Degradation of Diclofenac by Bisulfite Coupled with Iron and Manganous Ions: Dual Mechanism, DFT-Assisted Pathway Studies, and Toxicity Assessment
Diclofenac (DCF) is often detected in diverse aquatic bodies, and ineffective management can lead to detrimental effects on human health and ecosystems. In this study, degradation of DCF by Fe(III) and Mn(II) activating bisulfite (BS) was investigated. In the Fe(III)/Mn(II)/BS system, 93.4% DCF was...
Gespeichert in:
Veröffentlicht in: | Water (Basel) 2024-07, Vol.16 (14), p.1994 |
---|---|
Hauptverfasser: | , , , , , |
Format: | Artikel |
Sprache: | eng |
Schlagworte: | |
Online-Zugang: | Volltext |
Tags: |
Tag hinzufügen
Keine Tags, Fügen Sie den ersten Tag hinzu!
|
container_end_page | |
---|---|
container_issue | 14 |
container_start_page | 1994 |
container_title | Water (Basel) |
container_volume | 16 |
creator | Wang, Hongbin Kuang, Shijie Su, Youlun Ren, Xu Yang, Bowen Sun, Yongliang |
description | Diclofenac (DCF) is often detected in diverse aquatic bodies, and ineffective management can lead to detrimental effects on human health and ecosystems. In this study, degradation of DCF by Fe(III) and Mn(II) activating bisulfite (BS) was investigated. In the Fe(III)/Mn(II)/BS system, 93.4% DCF was degraded at 200 μM BS within 120 s, and additional research on 1000 μM BS achieved 88.4% degradation efficacy. Moreover, kinetics fitting of DCF degradation with the different BS concentrations was studied to find the two highest reaction rates (200 and 1000 μM, kobs = 0.0297 and 0.0317 s−1, respectively). Whereafter, SO4•− and Mn(III) were identified as the main active species at these two concentrations, respectively. Density functional theory (DFT) calculations, molecular frontier orbital theory, and surface electrostatic potential (ESP) forecast electrophilic attack sites. DCF degradation pathways by radical and non-radical ways were proposed by attack site prediction and thirteen intermediates identified by UPLC-QTOF-MS. ECOSAR software 2.2 was used for toxicity assessment. This work studied DCF degradation by the Fe(III)/Mn(II)/BS process in the presence of different concentrations of BS, providing a new insight into water purification. |
doi_str_mv | 10.3390/w16141994 |
format | Article |
fullrecord | <record><control><sourceid>gale_proqu</sourceid><recordid>TN_cdi_proquest_miscellaneous_3153739968</recordid><sourceformat>XML</sourceformat><sourcesystem>PC</sourcesystem><galeid>A803779261</galeid><sourcerecordid>A803779261</sourcerecordid><originalsourceid>FETCH-LOGICAL-c282t-f64eb2ad5f1b42fd4fdecfceda9eb5027b24e13feaf84b84ca338a390bca2ec33</originalsourceid><addsrcrecordid>eNptkd1u1DAQhSMEElXpBW9giRuQmhL_ZONwt-zSdqVWILFcWxN7vOsqsZfY0XZfgyfGbREtqJ4LW6PvHI3PFMVbWp1x3lYf93RGBW1b8aI4YlXDSyEEffnk_bo4ifGmyke0UtbVUfFriZsRDCQXPAmWLJ3ug0UPmnQH8tnFqbcuIVmEadejIXuXtmQ1Zhi8IdfgN-DDFMkq-PiJLCfoyTXqLXgXh1OyPF-X8xhdTFn6DdJ2DwfyPU3GYTy9d1iHW6ddOpCMYYwD-vSmeGWhj3jy5z4ufpx_WS8uy6uvF6vF_KrUTLJU2pnAjoGpLe0Es0ZYg9pqNNBiV1es6ZhAyi2ClaKTQgPnEnJMnQaGmvPj4v2D724MPyeMSQ0uaux78Ji_pDitecPbdiYz-u4_9CZMo8_TKV7lHCUVNX-kNtCjct6GNIK-M1VzWfGmadmMZursGSqXwcHp4NG63P9H8OFBoMcQ44hW7UY3wHhQtFJ3e1d_985_A2rcn9Q</addsrcrecordid><sourcetype>Aggregation Database</sourcetype><iscdi>true</iscdi><recordtype>article</recordtype><pqid>3085081453</pqid></control><display><type>article</type><title>Degradation of Diclofenac by Bisulfite Coupled