Effective Toluene Ozonation over δ‑MnO2: Oxygen Vacancy-Induced Reactive Oxygen Species
To improve the reactivity and lifetime of catalysts in the catalytic ozonation of toluene, a simple strategy was provided to regulate the morphology and microstructure of δ-MnO2 via the hydrothermal reaction temperature. The effects of the reaction temperature and the ozone to toluene concentration...
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Veröffentlicht in: | Environmental science & technology 2023-02, Vol.57 (7), p.2918-2927 |
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description | To improve the reactivity and lifetime of catalysts in the catalytic ozonation of toluene, a simple strategy was provided to regulate the morphology and microstructure of δ-MnO2 via the hydrothermal reaction temperature. The effects of the reaction temperature and the ozone to toluene concentration ratio on the catalyst performance were investigated. The optimized MnO2-260 catalyst prepared at the limiting hydrothermal temperature (260 °C) showed high catalytic activity (X Tol = 95%) and excellent stability (1200 min) at the approximately ambient temperature of 40 °C, which was superior to the results in previous studies. The structure and morphology of δ-MnO2 were characterized by extended X-ray absorption fine structure, X-ray diffraction, scanning electron microscopy, positron annihilation lifetime spectroscopy, electron spin resonance, and other techniques. Experimental results and density functional theory calculations were in agreement that surface oxygen vacancy clusters, especially surface oxygen dimer vacancies, are critical in ozone activation. Oxygen vacancies can facilitate the adsorption and activation of O3 to generate reactive oxygen species (ROS, including 1O2, O2 –, and •OH), leading to superior ozonation activity to degrade toluene and intermediates. Meanwhile, free radical detection and scavenger tests indicated that •OH is the primary ROS during toluene ozonation rather than 1O2 or O2 –. |
doi_str_mv | 10.1021/acs.est.2c07661 |
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The effects of the reaction temperature and the ozone to toluene concentration ratio on the catalyst performance were investigated. The optimized MnO2-260 catalyst prepared at the limiting hydrothermal temperature (260 °C) showed high catalytic activity (X Tol = 95%) and excellent stability (1200 min) at the approximately ambient temperature of 40 °C, which was superior to the results in previous studies. The structure and morphology of δ-MnO2 were characterized by extended X-ray absorption fine structure, X-ray diffraction, scanning electron microscopy, positron annihilation lifetime spectroscopy, electron spin resonance, and other techniques. Experimental results and density functional theory calculations were in agreement that surface oxygen vacancy clusters, especially surface oxygen dimer vacancies, are critical in ozone activation. Oxygen vacancies can facilitate the adsorption and activation of O3 to generate reactive oxygen species (ROS, including 1O2, O2 –, and •OH), leading to superior ozonation activity to degrade toluene and intermediates. Meanwhile, free radical detection and scavenger tests indicated that •OH is the primary ROS during toluene ozonation rather than 1O2 or O2 –.</description><identifier>ISSN: 0013-936X</identifier><identifier>EISSN: 1520-5851</identifier><identifier>DOI: 10.1021/acs.est.2c07661</identifier><language>eng</language><publisher>Easton: American Chemical Society</publisher><subject>Ambient temperature ; Catalysts ; Catalytic activity ; Density functional theory ; Electron paramagnetic resonance ; Electron spin ; Electron spin resonance ; Fine structure ; Free radicals ; Hydrothermal reactions ; Intermediates ; Manganese dioxide ; Morphology ; Oxygen ; Ozonation ; Ozone ; Positron annihilation ; Reactive oxygen species ; Scanning electron microscopy ; Spectroscopy ; Spin resonance ; Toluene ; Treatment and Resource Recovery ; Ultrastructure ; X ray absorption ; X-ray diffraction</subject><ispartof>Environmental science & technology, 2023-02, Vol.57 (7), p.2918-2927</ispartof><rights>2023 American Chemical Society</rights><rights>Copyright American