Activation of H2O2 using a single-atom Cu catalyst for efficient tetracycline degradation

被引:3
作者
Bi, Qiang [1 ]
Zhao, Yilin [1 ]
Yang, Bo [1 ]
Du, Yue [1 ]
Xue, Ying [1 ]
Zhang, Kun [1 ]
Xue, Juanqin [1 ]
机构
[1] Xian Univ Architecture & Technol, Sch Chem & Chem Engn, Xian 710055, Peoples R China
基金
中国国家自然科学基金;
关键词
Single-atom Cu catalyst; Tetracycline degradation; Fenton-like; Hydroxyl radical; RATIONAL DESIGN; ELECTRO-FENTON; CARBON; GENERATION; SITES; DYES;
D O I
10.1016/j.apsusc.2024.160943
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
The abuse of antibiotics has caused serious harm to the ecological environment and human health. Fenton-like advanced oxidation technology is a green and effective treatment means, but how to improve the Fenton reaction efficiency and wide pH adaptability is still a big challenge. Herein, we designed and developed a single-atom catalyst Cu-1-CN with graphite-phase carbon nitride as the carrier by loading a low amount of metal Cu. The N atom anchors the copper atom in the form of a coordination bond, and the single atom Cu site has excellent performance in activating H2O2. Not only a short period of time (10 min) oxidation degradation of tetracycline (degradation rate 80 %), and in a broad range of pH (3.2 similar to 9.5) still maintaining high removal performance (efficiency more than 70 %). Combined with X-ray absorption fine structure characterization and density functional theory (DFT) calculations, it is considered that isolated Cu atom and N atom cooperate to construct highly reactive Cu-N-4 active centre, which completes the task of H2O2 activation. This study provides a new theoretical basis and technical support for the degradation of antibiotic pollutants by single-atom Fenton-like reaction.
引用
收藏
页数:8
相关论文
共 34 条
[1]   THE ORIGINS OF PARTICLE-SIZE EFFECTS IN HETEROGENEOUS CATALYSIS [J].
BOND, GC .
SURFACE SCIENCE, 1985, 156 (JUN) :966-981
[2]   Atomic-Level Insight into Optimizing the Hydrogen Evolution Pathway over a Co1-N4 Single-Site Photocatalyst [J].
Cao, Yuanjie ;
Chen, Si ;
Luo, Qiquan ;
Yan, Huan ;
Lin, Yue ;
Liu, Wei ;
Cao, Linlin ;
Lu, Junling ;
Yang, Jinlong ;
Yao, Tao ;
Wei, Shiqiang .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2017, 56 (40) :12191-12196
[3]   Rational Design of Single Molybdenum Atoms Anchored on N-Doped Carbon for Effective Hydrogen Evolution Reaction [J].
Chen, Wenxing ;
Pei, Jiajing ;
He, Chun-Ting ;
Wan, Jiawei ;
Ren, Hanlin ;
Zhu, Youqi ;
Wang, Yu ;
Dong, Juncai ;
Tian, Shubo ;
Cheong, Weng-Chon ;
Lu, Siqi ;
Zheng, Lirong ;
Zheng, Xusheng ;
Yan, Wensheng ;
Zhuang, Zhongbin ;
Chen, Chen ;
Peng, Qing ;
Wang, Dingsheng ;
Li, Yadong .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2017, 56 (50) :16086-16090
[4]   Clays and oxide minerals as catalysts and nanocatalysts in Fenton-like reactions - A review [J].
Garrido-Ramirez, E. G. ;
Theng, B. K. G. ;
Mora, M. L. .
APPLIED CLAY SCIENCE, 2010, 47 (3-4) :182-192
[5]   Modulating the oxidative active species by regulating the valence of palladium cocatalyst in photocatalytic degradation of ciprofloxacin [J].
Guo, Fa ;
Zhang, Hao ;
Li, Hui ;
Shen, Zhurui .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2022, 306
[6]   A single-atom library for guided monometallic and concentration-complex multimetallic designs [J].
Han, Lili ;
Cheng, Hao ;
Liu, Wei ;
Li, Haoqiang ;
Ou, Pengfei ;
Lin, Ruoqian ;
Wang, Hsiao-Tsu ;
Pao, Chih-Wen ;
Head, Ashley R. ;
Wang, Chia-Hsin ;
Tong, Xiao ;
Sun, Cheng-Jun ;
Pong, Way-Faung ;
Luo, Jun ;
Zheng, Jin-Cheng ;
Xin, Huolin L. .
NATURE MATERIALS, 2022, 21 (06) :681-+
[7]  
Hou Linmeng, 2022, Huanjing Huaxue-Environmental Chemistry, V41, P1843, DOI 10.7524/j.issn.0254-6108.2021030301
[8]   Duet Fe3C and FeNx Sites for H2O2 Generation and Activation toward Enhanced Electro-Fenton Performance in Wastewater Treatment [J].
Hu, Jingjing ;
Wang, Sen ;
Yu, Jiaqi ;
Nie, Wenkai ;
Sun, Jie ;
Wang, Shaobin .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2021, 55 (02) :1260-1269
[9]   Rates of hydroxyl radical generation and organic compound oxidation in mineral-catalyzed Fenton-like systems [J].
Kwan, WP ;
Voelker, BM .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2003, 37 (06) :1150-1158
[10]   Boosting oxygen reduction catalysis with abundant copper single atom active sites [J].
Li, Feng ;
Han, Gao-Feng ;
Noh, Hyuk-Jun ;
Kim, Seok-Jin ;
Lu, Yalin ;
Jeong, Hu Young ;
Fu, Zhengping ;
Baek, Jong-Beom .
ENERGY & ENVIRONMENTAL SCIENCE, 2018, 11 (08) :2263-2269