State Key Laboratory of Fine Chemicals, Key Laboratory of Industrial Ecology and Environmental Engineering (MOE), School of Environmental Science and Technology, Dalian University of Technology, Dalian 116024, China.
Department of Chemical Engineering, Curtin University, GPO Box U1987, Perth, WA 6845, Australia.
Langmuir. 2020 Aug 25;36(33):9709-9718. doi: 10.1021/acs.langmuir.0c01072. Epub 2020 Aug 13.
A single semiconductor employed into photo(electro)catalysis is not sufficient for charge carrier separation. Designing a multiple heterojunction system is a practical method for photo(electro)catalysis. Herein, novel two-dimensional AgInS/SnS/RGO (AISR) photocatalysts with multiple junctions were prepared by a simple hydrothermal method. The synthesized AISR heterojunctions showed superior photoelectrochemical performance and photocatalytic degradation of norfloxacin, with a high degradation rate reaching 95%. More importantly, the toxicity of photocatalytic products decreased within the reaction process. High spatial separation efficiency of photogenerated electron-hole pairs was evidenced by optical and photoelectrochemical characterizations. Furthermore, a laser flash photolysis technique was carried on investigating the lifetime of the charge carrier of the fabricated dual heterostructures. In addition, sulfur and oxygen vacancies existed in AISR heterojunctions could largely constrain the recombination of electron-hole pairs. Density functional theory calculations were carried out to analyze the mechanism of photoinduced interfacial redox reactions, showing that reduced graphene oxide and AgInS act as electron and hole trappers in the photocatalytic reaction, respectively. Due to the interfacial electric field formed from AISR dual heterojunctions, the effective spatial charge separation and transfer contributed to the boosting photo(electro)catalytic performance.
单一的半导体用于光电催化时,电荷载流子的分离是不够的。设计一个多异质结系统是光电催化的一种实用方法。本文通过简单的水热法制备了具有多个结的新型二维 AgInS/SnS/RGO(AISR)光催化剂。所合成的 AISR 异质结表现出优异的光电化学性能和诺氟沙星的光催化降解性能,降解率高达 95%。更重要的是,光催化产物的毒性在反应过程中降低。光生载流子的高空间分离效率通过光学和光电化学特性得到了证明。此外,采用激光闪光光解技术研究了所制备的双异质结构的载流子寿命。此外,AISR 异质结中存在的硫和氧空位可以极大地抑制电子-空穴对的复合。通过密度泛函理论计算分析了光致界面氧化还原反应的机理,表明还原氧化石墨烯和 AgInS 在光催化反应中分别作为电子和空穴捕获剂。由于 AISR 双异质结形成的界面电场,有效的空间电荷分离和转移有助于提高光电催化性能。