Copper–catalyzed activation of molecular oxygen for oxidative destruction of acetaminophen: The mechanism and superoxide-mediated cycling of copper species
In this study, the commercial zero-valent copper (ZVC) was investigated to activate the molecular oxygen (O2) for the degradation of acetaminophen (ACT). 50 mg/L ACT could be completely decomposed within 4 h in the ZVC/air system at initial pH 3.0. The H2O2, hydroxyl radical (OH) and superoxide anio...
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Veröffentlicht in: | Chemosphere (Oxford) 2017-01, Vol.166, p.89-95 |
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description | In this study, the commercial zero-valent copper (ZVC) was investigated to activate the molecular oxygen (O2) for the degradation of acetaminophen (ACT). 50 mg/L ACT could be completely decomposed within 4 h in the ZVC/air system at initial pH 3.0. The H2O2, hydroxyl radical (OH) and superoxide anion radical (O2−) were identified as the main reactive oxygen species (ROSs) generated in the above reaction; however, only OH caused the decomposition and mineralization of ACT in the copper-catalyzed O2 activation process. In addition, the in-situ generated Cu+ from ZVC dissolution not only activated O2 to produce H2O2, but also initiated the decomposition of H2O2 to generate OH. Meanwhile, the H2O2 could also be partly decomposed into O2−, which served as a mediator for copper cycling by reduction of Cu2+ to Cu+ in the ZVC/air system. Therefore, OH could be continuously generated; and then ACT was effectively degraded. Additionally, the effect of solution pH and the dosage of ZVC were also investigated. As a result, this study indicated the key behavior of the O2− during Cu–catalyzed activation of O2, which further improved the understanding of O2 activation mechanism by zero-valent metals.
[Display omitted]
•The ZVC/air system was effective in degradation of ACT.•The Cu+ was responsible for activation of O2 to produce H2O2.•The O2− was formed via the decomposition of H2O2 in the ZVC/air system.•It was proved that the O2− mediated the copper cycling by reduction of Cu2+ to Cu+. |
doi_str_mv | 10.1016/j.chemosphere.2016.09.066 |
format | Article |
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[Display omitted]
•The ZVC/air system was effective in degradation of ACT.•The Cu+ was responsible for activation of O2 to produce H2O2.•The O2− was formed via the decomposition of H2O2 in the ZVC/air system.•It was proved that the O2− mediated the copper cycling by reduction of Cu2+ to Cu+.</description><identifier>ISSN: 0045-6535</identifier><identifier>EISSN: 1879-1298</identifier><identifier>DOI: 10.1016/j.chemosphere.2016.09.066</identifier><identifier>PMID: 27689888</identifier><language>eng</language><publisher>England: Elsevier Ltd</publisher><subject>Acetaminophen ; Acetaminophen - chemistry ; Activation molecular oxygen ; Aerobiosis ; Biodegradation, Environmental ; Catalysis ; Copper - chemistry ; Hydrogen Peroxide - chemistry ; Hydrogen-Ion Concentration ; Hydroxyl Radical - chemistry ; Oxidation-Reduction ; Oxidative destruction ; Oxygen - chemistry ; Reactive Oxygen Species - metabolism ; Solutions ; Superoxide anion radical ; Superoxides - chemistry ; X-Ray Diffraction ; Zero-valent copper</subject><ispartof>Chemosphere (Oxford), 2017-01, Vol.166, p.89-95</ispartof><rights>2016 Elsevier Ltd</rights><rights>Copyright © 2016 Elsevier Ltd. All rights reserved.</rights><lds50>peer_reviewed</lds50><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-c410t-7067f33678c8e1206b706ef44190dddf565605b4515dc0f703fda77af20ea1353</citedby><cites>FETCH-LOGICAL-c410t-7067f33678c8e1206b706ef44190dddf565605b4515dc0f703fda77af20ea1353</cites></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><linktohtml>$$Uhttps://dx.doi.org/10.1016/j.chemosphere.2016.09.066$$EHTML$$P50$$Gelsevier$$H</linktohtml><link.rule.ids>314,776,780,3536,27903,27904,45974</link.rule.ids><backlink>$$Uhttps://www.ncbi.nlm.nih.gov/pubmed/27689888$$D View this record in MEDLINE/PubMed$$Hfree_for_read</backlink></links><search><creatorcontrib>Zhang, Yunfei</creatorcontrib><creatorcontrib>Fan, Jinhong</creatorcontrib><creatorcontrib>Yang, Bo</creatorcontrib><creatorcontrib>Huang, Wutao</creatorcontrib><creatorcontrib>Ma, Luming</creatorcontrib><title>Copper–catalyzed activation of molecular oxygen for oxidative destruction of acetaminophen: The mechanism and superoxide-mediated cycling of copper species</title><title>Chemosphere (Oxford)</title><addtitle>Chemosphere</addtitle><description>In this study, the commercial zero-valent copper (ZVC) was investigated to activate the molecular oxygen (O2) for the degradation of acetaminophen (ACT). 50 mg/L ACT could be completely decomposed within 4 h in the ZVC/air system at initial pH 3.0. The H2O2, hydroxyl radical (OH) and superoxide anion radical (O2−) were identified as the main reactive oxygen species (ROSs) generated in the above reaction; however, only OH caused the decomposition and mineralization of ACT in the copper-catalyzed O2 activation process. In addition, the in-situ generated Cu+ from ZVC dissolution not only activated O2 to produce H2O2, but also initiated the decomposition of H2O2 to generate OH. Meanwhile, the H2O2 could also be partly decomposed into O2−, which served as a mediator for copper cycling by reduction of Cu2+ to Cu+ in the ZVC/air system. Therefore, OH could be continuously generated; and then ACT was effectively degraded. Additionally, the effect of solution pH and the dosage of ZVC were also investigated. As a result, this study indicated the key behavior of the O2− during Cu–catalyzed activation of O2, which further improved the understanding of O2 activation mechanism by zero-valent metals.
