Thermodynamic and Kinetic Behaviors of Persulfate-Based Electron-Transfer Regime in Carbocatalysis

A carbon-based advanced oxidation process is featured for the nonradical electron-transfer pathway (ETP) from electron-donating organic compounds to activated persulfate complexes, enabling it as a green technology for the selective oxidation of organic pollutants in complex water environments. Howe...

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Bibliographic Details
Published in:Environmental science & technology 2023-11, Vol.57 (47), p.19012-19022
Main Authors: Peng, Yanhua, Zhang, Qiming, Ren, Wei, Duan, Xiaoguang, Ding, Lin, Jing, Yunpeng, Shao, Penghui, Xiao, Xiao, Luo, Xubiao
Format: Article
Language:English
Subjects:
Adsorption
Carbon
Clean technology
Electron clouds
electron transfer
Electrostatic properties
hydrochemistry
Hydrophobicity
Mass transfer
Organic compounds
Oxidation
Oxidation process
Oxidation rate
Physicochemical properties
Pollutants
Reaction kinetics
sustainable technology
technology
Thermodynamics
wastewater
Water chemistry
Water pollution
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Summary:A carbon-based advanced oxidation process is featured for the nonradical electron-transfer pathway (ETP) from electron-donating organic compounds to activated persulfate complexes, enabling it as a green technology for the selective oxidation of organic pollutants in complex water environments. However, the thermodynamic and kinetic behaviors of the nonradical electron-transfer regime had been ambiguous due to a neglect of the influence of pH on the mechanisms. In this study, three kinds of organic pollutants were divided in the carbon-based ETP regime: (i) physio-adsorption, (ii) adsorption-dominated ETP (oxidation rate slightly surpasses adsorption rate), and (iii) oxidation-dominated ETP (oxidation rate outpaces the adsorption rate). The differential kinetic behaviors were attributed to the physicochemical properties of the organic pollutants. For example, the hydrophobicity, molecular radius, and positive electrostatic potential controlled the mass-transfer process of the adsorption stage of the reactants (peroxydisulfate (PDS) and organics). Meanwhile, other descriptors, including the Fukui index, oxidation potential, and electron cloud density regulated the electron-transfer processes and thus the kinetics of oxidation. Most importantly, the oxidation pathways of these organic pollutants could be altered by adjusting the water chemistry. This study reveals the principles for developing efficient nonradical systems to selectively remove and recycle organic pollutants in wastewater.
ISSN:0013-936X
1520-5851
1520-5851
DOI:10.1021/acs.est.3c02675