Chemical Society Feb 21, 2023</rights><lds50>peer_reviewed</lds50><woscitedreferencessubscribed>false</woscitedreferencessubscribed><orcidid>0000-0001-8476-8217 ; 0000-0003-2124-0620 ; 0000-0002-5258-906X</orcidid></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><linktopdf>$$Uhttps://pubs.acs.org/doi/pdf/10.1021/acs.est.2c07661$$EPDF$$P50$$Gacs$$H</linktopdf><linktohtml>$$Uhttps://pubs.acs.org/doi/10.1021/acs.est.2c07661$$EHTML$$P50$$Gacs$$H</linktohtml><link.rule.ids>314,780,784,27076,27924,27925,56738,56788</link.rule.ids></links><search><creatorcontrib>Lu, Yuqin</creatorcontrib><creatorcontrib>Deng, Hua</creatorcontrib><creatorcontrib>Pan, Tingting</creatorcontrib><creatorcontrib>Liao, Xu</creatorcontrib><creatorcontrib>Zhang, Changbin</creatorcontrib><creatorcontrib>He, Hong</creatorcontrib><title>Effective Toluene Ozonation over δ‑MnO2: Oxygen Vacancy-Induced Reactive Oxygen Species</title><title>Environmental science & technology</title><addtitle>Environ. Sci. Technol</addtitle><description>To improve the reactivity and lifetime of catalysts in the catalytic ozonation of toluene, a simple strategy was provided to regulate the morphology and microstructure of δ-MnO2 via the hydrothermal reaction temperature. The effects of the reaction temperature and the ozone to toluene concentration ratio on the catalyst performance were investigated. The optimized MnO2-260 catalyst prepared at the limiting hydrothermal temperature (260 °C) showed high catalytic activity (X Tol = 95%) and excellent stability (1200 min) at the approximately ambient temperature of 40 °C, which was superior to the results in previous studies. The structure and morphology of δ-MnO2 were characterized by extended X-ray absorption fine structure, X-ray diffraction, scanning electron microscopy, positron annihilation lifetime spectroscopy, electron spin resonance, and other techniques. Experimental results and density functional theory calculations were in agreement that surface oxygen vacancy clusters, especially surface oxygen dimer vacancies, are critical in ozone activation. Oxygen vacancies can facilitate the adsorption and activation of O3 to generate reactive oxygen species (ROS, including 1O2, O2 –, and •OH), leading to superior ozonation activity to degrade toluene and intermediates. Meanwhile, free radical detection and scavenger tests indicated that •OH is the primary ROS during toluene ozonation rather than 1O2 or O2 –.</description><subject>Ambient temperature</subject><subject>Catalysts</subject><subject>Catalytic activity</subject><subject>Density functional theory</subject><subject>Electron paramagnetic resonance</subject><subject>Electron spin</subject><subject>Electron spin resonance</subject><subject>Fine structure</subject><subject>Free radicals</subject><subject>Hydrothermal reactions</subject><subject>Intermediates</subject><subject>Manganese dioxide</subject><subject>Morphology</subject><subject>Oxygen</subject><subject>Ozonation</subject><subject>Ozone</subject><subject>Positron annihilation</subject><subject>Reactive oxygen species</subject><subject>Scanning electron microscopy</subject><subject>Spectroscopy</subject><subject>Spin resonance</subject><subject>Toluene</subject><subject>Treatment and Resource Recovery</subject><subject>Ultrastructure</subject><subject>X ray absorption</subject><subject>X-ray diffraction</subject><issn>0013-936X</issn><issn>1520-5851</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2023</creationdate><recordtype>article</recordtype><recordid>eNpdkMFKAzEQhoMoWKtnrwteBNmaSUyy8SalaqGyoFXEy5JmJ7JlzdZmt1hPvoLv4nP4ED6JW1oQPA3MfP_P8BFyCLQHlMGpsaGHoe4xS5WUsEU6IBiNRSJgm3QoBR5rLh93yV4IU0op4zTpkKeBc2jrYoHRuCob9Bil75U3dVH5qFrgPPr--vn4vPEpO4_St-Uz-ujBWOPtMh76vLGYR7do1g2b-90MbYFhn-w4UwY82Mwuub8cjPvX8Si9GvYvRrFhgtWxyoFbqSZIndEAWktLhVUuZzk6DTqZcEws6oSiVmAcGASjnRQSOE8SzbvkeN07m1evTasgeymCxbI0HqsmZExJzZWk4qxFj_6h06qZ-_a7llIahNJUtNTJmmqV_gFAs5XnbLVcJTee-S_lgHMC</recordid><startdate>20230221</startdate><enddate>20230221</enddate><creator>Lu, Yuqin</creator><creator>Deng, Hua</creator><creator>Pan, Tingting</creator><creator>Liao, Xu</creator><creator>Zhang, Changbin</creator><creator>He, Hong</creator><general>American Chemical