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Facile Construction of a Copper-Containing Covalent Bond for Peroxymonosulfate Activation: Efficient Redox Behavior of Copper Species via Electron Transfer Regulation

  • Ting Chen
    Ting Chen
    State Key Laboratory of Pollution Control and Resource Reuse, Tongji University, Shanghai 200092, China
    Shanghai Institute of Pollution Control and Ecological Safety, Shanghai 200092, China
    More by Ting Chen
  • Zhiliang Zhu*
    Zhiliang Zhu
    State Key Laboratory of Pollution Control and Resource Reuse, Tongji University, Shanghai 200092, China
    Key Laboratory of Yangtze River Water Environment, Ministry of Education, Tongji University, Shanghai 200092, China
    Shanghai Institute of Pollution Control and Ecological Safety, Shanghai 200092, China
    *Email: [email protected]
    More by Zhiliang Zhu
  • Hua Zhang
    Hua Zhang
    State Key Laboratory of Pollution Control and Resource Reuse, Tongji University, Shanghai 200092, China
    More by Hua Zhang
  • Yanling Qiu
    Yanling Qiu
    Key Laboratory of Yangtze River Water Environment, Ministry of Education, Tongji University, Shanghai 200092, China
    Shanghai Institute of Pollution Control and Ecological Safety, Shanghai 200092, China
    More by Yanling Qiu
  • Daqiang Yin
    Daqiang Yin
    Key Laboratory of Yangtze River Water Environment, Ministry of Education, Tongji University, Shanghai 200092, China
    Shanghai Institute of Pollution Control and Ecological Safety, Shanghai 200092, China
    More by Daqiang Yin
  • , and 
  • Guohua Zhao*
    Guohua Zhao
    School of Chemical Science and Engineering, Tongji University, Shanghai 200092, China
    *Email: [email protected]
    More by Guohua Zhao
Cite this: ACS Appl. Mater. Interfaces 2020, 12, 38, 42790–42802
Publication Date (Web):August 28, 2020
https://doi.org/10.1021/acsami.0c11268
Copyright © 2020 American Chemical Society
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Abstract

Heterogeneous catalysis can be enhanced through the construction of effective atom connection for rapid electron transport on the catalyst surface. Hence, this study proposed a new strategy for electron transfer regulation to facilitate redox cycle of Cu(II)/Cu(I). The objective was achieved by successful construction of copper-containing covalent bond through the in situ growth of porous g-C3N4 with oxygen dopants and nitrogen defects (O-CND) on CuAlxOy substrate ([email protected]D). On the basis of X-ray absorption fine structure (XAFS) and other characterization results, the facilitated redox behavior of copper species by electron transfer regulation was ascribed to the formation of a C–O–Cu bond on the porous-rich superficial of the catalyst; these covalent C–O–Cu bonds shortened the migration distance of electrons between Cu(II) and Cu(I) via Cu(I)–O–C–O–Cu(II) bridge. The construction of copper-containing covalent bonds in the catalyst resulted in efficient PMS activation for a rapid redox cycle of Cu(II)/Cu(I), triggering a series of reactions involving the continuous production of three highly active species (SO4·, ·OH and 1O2). The rapid diffusion and transportation of the generated active species from porous structures directly attack typical pharmaceutically active compounds (PhACs), achieving superior catalytic performance. This study provides a new routine to construct a C–O–Cu bond for PMS activation by regulating the electron transfer to accelerate the redox behavior of copper species for environmental remediation.

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The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acsami.0c11268.

  • Text S1-S2, including characterization and analytical methods; Table S1, including ESR-measured g value; Figure S1-S14, including structure of pollutants; SEM images of g-C3N4, TEM image of CuAlxO and SEM image of [email protected]; N2 adsorption–desorption isotherms and pore size distribution, Raman spectra, and TGA results of prepared samples; XPS spectra of Al 2p in [email protected] and [email protected]D; equivalent electric circuit (EEC) and fitted admittance Nyquist plots; quenching tests with various scavengers concentrations; adsorption experiments for different samples; effects of catalyst usage and PMS concentration on TAP degradation; and TAP degradation in the dissolved Cu ions solution (PDF)

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Cited By


This article is cited by 13 publications.

