·g–1·h–1 (λ > 400 nm). Theoretical simulations indicate that the activated Zn atoms are the dominant active sites via the formation of a Zn–OH bond with H2O. Especially, the strong interactions of electrons in atomic orbitals at vacancy pairs and the introduction of VZn are conducive to high stability. The optimal sample maintains an average hydrogen production rate of 6.59 mmol·g–1·h–1 (300 W Xe lamp) after nine cycles. Hence, this work deepens the understanding of vacancy defects and provides an idea for the design of a stable photocatalyst.

中文翻译:

表面空位缺陷对促进硫化锌纳米颗粒光催化稳定性和活性的协同作用

高活性、高稳定性、低成本一直是光催化剂设计开发的追求。在此,使用一种简单的方法整合ZnS (M-ZnS) 表面上丰富的阴离子空位 (V S ) 和阳离子空位 (V Zn ),推导出 V S和 V Zn对(空位对)、孤立的 Zn 原子( Zn iso ) 和孤立的 S 原子 (S iso )。丰富的表面空位缺陷充分暴露和激活表面原子,调节能带结构,显着改善光生载流子的分离。M-ZnS具有高活性,最佳样品的平均产氢速率提高到576.07 μmol·g –1 ·h–1 (λ > 400 nm)。理论模拟表明,活化的 Zn 原子是主要的活性位点,通过与 H 2 O形成 Zn-OH 键。尤其是空位对原子轨道中电子的强相互作用和 V Zn的引入有利于高稳定。最佳样品在 9 次循环后保持 6.59 mmol·g –1 ·h –1(300 W Xe 灯)的平均产氢速率。因此,这项工作加深了对空位缺陷的理解,并为稳定光催化剂的设计提供了思路。
更新日期:2021-11-05
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