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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| Veröffentlicht in: | Environmental science & technology Jg. 57; H. 9; S. 3623 |
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United States
07.03.2023
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| ISSN: | 1520-5851 |
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| Abstract | 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. |
|---|---|
| AbstractList | 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. |
| Author | Yin, Mengxi Zhang, Xiaoyuan Huang, Xia Chen, Shuning Ouyang, Changpei Ren, Tengfei |
| Author_xml | – sequence: 1 givenname: Tengfei surname: Ren fullname: Ren, Tengfei organization: State Key Joint Laboratory of Environment Simulation and Pollution Control, School of Environment, Tsinghua University, Beijing 100084, People's Republic of China – sequence: 2 givenname: Mengxi surname: Yin fullname: Yin, Mengxi organization: State Key Joint Laboratory of Environment Simulation and Pollution Control, School of Environment, Tsinghua University, Beijing 100084, People's Republic of China – sequence: 3 givenname: Shuning surname: Chen fullname: Chen, Shuning organization: State Key Joint Laboratory of Environment Simulation and Pollution Control, School of Environment, Tsinghua University, Beijing 100084, People's Republic of China – sequence: 4 givenname: Changpei surname: Ouyang fullname: Ouyang, Changpei organization: State Key Joint Laboratory of Environment Simulation and Pollution Control, School of Environment, Tsinghua University, Beijing 100084, People's Republic of China – sequence: 5 givenname: Xia orcidid: 0000-0003-4076-1464 surname: Huang fullname: Huang, Xia organization: State Key Joint Laboratory of Environment Simulation and Pollution Control, School of Environment, Tsinghua University, Beijing 100084, People's Republic of China – sequence: 6 givenname: Xiaoyuan orcidid: 0000-0003-3196-3443 surname: Zhang fullname: Zhang, Xiaoyuan organization: State Key Joint Laboratory of Environment Simulation and Pollution Control, School of Environment, Tsinghua University, Beijing 100084, People's Republic of China |
| BackLink | https://www.ncbi.nlm.nih.gov/pubmed/36790324$$D View this record in MEDLINE/PubMed |
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| Keywords | catalytic ozonation Fe-N4 active sites single-atom iron catalysts advanced wastewater treatment nonradical pathway |
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| SubjectTerms | Carbon Catalysis Iron - chemistry Oxalic Acid Oxidation-Reduction Ozone Water Pollutants, Chemical - analysis Water Purification |
| Title | Single-Atom Fe-N 4 Sites for Catalytic Ozonation to Selectively Induce a Nonradical Pathway toward Wastewater Purification |
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