with Iron and Manganous Ions: Dual Mechanism, DFT-Assisted Pathway Studies, and Toxicity Assessment</title><source>MDPI - Multidisciplinary Digital Publishing Institute</source><source>Elektronische Zeitschriftenbibliothek - Frei zugängliche E-Journals</source><creator>Wang, Hongbin ; Kuang, Shijie ; Su, Youlun ; Ren, Xu ; Yang, Bowen ; Sun, Yongliang</creator><creatorcontrib>Wang, Hongbin ; Kuang, Shijie ; Su, Youlun ; Ren, Xu ; Yang, Bowen ; Sun, Yongliang</creatorcontrib><description>Diclofenac (DCF) is often detected in diverse aquatic bodies, and ineffective management can lead to detrimental effects on human health and ecosystems. In this study, degradation of DCF by Fe(III) and Mn(II) activating bisulfite (BS) was investigated. In the Fe(III)/Mn(II)/BS system, 93.4% DCF was degraded at 200 μM BS within 120 s, and additional research on 1000 μM BS achieved 88.4% degradation efficacy. Moreover, kinetics fitting of DCF degradation with the different BS concentrations was studied to find the two highest reaction rates (200 and 1000 μM, kobs = 0.0297 and 0.0317 s−1, respectively). Whereafter, SO4•− and Mn(III) were identified as the main active species at these two concentrations, respectively. Density functional theory (DFT) calculations, molecular frontier orbital theory, and surface electrostatic potential (ESP) forecast electrophilic attack sites. DCF degradation pathways by radical and non-radical ways were proposed by attack site prediction and thirteen intermediates identified by UPLC-QTOF-MS. ECOSAR software 2.2 was used for toxicity assessment. This work studied DCF degradation by the Fe(III)/Mn(II)/BS process in the presence of different concentrations of BS, providing a new insight into water purification.</description><identifier>ISSN: 2073-4441</identifier><identifier>EISSN: 2073-4441</identifier><identifier>DOI: 10.3390/w16141994</identifier><language>eng</language><publisher>Basel: MDPI AG</publisher><subject>Acids ; Alcohol ; Aquatic resources ; Aqueous solutions ; bisulfites ; China ; computer software ; density functional theory ; Density functionals ; diclofenac ; Drinking water ; Experiments ; human health ; Lewis acids ; Nitrates ; Nonsteroidal anti-inflammatory drugs ; Oxidation ; Performance evaluation ; Personal care industry ; prediction ; Sodium ; Software ; species ; Sulfites ; Tetracycline ; Tetracyclines ; Toiletries ; Toxicity ; water ; water purification ; Water treatment</subject><ispartof>Water (Basel), 2024-07, Vol.16 (14), p.1994</ispartof><rights>COPYRIGHT 2024 MDPI AG</rights><rights>2024 by the authors. Licensee MDPI, Basel, Switzerland. This article is an open access article distributed under the terms and conditions of the Creative Commons Attribution (CC BY) license (https://creativecommons.org/licenses/by/4.0/). Notwithstanding the ProQuest Terms and Conditions, you may use this content in accordance with the terms of the License.