Effects of Molecular Structure on Organic Contaminants' Degradation Efficiency and Dominant ROS in the Advanced Oxidation Process with Multiple ROS
In this study, the previously overlooked effects of contaminants' molecular structure on their degradation efficiencies and dominant reactive oxygen species (ROS) in advanced oxidation processes (AOPs) are investigated with a peroxymonosulfate (PMS) activation system selected as the typical AOP...
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| Vydané v: | Environmental science & technology Ročník 56; číslo 12; s. 8784 |
|---|---|
| Hlavní autori: | , , , , , , , , |
| Médium: | Journal Article |
| Jazyk: | English |
| Vydavateľské údaje: |
United States
21.06.2022
|
| Predmet: | |
| ISSN: | 1520-5851, 1520-5851 |
| On-line prístup: | Zistit podrobnosti o prístupe |
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| Abstract | In this study, the previously overlooked effects of contaminants' molecular structure on their degradation efficiencies and dominant reactive oxygen species (ROS) in advanced oxidation processes (AOPs) are investigated with a peroxymonosulfate (PMS) activation system selected as the typical AOP system. Averagely, degradation efficiencies of 19 contaminants are discrepant in the CoCaAl-LDO/PMS system with production of SO
,
OH, and
O
. Density functional theory calculations indicated that compounds with high
, low-energy gap (Δ
=
-
), and low vertical ionization potential are more vulnerable to be attacked. Further analysis disclosed that the dominant ROS was the same one when treating similar types of contaminants, namely SO
,
O
,
O
, and
OH for the degradation of CBZ-like compounds, SAs, bisphenol, and triazine compounds, respectively. This phenomenon may be caused by the contaminants' structures especially the commonly shared or basic parent structures which can affect their effective reaction time and second-order rate constants with ROS, thus influencing the contribution of each ROS during its degradation. Overall, the new insights gained in this study provide a basis for designing more effective AOPs to improve their practical application in wastewater treatment. |
|---|---|
| AbstractList | In this study, the previously overlooked effects of contaminants' molecular structure on their degradation efficiencies and dominant reactive oxygen species (ROS) in advanced oxidation processes (AOPs) are investigated with a peroxymonosulfate (PMS) activation system selected as the typical AOP system. Averagely, degradation efficiencies of 19 contaminants are discrepant in the CoCaAl-LDO/PMS system with production of SO4•-, •OH, and 1O2. Density functional theory calculations indicated that compounds with high EHOMO, low-energy gap (ΔE = ELUMO - EHOMO), and low vertical ionization potential are more vulnerable to be attacked. Further analysis disclosed that the dominant ROS was the same one when treating similar types of contaminants, namely SO4•-, 1O2, 1O2, and •OH for the degradation of CBZ-like compounds, SAs, bisphenol, and triazine compounds, respectively. This phenomenon may be caused by the contaminants' structures especially the commonly shared or basic parent structures which can affect their effective reaction time and second-order rate constants with ROS, thus influencing the contribution of each ROS during its degradation. Overall, the new insights gained in this study provide a basis for designing more effective AOPs to improve their practical application in wastewater treatment.In this study, the previously overlooked effects of contaminants' molecular structure on their degradation efficiencies and dominant reactive oxygen species (ROS) in advanced oxidation processes (AOPs) are investigated with a peroxymonosulfate (PMS) activation system selected as the typical AOP system. Averagely, degradation efficiencies of 19 contaminants are discrepant in the CoCaAl-LDO/PMS system with production of SO4•-, •OH, and 1O2. Density functional theory calculations indicated that compounds with high EHOMO, low-energy gap (ΔE = ELUMO - EHOMO), and low vertical ionization potential are more vulnerable to be attacked. Further analysis disclosed that the dominant ROS was the same one when treating similar types of contaminants, namely SO4•-, 1O2, 1O2, and •OH for the degradation of CBZ-like compounds, SAs, bisphenol, and triazine compounds, respectively. This phenomenon may be caused by the contaminants' structures especially the commonly shared or basic parent structures which can affect their effective reaction time and second-order rate constants with ROS, thus influencing the contribution of each ROS during its degradation. Overall, the new insights gained in this study provide a basis for designing more effective AOPs to improve their practical application in wastewater treatment. In this study, the previously overlooked effects of contaminants' molecular structure on their degradation efficiencies and dominant reactive oxygen species (ROS) in advanced oxidation processes (AOPs) are investigated with a peroxymonosulfate (PMS) activation system selected as the typical AOP system. Averagely, degradation efficiencies of 19 contaminants are discrepant in the CoCaAl-LDO/PMS system with production of SO , OH, and O . Density functional theory calculations indicated that compounds with high , low-energy gap (Δ = - ), and low vertical ionization potential are more vulnerable to be attacked. Further analysis disclosed that the dominant ROS was the same one when treating similar types of contaminants, namely SO , O , O , and OH for the degradation of CBZ-like compounds, SAs, bisphenol, and triazine compounds, respectively. This phenomenon may be caused by the contaminants' structures especially the commonly shared or basic parent structures which can affect their effective reaction time and second-order rate constants with ROS, thus influencing the contribution of each ROS during its degradation. Overall, the new insights gained in this study provide a basis for designing more effective AOPs to improve their practical application in wastewater treatment. |
| Author | Li, Ling-Li Xie, Zhi-Hui Zhou, Hong-Yu Mu, Yang Liu, Yang He, Chuan-Shu Liu, Wen Lai, Bo Du, Ye |
| Author_xml | – sequence: 1 givenname: Zhi-Hui orcidid: 0000-0003-4699-5093 surname: Xie fullname: Xie, Zhi-Hui organization: Sino-German Centre for Water and Health Research, Sichuan University, Chengdu 610065, China – sequence: 2 givenname: Chuan-Shu orcidid: 0000-0002-7805-0142 surname: He fullname: He, Chuan-Shu organization: Sino-German Centre for Water and Health Research, Sichuan University, Chengdu 610065, China – sequence: 3 givenname: Hong-Yu surname: Zhou fullname: Zhou, Hong-Yu organization: Sino-German Centre for Water and Health Research, Sichuan University, Chengdu 610065, China – sequence: 4 givenname: Ling-Li surname: Li fullname: Li, Ling-Li organization: Sino-German Centre for Water and Health Research, Sichuan University, Chengdu 610065, China – sequence: 5 givenname: Yang surname: Liu fullname: Liu, Yang organization: Sino-German Centre for Water and Health Research, Sichuan University, Chengdu 610065, China – sequence: 6 givenname: Ye orcidid: 0000-0001-8099-0996 surname: Du fullname: Du, Ye organization: Sino-German Centre for Water and Health Research, Sichuan University, Chengdu 610065, China – sequence: 7 givenname: Wen orcidid: 0000-0002-6787-2431 surname: Liu fullname: Liu, Wen organization: College of Environmental Sciences and Engineering, Peking University, Beijing 100871, China – sequence: 8 givenname: Yang orcidid: 0000-0001-7338-7398 surname: Mu fullname: Mu, Yang organization: CAS Key Laboratory of Urban Pollutant Conversion, Department of Environmental Science and Engineering, University of Science and Technology of China, Hefei 230026, China – sequence: 9 givenname: Bo orcidid: 0000-0002-7105-1345 surname: Lai fullname: Lai, Bo organization: Sino-German Centre for Water and Health Research, Sichuan University, Chengdu 610065, China |
| BackLink | https://www.ncbi.nlm.nih.gov/pubmed/35584301$$D View this record in MEDLINE/PubMed |
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