Selective degradation of organic micropollutants by activation of peroxymonosulfate by Se@NC: Role of Se doping and nonradical pathway mechanism
In this study, Se@NC-x decorated with Se was successfully prepared via two-step calcination with zeolitic imidazole framework (ZIF) as a precursor. Mechanistic studies show that PMS would be adsorbed onto the surface of Se@NC-900 to form an active complex (Se@NC-900/PMS*), and the active Se@NC-900/P...
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| Published in | Journal of hazardous materials Vol. 452; p. 131202 |
|---|---|
| Main Authors | , , , , , , , , |
| Format | Journal Article |
| Language | English |
| Published |
Netherlands
Elsevier B.V
15.06.2023
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| Subjects | |
| Online Access | Get full text |
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| Abstract | In this study, Se@NC-x decorated with Se was successfully prepared via two-step calcination with zeolitic imidazole framework (ZIF) as a precursor. Mechanistic studies show that PMS would be adsorbed onto the surface of Se@NC-900 to form an active complex (Se@NC-900/PMS*), and the active Se@NC-900/PMS* could oxidize phenol by the rapid decomposition of PMS. Specifically, electrons are extracted by Se@NC-900/PMS* and then transferred to the surface of Se@NC-900, which can trigger the degradation of phenol. Notably, it is found that the local charge redistribution caused by the doping of Se can activate the catalytic potential of the intrinsically inert carbon skeleton through density flooding theory (DFT) calculations. The XLogP, ΔE, VIP, and ELUMO (Se@NC/PMS)-HOMO (pollutants) and degradation rate constants of different micropollutants were correlated well linearly. This indicates that the Se@NC-900/PMS system has a great selectivity for the degradation of pollutants. Overall, these findings not only illustrate the role of Se in tuning the electronic structure of Se@NC-x to enhance the activation of PMS, but also bridge the gap in our knowledge about the physicochemical properties and degradation performance of Se@NC catalysts.
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•Se@NC-x was used as catalysts to activate the PMS for micropollutants degradation.•Se@NC-x shows its universality and stability in the PMS-based oxidation process.•The Se@NC-x /PMS system catalytic mechanisms were elucidated.•The relation of parameters and degradation rate constants are correlated linearly. |
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| AbstractList | In this study, Se@NC-x decorated with Se was successfully prepared via two-step calcination with zeolitic imidazole framework (ZIF) as a precursor. Mechanistic studies show that PMS would be adsorbed onto the surface of Se@NC-900 to form an active complex (Se@NC-900/PMS*), and the active Se@NC-900/PMS* could oxidize phenol by the rapid decomposition of PMS. Specifically, electrons are extracted by Se@NC-900/PMS* and then transferred to the surface of Se@NC-900, which can trigger the degradation of phenol. Notably, it is found that the local charge redistribution caused by the doping of Se can activate the catalytic potential of the intrinsically inert carbon skeleton through density flooding theory (DFT) calculations. The XLogP, ΔE, VIP, and ELUMO (Se@NC/PMS)-HOMO (pollutants) and degradation rate constants of different micropollutants were correlated well linearly. This indicates that the Se@NC-900/PMS system has a great selectivity for the degradation of pollutants. Overall, these findings not only illustrate the role of Se in tuning the electronic structure of Se@NC-x to enhance the activation of PMS, but also bridge the gap in our knowledge about the physicochemical properties and degradation performance of Se@NC catalysts.
[Display omitted]
•Se@NC-x was used as catalysts to activate the PMS for micropollutants degradation.•Se@NC-x shows its universality and stability in the PMS-based oxidation process.•The Se@NC-x /PMS system catalytic mechanisms were elucidated.•The relation of parameters and degradation rate constants are correlated linearly. In this study, Se@NC-x decorated with Se was successfully prepared via two-step calcination with zeolitic imidazole framework (ZIF) as a precursor. Mechanistic studies show that PMS would be adsorbed onto the surface of Se@NC-900 to form an active complex (Se@NC-900/PMS*), and the active Se@NC-900/PMS* could oxidize phenol by the rapid decomposition of PMS. Specifically, electrons are extracted by Se@NC-900/PMS* and then transferred to the surface of Se@NC-900, which can trigger the degradation of phenol. Notably, it is found that the local charge redistribution caused by the doping of Se can activate the catalytic potential of the intrinsically inert carbon skeleton through density flooding theory (DFT) calculations. The XLogP, ΔE, VIP, and E and degradation rate constants of different micropollutants were correlated well linearly. This indicates that the Se@NC-900/PMS system has a great selectivity for the degradation of pollutants. Overall, these findings not only illustrate the role of Se in tuning the electronic structure of Se@NC-x to enhance the activation of PMS, but also bridge the gap in our knowledge about the physicochemical properties and degradation performance of Se@NC catalysts. In this study, Se@NC-x decorated with Se was successfully prepared via two-step calcination with zeolitic imidazole framework (ZIF) as a precursor. Mechanistic studies show that PMS would be adsorbed onto the surface of Se@NC-900 to form an active complex (Se@NC-900/PMS*), and the active Se@NC-900/PMS* could oxidize phenol by the rapid decomposition of PMS. Specifically, electrons are extracted by Se@NC-900/PMS* and then transferred to the