[Display omitted]
•The ZVC/air system was effective in degradation of ACT.•The Cu+ was responsible for activation of O2 to produce H2O2.•The O2− was formed via the decomposition of H2O2 in the ZVC/air system.•It was proved that the O2− mediated the copper cycling by reduction of Cu2+ to Cu+.</description><subject>Acetaminophen</subject><subject>Acetaminophen - chemistry</subject><subject>Activation molecular oxygen</subject><subject>Aerobiosis</subject><subject>Biodegradation, Environmental</subject><subject>Catalysis</subject><subject>Copper - chemistry</subject><subject>Hydrogen Peroxide - chemistry</subject><subject>Hydrogen-Ion Concentration</subject><subject>Hydroxyl Radical - chemistry</subject><subject>Oxidation-Reduction</subject><subject>Oxidative destruction</subject><subject>Oxygen - chemistry</subject><subject>Reactive Oxygen Species - metabolism</subject><subject>Solutions</subject><subject>Superoxide anion radical</subject><subject>Superoxides - chemistry</subject><subject>X-Ray Diffraction</subject><subject>Zero-valent copper</subject><issn>0045-6535</issn><issn>1879-1298</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2017</creationdate><recordtype>article</recordtype><sourceid>EIF</sourceid><recordid>eNqNkc1u1DAUhS0EokPhFZDZsUm4TmInYYdG_EmV2JS15bGvOx4ldrCTEdMV78Cal-NJcJgWsaw3tqzv-FyfQ8grBiUDJt4cSr3HMaRpjxHLKl-V0JcgxCOyYV3bF6zqu8dkA9DwQvCaX5BnKR0AMsn7p-SiakXXd123Ib-2YZow_v7xU6tZDadbNFTp2R3V7IKnwdIxDKiXQUUavp9u0FMb1qMzmTgiNZjmuOh7Wmmc1eh8yLP5t_R6j3REvVfepZEqb2hast0qx2JE49ScDfVJD87frHr9dxyaJtQO03PyxKoh4Yu7_ZJ8_fD-evupuPry8fP23VWhGwZz0YJobV2LttMdsgrELt-gbRrWgzHGcsEF8F3DGTcabAu1Naptla0AFat5fUlen9-dYvi25B_J0SWNw6A8hiVJ1tVt1fO8HoLyJtM1ZLQ_ozqGlCJaOUU3qniSDORapDzI_4qUa5ESepmLzNqXdzbLLuf0T3nfXAa2ZwBzLkeHUaacmNc504h6lia4B9j8AQ4Eug8</recordid><startdate>201701</startdate><enddate>201701</enddate><creator>Zhang, Yunfei</creator><creator>Fan, Jinhong</creator><creator>Yang, Bo</creator><creator>Huang, Wutao</creator><creator>Ma, Luming</creator><general>Elsevier Ltd</general><scope>CGR</scope><scope>CUY</scope><scope>CVF</scope><scope>ECM</scope><scope>EIF</scope><scope>NPM</scope><scope>AAYXX</scope><scope>CITATION</scope><scope>7X8</scope><scope>7ST</scope><scope>7TV</scope><scope>7U7</scope><scope>C1K</scope><scope>SOI</scope></search><sort><creationdate>201701</creationdate><title>Copper–catalyzed activation of molecular oxygen for oxidative destruction of acetaminophen: The mechanism and superoxide-mediated cycling of copper species</title><author>Zhang, Yunfei ; Fan, Jinhong ; Yang, Bo ; Huang, Wutao ; Ma, Luming</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-c410t-7067f33678c8e1206b706ef44190dddf565605b4515dc0f703fda77af20ea1353</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2017</creationdate><topic>Acetaminophen</topic><topic>Acetaminophen - chemistry</topic><topic>Activation molecular oxygen</topic><topic>Aerobiosis</topic><topic>Biodegradation, Environmental</topic><topic>Catalysis</topic><topic>Copper - chemistry</topic><topic>Hydrogen Peroxide - chemistry</topic><topic>Hydrogen-Ion Concentration</topic><topic>Hydroxyl Radical - chemistry</topic><topic>Oxidation-Reduction</topic><topic>Oxidative destruction</topic><topic>Oxygen - chemistry</topic><topic>Reactive Oxygen Species - metabolism</topic><topic>Solutions</topic><topic>Superoxide anion radical</topic><topic>Superoxides - chemistry</topic><topic>X-Ray Diffraction</topic><topic>Zero-valent