</rights><lds50>peer_reviewed</lds50><oa>free_for_read</oa><woscitedreferencessubscribed>false</woscitedreferencessubscribed><cites>FETCH-LOGICAL-c282t-f64eb2ad5f1b42fd4fdecfceda9eb5027b24e13feaf84b84ca338a390bca2ec33</cites><orcidid>0000-0003-0588-571X</orcidid></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><link.rule.ids>314,776,780,27901,27902</link.rule.ids></links><search><creatorcontrib>Wang, Hongbin</creatorcontrib><creatorcontrib>Kuang, Shijie</creatorcontrib><creatorcontrib>Su, Youlun</creatorcontrib><creatorcontrib>Ren, Xu</creatorcontrib><creatorcontrib>Yang, Bowen</creatorcontrib><creatorcontrib>Sun, Yongliang</creatorcontrib><title>Degradation of Diclofenac by Bisulfite Coupled with Iron and Manganous Ions: Dual Mechanism, DFT-Assisted Pathway Studies, and Toxicity Assessment</title><title>Water (Basel)</title><description>Diclofenac (DCF) is often detected in diverse aquatic bodies, and ineffective management can lead to detrimental effects on human health and ecosystems. In this study, degradation of DCF by Fe(III) and Mn(II) activating bisulfite (BS) was investigated. In the Fe(III)/Mn(II)/BS system, 93.4% DCF was degraded at 200 μM BS within 120 s, and additional research on 1000 μM BS achieved 88.4% degradation efficacy. Moreover, kinetics fitting of DCF degradation with the different BS concentrations was studied to find the two highest reaction rates (200 and 1000 μM, kobs = 0.0297 and 0.0317 s−1, respectively). Whereafter, SO4•− and Mn(III) were identified as the main active species at these two concentrations, respectively. Density functional theory (DFT) calculations, molecular frontier orbital theory, and surface electrostatic potential (ESP) forecast electrophilic attack sites. DCF degradation pathways by radical and non-radical ways were proposed by attack site prediction and thirteen intermediates identified by UPLC-QTOF-MS. ECOSAR software 2.2 was used for toxicity assessment. This work studied DCF degradation by the Fe(III)/Mn(II)/BS process in the presence of different concentrations of BS, providing a new insight into water purification.</description><subject>Acids</subject><subject>Alcohol</subject><subject>Aquatic resources</subject><subject>Aqueous solutions</subject><subject>bisulfites</subject><subject>China</subject><subject>computer software</subject><subject>density functional theory</subject><subject>Density functionals</subject><subject>diclofenac</subject><subject>Drinking water</subject><subject>Experiments</subject><subject>human health</subject><subject>Lewis acids</subject><subject>Nitrates</subject><subject>Nonsteroidal anti-inflammatory drugs</subject><subject>Oxidation</subject><subject>Performance evaluation</subject><subject>Personal care industry</subject><subject>prediction</subject><subject>Sodium</subject><subject>Software</subject><subject>species</subject><subject>Sulfites</subject><subject>Tetracycline</subject><subject>Tetracyclines</subject><subject>Toiletries</subject><subject>Toxicity</subject><subject>water</subject><subject>water purification</subject><subject>Water treatment</subject><issn>2073-4441</issn><issn>2073-4441</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2024</creationdate><recordtype>article</recordtype><sourceid>BENPR</sourceid><recordid>eNptkd1u1DAQhSMEElXpBW9giRuQmhL_ZONwt-zSdqVWILFcWxN7vOsqsZfY0XZfgyfGbREtqJ4LW6PvHI3PFMVbWp1x3lYf93RGBW1b8aI4YlXDSyEEffnk_bo4ifGmyke0UtbVUfFriZsRDCQXPAmWLJ3ug0UPmnQH8tnFqbcuIVmEadejIXuXtmQ1Zhi8IdfgN-DDFMkq-PiJLCfoyTXqLXgXh1OyPF-X8xhdTFn6DdJ2DwfyPU3GYTy9d1iHW6ddOpCMYYwD-vSmeGWhj3jy5z4ufpx_WS8uy6uvF6vF_KrUTLJU2pnAjoGpLe0Es0ZYg9pqNNBiV1es6ZhAyi2ClaKTQgPnEnJMnQaGmvPj4v2D724MPyeMSQ0uaux78Ji_pDitecPbdiYz-u4_9CZMo8_TKV7lHCUVNX-kNtCjct6GNIK-M1VzWfGmadmMZursGSqXwcHp4NG63P9H8OFBoMcQ44hW7UY3wHhQtFJ3e1d_985_A2rcn9Q</recordid><startdate>20240701</startdate><enddate>20240701</enddate><creator>Wang, Hongbin</creator><creator>Kuang, Shijie</creator><creator>Su, Youlun</creator><creator>Ren, Xu</creator><creator>Yang, Bowen</creator><creator>Sun, Yongliang</creator><general>MDPI