  1. Xiaoqian Wan, Dandan Qian, Lunhong Ai, Jing Jiang. Highly Efficient Peroxymonosulfate Activation by Surface Oxidized Nickel Phosphide with Dual Active Sites. Industrial & Engineering Chemistry Research 2020, 59 (51) , 22040-22048. https://doi.org/10.1021/acs.iecr.0c04797
  2. Yujie Bao, Ting Chen, Zhiliang Zhu, Hua Zhang, Yanling Qiu, Daqiang Yin. Mo2C/C catalyst as efficient peroxymonosulfate activator for carbamazepine degradation. Chemosphere 2022, 287 , 132047. https://doi.org/10.1016/j.chemosphere.2021.132047
  3. Shouwei Zhang, Xiaohua Ren, Xizhong Zhou, Huihui Gao, Xiao Wang, Jinzhao Huang, Xijin Xu. Hierarchical multi-active component yolk-shell nanoreactors as highly active peroxymonosulfate activator for ciprofloxacin degradation. Journal of Colloid and Interface Science 2022, 605 , 766-778. https://doi.org/10.1016/j.jcis.2021.07.130
  4. Xinyu Li, Xiaobo Min, Xiaoxian Hu, Zhi Jiang, Chaofang Li, Weichun Yang, Feiping Zhao. In-situ synthesis of highly dispersed Cu-CuxO nanoparticles on porous carbon for the enhanced persulfate activation for phenol degradation. Separation and Purification Technology 2021, 276 , 119260. https://doi.org/10.1016/j.seppur.2021.119260
  5. Ting Chen, Zhiliang Zhu, Hua Zhang, Yanling Qiu, Daqiang Yin. Cu-O-incorporation design for promoted heterogeneous catalysis: synergistic effect of surface adsorption and catalysis towards efficient bisphenol A removal. Applied Surface Science 2021, 569 , 151107. https://doi.org/10.1016/j.apsusc.2021.151107
  6. Yu Wang, Lianhu Fang, Zhen Wang, Qi Yang. Peroxymonosulfate activation by graphitic carbon nitride co-doped with manganese, cobalt, and oxygen for degradation of trichloroethylene: Effect of oxygen precursors, kinetics, and mechanism. Separation and Purification Technology 2021, 278 , 119580. https://doi.org/10.1016/j.seppur.2021.119580
  7. Jian Ye, Dayi Yang, Jiangdong Dai, Chunxiang Li, Yongsheng Yan, Yi Wang. Strongly Coupled Cobalt/Oxygen Co-doped Porous g-C3N4 Heterostructure with Abundant Oxygen Vacancies Modulated the Peroxymonosulfate Activation Pathway. Chemical Engineering Journal 2021, 418 , 133972. https://doi.org/10.1016/j.cej.2021.133972
  8. Lin Xu, Lifen Liu. Piezo-photocatalytic fuel cell with atomic [email protected] on CFC helical electrode has enhanced peroxymonosulfate activation, pollutant degradation and power generation. Applied Catalysis B: Environmental 2021, 659 , 120953. https://doi.org/10.1016/j.apcatb.2021.120953
  9. Hefei Wang, Tian Tian, Dong Wang, Fangdi Xu, Wei Ren. Adsorption of bisphenol A and 2,4-dichlorophenol onto cetylpyridinium chloride-modified pine sawdust: a kinetic and thermodynamic study. Environmental Science and Pollution Research 2021, 136 https://doi.org/10.1007/s11356-021-17157-3
  10. Bayram Hashemzadeh, Hassan Alamgholiloo, Nader Noroozi Pesyan, Esrafil Asgari, Amir Sheikhmohammadi, Jaber Yeganeh, Hassan Hashemzadeh. Degradation of ciprofloxacin using hematite/MOF nanocomposite as a heterogeneous Fenton-like catalyst: A comparison of composite and core−shell structures. Chemosphere 2021, 281 , 130970. https://doi.org/10.1016/j.chemosphere.2021.130970
  11. Ting Chen, Zhiliang Zhu, Yujie Bao, Hua Zhang, Yanling Qiu, Daqiang Yin. Promoted peroxymonosulfate activation by electron transport channel construction for rapid Cu( ii )/Cu( i ) redox couple circulation. Environmental Science: Nano 2021, 8 (9) , 2618-2628. https://doi.org/10.1039/D1EN00426C
  12. Bofan Zhang, Mutian Zhang, Liang Zhang, Paul A. Bingham, Manabu Tanaka, Wen Li, Shiro Kubuki. BiOBr/MoS2 catalyst as heterogenous peroxymonosulfate activator toward organic pollutant removal: Energy band alignment and mechanism insight. Journal of Colloid and Interface Science 2021, 594 , 635-649. https://doi.org/10.1016/j.jcis.2021.03.066
  13. Zhiwei Yang, Xiaonan Tan, Daojian Tang, Jing Li, Jiahai Ma. A tale of two metal ions: contrasting behaviors of high oxidation states of Cu and Mn in a bicarbonate–H 2 O 2 system. Environmental Science: Water Research & Technology 2021, 7 (3) , 479-486. https://doi.org/10.1039/D0EW00910E