copper</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Zhang, Yunfei</creatorcontrib><creatorcontrib>Fan, Jinhong</creatorcontrib><creatorcontrib>Yang, Bo</creatorcontrib><creatorcontrib>Huang, Wutao</creatorcontrib><creatorcontrib>Ma, Luming</creatorcontrib><collection>Medline</collection><collection>MEDLINE</collection><collection>MEDLINE (Ovid)</collection><collection>MEDLINE</collection><collection>MEDLINE</collection><collection>PubMed</collection><collection>CrossRef</collection><collection>MEDLINE - Academic</collection><collection>Environment Abstracts</collection><collection>Pollution Abstracts</collection><collection>Toxicology Abstracts</collection><collection>Environmental Sciences and Pollution Management</collection><collection>Environment Abstracts</collection><jtitle>Chemosphere (Oxford)</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Zhang, Yunfei</au><au>Fan, Jinhong</au><au>Yang, Bo</au><au>Huang, Wutao</au><au>Ma, Luming</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Copper–catalyzed activation of molecular oxygen for oxidative destruction of acetaminophen: The mechanism and superoxide-mediated cycling of copper species</atitle><jtitle>Chemosphere (Oxford)</jtitle><addtitle>Chemosphere</addtitle><date>2017-01</date><risdate>2017</risdate><volume>166</volume><spage>89</spage><epage>95</epage><pages>89-95</pages><issn>0045-6535</issn><eissn>1879-1298</eissn><abstract>In this study, the commercial zero-valent copper (ZVC) was investigated to activate the molecular oxygen (O2) for the degradation of acetaminophen (ACT). 50 mg/L ACT could be completely decomposed within 4 h in the ZVC/air system at initial pH 3.0. The H2O2, hydroxyl radical (OH) and superoxide anion radical (O2−) were identified as the main reactive oxygen species (ROSs) generated in the above reaction; however, only OH caused the decomposition and mineralization of ACT in the copper-catalyzed O2 activation process. In addition, the in-situ generated Cu+ from ZVC dissolution not only activated O2 to produce H2O2, but also initiated the decomposition of H2O2 to generate OH. Meanwhile, the H2O2 could also be partly decomposed into O2−, which served as a mediator for copper cycling by reduction of Cu2+ to Cu+ in the ZVC/air system. Therefore, OH could be continuously generated; and then ACT was effectively degraded. Additionally, the effect of solution pH and the dosage of ZVC were also investigated. As a result, this study indicated the key behavior of the O2− during Cu–catalyzed activation of O2, which further improved the understanding of O2 activation mechanism by zero-valent metals.
[Display omitted]
•The ZVC/air system was effective in degradation of ACT.•The Cu+ was responsible for activation of O2 to produce H2O2.•The O2− was formed via the decomposition of H2O2 in the ZVC/air system.•It was proved that the O2− mediated the copper cycling by reduction of Cu2+ to Cu+.</abstract><cop>England</cop><pub>Elsevier Ltd</pub><pmid>27689888</pmid><doi>10.1016/j.chemosphere.2016.09.066</doi><tpages>7</tpages></addata></record> |
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subjects | Acetaminophen Acetaminophen - chemistry Activation molecular oxygen Aerobiosis Biodegradation, Environmental Catalysis Copper - chemistry Hydrogen Peroxide - chemistry Hydrogen-Ion Concentration Hydroxyl Radical - chemistry Oxidation-Reduction Oxidative destruction Oxygen - chemistry Reactive Oxygen Species - metabolism Solutions Superoxide anion radical Superoxides - chemistry X-Ray Diffraction Zero-valent copper |
title | Copper–catalyzed activation of molecular oxygen for oxidative destruction of acetaminophen: The mechanism and superoxide-mediated cycling of copper species |
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