Single-Atom Fe-N 4 Sites for Catalytic Ozonation to Selectively Induce a Nonradical Pathway toward Wastewater Purification

Nonradical oxidation has been determined to be a promising pathway for the degradation of organic pollutants in heterogeneous catalytic ozonation (HCO). However, the bottlenecks are the rational design of catalysts to selectively induce nonradicals and the interpretation of detailed nonradical gener...

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Vydáno v:Environmental science & technology Ročník 57; číslo 9; s. 3623
Hlavní autoři: Ren, Tengfei, Yin, Mengxi, Chen, Shuning, Ouyang, Changpei, Huang, Xia, Zhang, Xiaoyuan
Médium: Journal Article
Jazyk:angličtina
Vydáno: United States 07.03.2023
Témata:
Carbon
Catalysis
Iron - chemistry
Oxalic Acid
Oxidation-Reduction
Ozone
Water Pollutants, Chemical - analysis
Water Purification
catalytic ozonation
Fe-N4 active sites
single-atom iron catalysts
advanced wastewater treatment
nonradical pathway
ISSN:1520-5851
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Shrnutí:Nonradical oxidation has been determined to be a promising pathway for the degradation of organic pollutants in heterogeneous catalytic ozonation (HCO). However, the bottlenecks are the rational design of catalysts to selectively induce nonradicals and the interpretation of detailed nonradical generation mechanisms. Herein, we propose a new HCO process based on single-atom iron catalysts, in which Fe-N sites anchored on the carbon skeleton exhibited outstanding catalytic ozonation activity and stability for the degradation of oxalic acid (OA) and -hydroxybenzoic acid (pHBA) as well as the advanced treatment of a landfill leachate secondary effluent. Unlike traditional radical oxidation, nonradical pathways based on surface-adsorbed atomic oxygen (*O ) and singlet oxygen ( O ) were identified. A substrate-dependent behavior was also observed. OA was adsorbed on the catalyst surface and mainly degraded by *O , while pHBA was mostly removed by O and O in the bulk solution. Density functional theory calculations and molecular dynamics simulations revealed that one terminal oxygen atom of ozone preferred bonding with the central iron atom of Fe-N , subsequently inducing the cleavage of the O-O bond near the catalyst surface to produce *O and O . These findings highlight the structural design of an ozone catalyst and an atomic-level understanding of the nonradical HCO process.
ISSN:1520-5851
DOI:10.1021/acs.est.2c07653