Activation of peroxymonosulfate by single-atom Fe-g-C3N4 catalysts for high efficiency degradation of tetracycline via nonradical pathways: Role of high-valent iron-oxo species and Fe–Nx sites
Activation of peroxymonosulfate by single-atom Fe-g-C3N4 catalysts for high efficiency degradation of tetracycline via nonradical pathways: Role of high-valent iron-oxo species and Fe–Nx sites
复制标题
单原子 Fe-g-C3N4 催化剂活化过一硫酸盐，通过非自由基途径高效降解四环素：高价铁氧物种和 Fe-Nx 位点的作用
DOI：
10.1016/j.cej.2021.130803
复制
发表时间：
2022
影响因子：
15.1
通讯作者：
Fengping Hu
中科院分区：
文献类型：
--
作者：
Xiaoming Peng;Jianqun Wu;Zilong Zhao;Xinyu Wang;Hongling Dai;Li Xu;Gaoping Xu;Yan Jian;Fengping Hu
·采用简便的方法成功地合成了单Fe原子催化剂。·单Fe原子催化剂在反应过程中表现出上级催化性能。实验和密度泛函理论计算表明FeN 4是最佳活性位。·Fe IV = O和1 O2被认为是主要的反应途径。基于孤立的Fe单原子和固定在g-C3 N4骨架上的Fe团簇制备了类Fenton催化剂。在多相活化过一硫酸盐（PMS）降解四环素（TC）中表现出较高的活性和稳定性。实验和密度泛函理论计算结果都表明，具有最佳结合能的单一N配位Fe原子（Fe-N4）是PMS活化的活性中心.实验分析表明，单个Fe原子比Fe原子簇表现出上级的催化活性。此外，高价铁氧物种和单一的氧占主导地位的非自由基过程引起TC降解。其中，锚定在Fe-g-C3 N4上的单个Fe原子作为Fe-N4活性中心，可直接活化PMS生成高价铁氧物种，是TC降解的关键活性非自由基物种。
• Single Fe atom catalyst was successfully synthesized by facile method. • Single Fe atom catalyst showed that superior catalytic performance in reaction process. • Experiment and DFT calculation demonstrated FeN 4 was optimum active site. • The Fe IV = O and 1 O 2 were regarded as the dominated reactive pathway. A Fenton-like catalyst was prepared based on isolated Fe single-atom and Fe clusters anchored onto a g-C 3 N 4 framework. It exhibited high activity and stability in the heterogeneous activation of peroxymonosulfate (PMS) for tetracycline (TC) degradation. Both experimental and density functional theory calculation results demonstrated that the unique N-coordinated single Fe atom (Fe–N 4 ) served as active sites with optimal binding energy for PMS activation. The experimental analysis indicated that the single Fe atoms displayed superior catalytic activity to Fe clusters. Furthermore, both high-valent iron-oxo species and single oxygen-dominated nonradical processes caused TC degradation. Among them, single Fe atoms anchored onto Fe-g-C 3 N 4 served as Fe–N 4 reactive sites can directly activate PMS to produce high-valent iron-oxo species, which was the key active nonradical species causing TC degradation.
登录
查看更多内容
使用还原介孔MnO@MnOx微球显着增强硫酸根基左氧氟沙星的类光芬顿降解
影响因子：
15.1
作者：
Wang Anqi;Chen Zuo;Zheng Zhikeng;Xu Hong;Wang Hui;Hu Kang;Yan Kai
通讯作者：
Yan Kai
影响因子：
19
作者：
Huabin Zhang;Le Yu;Tao Chen;Wei Zhou;X. Lou
通讯作者：
Huabin Zhang;Le Yu;Tao Chen;Wei Zhou;X. Lou
影响因子：
22.1
作者：
Mian, Md Manik;Liu, Guijian;Song, Yu
通讯作者：
Song, Yu
影响因子：
9.5
作者：
Tang, Lian;Huang, Shaodong;Wang, Wei
通讯作者：
Wang, Wei
影响因子：
22.1
作者：
Peng, Lijng;Duan, Xiaoguang;Xu, Xing
通讯作者：
Xu, Xing