AG</general><scope>AAYXX</scope><scope>CITATION</scope><scope>ABUWG</scope><scope>AFKRA</scope><scope>AZQEC</scope><scope>BENPR</scope><scope>CCPQU</scope><scope>DWQXO</scope><scope>PIMPY</scope><scope>PQEST</scope><scope>PQQKQ</scope><scope>PQUKI</scope><scope>PRINS</scope><scope>7S9</scope><scope>L.6</scope><orcidid>https://orcid.org/0000-0003-0588-571X</orcidid></search><sort><creationdate>20240701</creationdate><title>Degradation of Diclofenac by Bisulfite Coupled with Iron and Manganous Ions: Dual Mechanism, DFT-Assisted Pathway Studies, and Toxicity Assessment</title><author>Wang, Hongbin ; Kuang, Shijie ; Su, Youlun ; Ren, Xu ; Yang, Bowen ; Sun, Yongliang</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-c282t-f64eb2ad5f1b42fd4fdecfceda9eb5027b24e13feaf84b84ca338a390bca2ec33</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2024</creationdate><topic>Acids</topic><topic>Alcohol</topic><topic>Aquatic resources</topic><topic>Aqueous solutions</topic><topic>bisulfites</topic><topic>China</topic><topic>computer software</topic><topic>density functional theory</topic><topic>Density functionals</topic><topic>diclofenac</topic><topic>Drinking water</topic><topic>Experiments</topic><topic>human health</topic><topic>Lewis acids</topic><topic>Nitrates</topic><topic>Nonsteroidal anti-inflammatory drugs</topic><topic>Oxidation</topic><topic>Performance evaluation</topic><topic>Personal care industry</topic><topic>prediction</topic><topic>Sodium</topic><topic>Software</topic><topic>species</topic><topic>Sulfites</topic><topic>Tetracycline</topic><topic>Tetracyclines</topic><topic>Toiletries</topic><topic>Toxicity</topic><topic>water</topic><topic>water purification</topic><topic>Water treatment</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Wang, Hongbin</creatorcontrib><creatorcontrib>Kuang, Shijie</creatorcontrib><creatorcontrib>Su, Youlun</creatorcontrib><creatorcontrib>Ren, Xu</creatorcontrib><creatorcontrib>Yang, Bowen</creatorcontrib><creatorcontrib>Sun, Yongliang</creatorcontrib><collection>CrossRef</collection><collection>ProQuest Central (Alumni Edition)</collection><collection>ProQuest Central UK/Ireland</collection><collection>ProQuest Central Essentials</collection><collection>ProQuest Central</collection><collection>ProQuest One Community College</collection><collection>ProQuest Central Korea</collection><collection>Publicly Available Content Database</collection><collection>ProQuest One Academic Eastern Edition (DO NOT USE)</collection><collection>ProQuest One Academic</collection><collection>ProQuest One Academic UKI Edition</collection><collection>ProQuest Central China</collection><collection>AGRICOLA</collection><collection>AGRICOLA - Academic</collection><jtitle>Water (Basel)</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Wang, Hongbin</au><au>Kuang, Shijie</au><au>Su, Youlun</au><au>Ren, Xu</au><au>Yang, Bowen</au><au>Sun, Yongliang</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Degradation of Diclofenac by Bisulfite Coupled with Iron and Manganous Ions: Dual Mechanism, DFT-Assisted Pathway Studies, and Toxicity Assessment</atitle><jtitle>Water (Basel)</jtitle><date>2024-07-01</date><risdate>2024</risdate><volume>16</volume><issue>14</issue><spage>1994</spage><pages>1994-</pages><issn>2073-4441</issn><eissn>2073-4441</eissn><abstract>Diclofenac (DCF) is often detected in diverse aquatic bodies, and ineffective management can lead to detrimental effects on human health and ecosystems. In this study, degradation of DCF by Fe(III) and Mn(II) activating bisulfite (BS) was investigated. In the Fe(III)/Mn(II)/BS system, 93.4% DCF was degraded at 200 μM BS within 120 s, and additional research on 1000 μM BS achieved 88.4% degradation efficacy. Moreover, kinetics fitting of DCF degradation with the different BS concentrations was studied to find the two highest reaction rates (200 and 1000 μM, kobs = 0.0297 and 0.0317 s−1, respectively). Whereafter, SO4•− and Mn(III) were identified as the main active species at these two concentrations, respectively. Density functional theory (DFT) calculations, molecular frontier orbital theory, and surface electrostatic potential (ESP) forecast electrophilic attack sites. DCF degradation pathways by radical and non-radical ways were proposed by attack site prediction and thirteen intermediates identified by UPLC-QTOF-MS. ECOSAR software 2.2 was used for toxicity assessment. This work studied DCF degradation by the Fe(III)/Mn(II)/BS process in the presence of different concentrations of BS, providing a new insight into water purification.</abstract><cop>Basel</cop><pub>MDPI AG</pub><doi>10.3390/w16141994</doi><orcidid>https://orcid.org/0000-0003-0588-571X</orcidid><oa>free_for_read</oa></addata></record> |
fulltext | fulltext |
identifier | ISSN: 2073-4441 |
ispartof | Water (Basel), 2024-07, Vol.16 (14), p.1994 |
issn | 2073-4441 2073-4441 |
language | eng |
recordid | cdi_proquest_miscellaneous_3153739968 |
source | MDPI - Multidisciplinary Digital Publishing Institute; Elektronische Zeitschriftenbibliothek - Frei zugängliche E-Journals |
subjects | Acids Alcohol Aquatic resources Aqueous solutions bisulfites China computer software density functional theory Density functionals diclofenac Drinking water Experiments human health Lewis acids Nitrates Nonsteroidal anti-inflammatory drugs Oxidation Performance evaluation Personal care industry prediction Sodium Software species Sulfites Tetracycline Tetracyclines Toiletries Toxicity water water purification Water treatment |
title | Degradation of Diclofenac by Bisulfite Coupled with Iron and Manganous Ions: Dual Mechanism, DFT-Assisted Pathway Studies, and Toxicity Assessment |
url | https://sfx.bib-bvb.de/sfx_tum?ctx_ver=Z39.88-2004&ctx_enc=info:ofi/enc:UTF-8&ctx_tim=2025-01-28T17%3A48%3A07IST&url_ver=Z39.88-2004&url_ctx_fmt=infofi/fmt:kev:mtx:ctx&rfr_id=info:sid/primo.exlibrisgroup.com:primo3-Article-gale_proqu&rft_val_fmt=info:ofi/fmt:kev:mtx:journal&rft.genre=article&rft.atitle=Degradation%20of%20Diclofenac%20by%20Bisulfite%20Coupled%20with%20Iron%20and%20Manganous%20Ions:%20Dual%20Mechanism,%20DFT-Assisted%20Pathway%20Studies,%20and%20Toxicity%20Assessment&rft.jtitle=Water%20(Basel)&rft.au=Wang,%20Hongbin&rft.date=2024-07-01&rft.volume=16&rft.issue=14&rft.spage=1994&rft.pages=1994-&rft.issn=2073-4441&rft.eissn=2073-4441&rft_id=info:doi/10.3390/w16141994&rft_dat=%3Cgale_proqu%3EA803779261%3C/gale_proqu%3E%3Curl%3E%3C/url%3E&disable_directlink=true&sfx.directlink=off&sfx.report_link=0&rft_id=info:oai/&rft_pqid=3085081453&rft_id=info:pmid/&rft_galeid=A803779261&rfr_iscdi=true |