College of Chemical Engineering, China University of Petroleum, Qingdao 266580, China.
College of Chemical Engineering, China University of Petroleum, Qingdao 266580, China; State Key Laboratory of Petroleum Pollution Control, Beijing 102206, China; State Key Laboratory of Heavy Oil Processing, China University of Petroleum, Qingdao 266580, China.
J Environ Sci (China). 2023 Mar;125:244-257. doi: 10.1016/j.jes.2021.12.023. Epub 2022 Jan 3.
High-efficiency photocatalysts are of great significance for the application of photocatalytic technology in water treatment. In this study, N/Cu co-doped ZnS nanosphere photocatalyst (N/Cu-ZnS) is synthesized by a hydrothermal method for the first time. After doping, the texture of nanosphere becomes loose, the nanometer diameter is reduced, making the specific surface area of catalyst increased from 34.73 to 101.59 m/g. The characterization results show that more ZnS (111) crystal planes are exposed by N/Cu co-doping; the calculations of density functional theory show that N/Cu co-doping can increase the catalytic activity of the ZnS (111) crystal plane, enhance the adsorption capacity of (111) crystal plane to O, and promote the generation of •O. The energy levels of the introduced impurities can be hybridized with the energy levels of S and Zn at the top of valence band and the bottom of conduction band, which makes the band gap narrower, thus enhancing the absorption of visible light. Compared with pure ZnS, the degradation rates of 2,4-dichlorophenol (2,4-DCP) and tetracycline (TC) by N/Cu-ZnS under visible light (>420 nm) are increased by 83.7 and 51 times, respectively. In this research, a promising photocatalyst for photocatalytic degradation of organic pollutants in wastewater is provided.
高效光催化剂对于将光催化技术应用于水处理具有重要意义。本研究首次通过水热法合成了 N/Cu 共掺杂的 ZnS 纳米球光催化剂(N/Cu-ZnS)。掺杂后,纳米球的结构变得疏松,纳米直径减小,使催化剂的比表面积从 34.73 增加到 101.59 m/g。表征结果表明,N/Cu 共掺杂可以暴露更多的 ZnS(111)晶面;密度泛函理论计算表明,N/Cu 共掺杂可以提高 ZnS(111)晶面的催化活性,增强(111)晶面对 O 的吸附能力,促进•O 的生成。引入杂质的能级可以与价带顶和导带底的 S 和 Zn 能级杂化,使带隙变窄,从而增强可见光的吸收。与纯 ZnS 相比,N/Cu-ZnS 在可见光(>420nm)下对 2,4-二氯苯酚(2,4-DCP)和四环素(TC)的降解速率分别提高了 83.7 倍和 51 倍。本研究为光催化降解废水中有机污染物提供了一种有前景的光催化剂。