surface of Se@NC-900, which can trigger the degradation of phenol. Notably, it is found that the local charge redistribution caused by the doping of Se can activate the catalytic potential of the intrinsically inert carbon skeleton through density flooding theory (DFT) calculations. The XLogP, ΔE, VIP, and ELUMO (Se@NC/PMS)-HOMO (pollutants) and degradation rate constants of different micropollutants were correlated well linearly. This indicates that the Se@NC-900/PMS system has a great selectivity for the degradation of pollutants. Overall, these findings not only illustrate the role of Se in tuning the electronic structure of Se@NC-x to enhance the activation of PMS, but also bridge the gap in our knowledge about the physicochemical properties and degradation performance of Se@NC catalysts.In this study, Se@NC-x decorated with Se was successfully prepared via two-step calcination with zeolitic imidazole framework (ZIF) as a precursor. Mechanistic studies show that PMS would be adsorbed onto the surface of Se@NC-900 to form an active complex (Se@NC-900/PMS*), and the active Se@NC-900/PMS* could oxidize phenol by the rapid decomposition of PMS. Specifically, electrons are extracted by Se@NC-900/PMS* and then transferred to the surface of Se@NC-900, which can trigger the degradation of phenol. Notably, it is found that the local charge redistribution caused by the doping of Se can activate the catalytic potential of the intrinsically inert carbon skeleton through density flooding theory (DFT) calculations. The XLogP, ΔE, VIP, and ELUMO (Se@NC/PMS)-HOMO (pollutants) and degradation rate constants of different micropollutants were correlated well linearly. This indicates that the Se@NC-900/PMS system has a great selectivity for the degradation of pollutants. Overall, these findings not only illustrate the role of Se in tuning the electronic structure of Se@NC-x to enhance the activation of PMS, but also bridge the gap in our knowledge about the physicochemical properties and degradation performance of Se@NC catalysts. In this study, Se@NC-x decorated with Se was successfully prepared via two-step calcination with zeolitic imidazole framework (ZIF) as a precursor. Mechanistic studies show that PMS would be adsorbed onto the surface of Se@NC-900 to form an active complex (Se@NC-900/PMS*), and the active Se@NC-900/PMS* could oxidize phenol by the rapid decomposition of PMS. Specifically, electrons are extracted by Se@NC-900/PMS* and then transferred to the surface of Se@NC-900, which can trigger the degradation of phenol. Notably, it is found that the local charge redistribution caused by the doping of Se can activate the catalytic potential of the intrinsically inert carbon skeleton through density flooding theory (DFT) calculations. The XLogP, ΔE, VIP, and ELUMO ₍Sₑ@NC/PMS₎₋HOMO ₍ₚₒₗₗᵤₜₐₙₜₛ₎ and degradation rate constants of different micropollutants were correlated well linearly. This indicates that the Se@NC-900/PMS system has a great selectivity for the degradation of pollutants. Overall, these findings not only illustrate the role of Se in tuning the electronic structure of Se@NC-x to enhance the activation of PMS, but also bridge the gap in our knowledge about the physicochemical properties and degradation performance of Se@NC catalysts. |
| ArticleNumber | 131202 |
| Author | Zhan, Peng Peng, Xiaoming Dai, Hongling Xu, Xing Chai, Yandong Hu, Fengping Liu, Zhaochen Huang, Zhen Tan, Chaoqun |
| Author_xml | – sequence: 1 givenname: Yandong surname: Chai fullname: Chai, Yandong organization: School of Civil Engineering and Architecture, East China Jiaotong University, Nanchang 330013, PR China – sequence: 2 givenname: Hongling surname: Dai fullname: Dai, Hongling organization: School of Civil Engineering and Architecture, East China Jiaotong University, Nanchang 330013, PR China – sequence: 3 givenname: Peng surname: Zhan fullname: Zhan, Peng organization: Jiangxi Water Resources Institute, Nanchang 330013, PR China – sequence: 4 givenname: Zhaochen surname: Liu fullname: Liu, Zhaochen organization: School of Civil Engineering and Architecture, East China Jiaotong University, Nanchang 330013, PR China – sequence: 5 givenname: Zhen surname: Huang fullname: Huang, Zhen organization: School of Civil Engineering and Architecture, East China Jiaotong University, Nanchang 330013, PR China – sequence: 6 givenname: Chaoqun surname: Tan fullname: Tan, Chaoqun organization: Department of Municipal Engineering, Southeast University, Nanjing 210000, PR China – sequence: 7 givenname: Fengping surname: Hu fullname: Hu, Fengping organization: School of Civil Engineering and Architecture, East China Jiaotong University, Nanchang 330013, PR China – sequence: 8 givenname: Xing surname: Xu fullname: Xu, Xing organization: Shandong Key Laboratory of Water Pollution Control and Resource Reuse, School of Environmental Science and Engineering, Shandong University, Qingdao 266237, PR China – sequence: 9 givenname: Xiaoming surname: Peng fullname: Peng, Xiaoming email: pengxiaoming70@ecjtu.edu.cn organization: School of Civil Engineering and Architecture, East China Jiaotong University, Nanchang 330013, PR China |
| BackLink | https://www.ncbi.nlm.nih.gov/pubmed/36934627$$D View this record in MEDLINE/PubMed |
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| Keywords | Open-circuit potential Se Electronic structure Degradation performance |
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| SubjectTerms | carbon Degradation performance Electronic structure imidazole Open-circuit potential phenol pollutants |
| Title | Selective degradation of organic micropollutants by activation of peroxymonosulfate by Se@NC: Role of Se doping and nonradical pathway mechanism |
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