Facile low-temperature supercritical carbonization method to prepare high-loading nickel single atom catalysts for efficient photodegradation of tetracycline

作     者：Han Qiao Lirong Zheng Shiwen Hu Gang Tang Hongri Suo Chongxuan Liu Han Qiao;Lirong Zheng;Shiwen Hu;Gang Tang;Hongri Suo;Chongxuan Liu

作者机构：School of EnvironmentHarbin Institute of TechnologyHarbin 150090China State Environmental Protection Key Laboratory of Integrated Surface Water-Groundwater Pollution ControlSchool of Environmental Science and EngineeringSouthern University of Science and TechnologyShenzhen 518055China Beijing Synchrotron Radiation Facility(BSRF)Institute of High Energy PhysicsChinese Academy of SciencesBeijing 100049China 

出 版 物：《Journal of Environmental Sciences》 (环境科学学报（英文版）)

年 卷 期：2024年第138卷第4期

页      面：373-384页

核心收录：

学科分类：083002[工学-环境工程] 0830[工学-环境科学与工程（可授工学、理学、农学学位）] 081705[工学-工业催化] 08[工学] 0817[工学-化学工程与技术] 080502[工学-材料学] 0805[工学-材料科学与工程（可授工学、理学学位）] 

基　　金：supported by the National Key Research and Development Program(No.2019YFC1803903) the Program for Guangdong Introducing Innovative and Entrepreneurial Teams(No.2017ZT07Z479) China Postdoctoral Science Foundation(No.2021M701561) the National Natural Science Foundation of China(No.42007318) 

主　　题：Carbon-based single-atom catalyst Nickel Photocatalytic degradation Tetracycline Visible light 

摘      要：Environmental photocatalysis is a promising technology for treating antibiotics in *** this study,a supercritical carbonization method was developed to synthesize a single-atom photocatalyst with a high loading of Ni(above 5 wt.%)anchored on a carbonnitrogen-silicate substrate for the efficient photodegradation of a ubiquitous environmental contaminant of tetracycline(TC).The photocatalyst was prepared from an easily obtained metal-biopolymer-inorganic supramolecular hydrogel,followed by supercritical drying and carbonization *** low-temperature(300℃)supercritical ethanol treatment prevents the excessive structural degradation of hydrogel and greatly reduces the metal clustering and aggregation,which contributed to the high Ni *** characterizations confirmed that Ni was present at isolated sites and stabilized by Ni-N and Ni-O bonds in a Ni-(N/O)_(6)-C/SiC configuration.A 5%Ni-C-Si catalyst,which performed the best among the studied catalysts,exhibited a wide visible light response with a narrow bandgap of 1.45 eV that could efficiently and repeatedly catalyze the oxidation of TC with a conversion rate of almost 100% within 40 *** reactive species trapping experiments and electron spin resonance(ESR)tests demonstrated that the h+,and·O_(2)-were mainly responsible for TC *** TC degradation mechanism and possible reaction pathways were provided ***,this study proposed a novel strategy to synthesize a high metal loading singleatom photocatalyst that can efficiently remove TC with high concentrations,and this strategy might be extended for synthesis of other carbon-based single-atom catalysts with valuable properties.