College of Chemical Engineering, China University of Petroleum, Qingdao, 266580, China.
State Key Laboratory of Pollution Control and Treatment in Petroleum and Petrochemical Industry, State Key Laboratory of Heavy Oil Processing, Beijing, China.
Environ Sci Pollut Res Int. 2022 Aug;29(39):58716-58729. doi: 10.1007/s11356-022-19852-1. Epub 2022 Apr 2.
In order to improve the visible light response, N-doping ZnS (N-ZnS) nanospheres with Zn vacancy and porous surface were prepared by a simple one-pot hydrothermal method. Characterizations and density functional theory simulations showed excellent visible light response of N-ZnS. N-doping introduced impurity energy levels, which led to orbital hybridization and changed the original dipole moment. The presence of ortho Zn vacancy (O-Zn) can effectively reduce e-h recombination and photocorrosion. Furthermore, O-Zn caused lattice distortion (twisted the -S-Zn-N-(O-Zn)-S-Zn-S- chemical bond chain), resulting in "vacancy effect" to accelerate e flow. Under visible light, the photocatalytic degradation efficiency of tetracycline (TC) and 2,4-dichlorophenol (2,4-DCP) was 90.31% and 60.84%, respectively. TOC degradation efficiency was 31.4% and 25.6%, respectively. Combined with Fukui index and LC-MS methods, it was found that TC and 2,4-DCP were degraded under the constant attack of active substances such as ·OH. This work can provide a reference for the application of catalytic materials in the field of visible light photocatalysis.
为了提高可见光响应，采用简单的一步水热法制备了具有锌空位和多孔表面的 N 掺杂 ZnS（N-ZnS）纳米球。表征和密度泛函理论模拟表明 N-ZnS 具有优异的可见光响应。N 掺杂引入了杂质能级，导致轨道杂化并改变了原始偶极矩。正交 Zn 空位（O-Zn）的存在可以有效减少电子-空穴复合和光腐蚀。此外，O-Zn 引起晶格畸变（扭曲了-S-Zn-N-(O-Zn)-S-Zn-S-化学键链），从而产生“空位效应”以加速电子流动。在可见光下，四环素（TC）和 2,4-二氯苯酚（2,4-DCP）的光催化降解效率分别为 90.31%和 60.84%。TOC 降解效率分别为 31.4%和 25.6%。结合福井指数和 LC-MS 方法，发现 TC 和 2,4-DCP 在·OH 等活性物质的持续攻击下被降解。这项工作可为催化材料在可见光光催化领域的应用提供参考。
