Selective oxidation of organic pollutants based on reactive oxygen species and the molecular structure: Degradation behavior and mechanism analysis

Ming Zhang; Jingqi Ruan; Xinhao Wang; Weizhen Shao; Zhonglin Chen; Zhanghao Chen; Cheng Gu; Weichuan Qiao; Jiansheng Li

doi:10.1016/j.watres.2023.120697

Selective oxidation of organic pollutants based on reactive oxygen species and the molecular structure: Degradation behavior and mechanism analysis

Water Res. 2023 Nov 1:246:120697. doi: 10.1016/j.watres.2023.120697. Epub 2023 Oct 4.

Authors

Ming Zhang¹, Jingqi Ruan², Xinhao Wang³, Weizhen Shao², Zhonglin Chen², Zhanghao Chen⁴, Cheng Gu³, Weichuan Qiao⁵, Jiansheng Li⁶

Affiliations

¹ Department of Environmental Engineering, College of Ecology and the Environment, Nanjing Forestry University, Nanjing 210037, China; Jiangsu Key Laboratory of Chemical Pollution Control and Resources Reuse, School of Environmental and Biological Engineering, Nanjing University of Science and Technology, Nanjing 210094, China; State Key Laboratory of Pollution Control and Resource Reuse, School of the Environment, Nanjing University, Nanjing 210023, China.
² Department of Environmental Engineering, College of Ecology and the Environment, Nanjing Forestry University, Nanjing 210037, China.
³ State Key Laboratory of Pollution Control and Resource Reuse, School of the Environment, Nanjing University, Nanjing 210023, China.
⁴ State Key Laboratory of Pollution Control and Resource Reuse, School of the Environment, Nanjing University, Nanjing 210023, China. Electronic address: zhchen@nju.edu.cn.
⁵ Department of Environmental Engineering, College of Ecology and the Environment, Nanjing Forestry University, Nanjing 210037, China. Electronic address: hgqwc@njfu.edu.cn.
⁶ Jiangsu Key Laboratory of Chemical Pollution Control and Resources Reuse, School of Environmental and Biological Engineering, Nanjing University of Science and Technology, Nanjing 210094, China. Electronic address: lijsh@njust.edu.cn.

PMID: 37837899
DOI: 10.1016/j.watres.2023.120697

Abstract

The selective and rapid elimination of refractory organic pollutants from surface water is significant. However, the relationship of between reactive oxygen species (ROSs) and diversified pollutants molecular structures still needs to be further clarified. Here, we utilize polydopamine (PDA)-assisted coating strategy to prepare hollow 2D carbon nanosheet (ZPL-HCNS) and 2D Co₃O₄ nanosheet (ZPL-Co₃O₄) by thermolysis of PDA coated ZIF-L (ZIF-L@PDA) precursor under different gas atmosphere, which realizes the controlled generation of radicals and non-radicals. Organic pollutants including bisphenols, sulfonamides, quinolones, tetracyclines, and azo dyes are applied to assess the catalytic performance. Results show that dyes containing azo structure are more likely to be degraded by radical process, which is due to that the energy (ΔE) requirements to break the azo bond is higher than energy released from singlet oxygen to oxygen molecule and lower than that of sulfate radical to sulfate. Frontier molecular orbital theory HOMO-LUMO and Fukui function expounded the possible selectivity mechanism. In addition, the degradation pathway and biotoxicity test are carried out. This work provides a reference to illustrate the selective degradation for ROSs and molecular structure of pollutants.

Keywords: Azo structure; Degradation efficiencies; Selective oxidation; Singlet oxygen; Sulfate radical.

MeSH terms

Environmental Pollutants*
Molecular Structure
Oxidation-Reduction
Reactive Oxygen Species
Singlet Oxygen

Substances

Reactive Oxygen Species
Environmental Pollutants
cobalt tetraoxide
Singlet Oxygen