Society</general><scope>7QO</scope><scope>7ST</scope><scope>7T7</scope><scope>7U7</scope><scope>8FD</scope><scope>C1K</scope><scope>FR3</scope><scope>P64</scope><scope>SOI</scope><scope>7X8</scope><orcidid>https://orcid.org/0000-0001-8476-8217</orcidid><orcidid>https://orcid.org/0000-0003-2124-0620</orcidid><orcidid>https://orcid.org/0000-0002-5258-906X</orcidid></search><sort><creationdate>20230221</creationdate><title>Effective Toluene Ozonation over δ‑MnO2: Oxygen Vacancy-Induced Reactive Oxygen Species</title><author>Lu, Yuqin ; Deng, Hua ; Pan, Tingting ; Liao, Xu ; Zhang, Changbin ; He, Hong</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-a252t-7d13c67be0fa911996c05c7fd2def9198b3e8ce980e971af1ae1a9f6561338893</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2023</creationdate><topic>Ambient temperature</topic><topic>Catalysts</topic><topic>Catalytic activity</topic><topic>Density functional theory</topic><topic>Electron paramagnetic resonance</topic><topic>Electron spin</topic><topic>Electron spin resonance</topic><topic>Fine structure</topic><topic>Free radicals</topic><topic>Hydrothermal reactions</topic><topic>Intermediates</topic><topic>Manganese dioxide</topic><topic>Morphology</topic><topic>Oxygen</topic><topic>Ozonation</topic><topic>Ozone</topic><topic>Positron annihilation</topic><topic>Reactive oxygen species</topic><topic>Scanning electron microscopy</topic><topic>Spectroscopy</topic><topic>Spin resonance</topic><topic>Toluene</topic><topic>Treatment and Resource Recovery</topic><topic>Ultrastructure</topic><topic>X ray absorption</topic><topic>X-ray diffraction</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Lu, Yuqin</creatorcontrib><creatorcontrib>Deng, Hua</creatorcontrib><creatorcontrib>Pan, Tingting</creatorcontrib><creatorcontrib>Liao, Xu</creatorcontrib><creatorcontrib>Zhang, Changbin</creatorcontrib><creatorcontrib>He, Hong</creatorcontrib><collection>Biotechnology Research Abstracts</collection><collection>Environment Abstracts</collection><collection>Industrial and Applied Microbiology Abstracts (Microbiology A)</collection><collection>Toxicology Abstracts</collection><collection>Technology Research Database</collection><collection>Environmental Sciences and Pollution Management</collection><collection>Engineering Research Database</collection><collection>Biotechnology and BioEngineering Abstracts</collection><collection>Environment Abstracts</collection><collection>MEDLINE - Academic</collection><jtitle>Environmental science & technology</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Lu, Yuqin</au><au>Deng, Hua</au><au>Pan, Tingting</au><au>Liao, Xu</au><au>Zhang, Changbin</au><au>He, Hong</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Effective Toluene Ozonation over δ‑MnO2: Oxygen Vacancy-Induced Reactive Oxygen Species</atitle><jtitle>Environmental science & technology</jtitle><addtitle>Environ. Sci. Technol</addtitle><date>2023-02-21</date><risdate>2023</risdate><volume>57</volume><issue>7</issue><spage>2918</spage><epage>2927</epage><pages>2918-2927</pages><issn>0013-936X</issn><eissn>1520-5851</eissn><abstract>To improve the reactivity and lifetime of catalysts in the catalytic ozonation of toluene, a simple strategy was provided to regulate the morphology and microstructure of δ-MnO2 via the hydrothermal reaction temperature. The effects of the reaction temperature and the ozone to toluene concentration ratio on the catalyst performance were investigated. The optimized MnO2-260 catalyst prepared at the limiting hydrothermal temperature (260 °C) showed high catalytic activity (X Tol = 95%) and excellent stability (1200 min) at the approximately ambient temperature of 40 °C, which was superior to the results in previous studies. The structure and morphology of δ-MnO2 were characterized by extended X-ray absorption fine structure, X-ray diffraction, scanning electron microscopy, positron annihilation lifetime spectroscopy, electron spin resonance, and other techniques. Experimental results and density functional theory calculations were in agreement that surface oxygen vacancy clusters, especially surface oxygen dimer vacancies, are critical in ozone activation. Oxygen vacancies can facilitate the adsorption and activation of O3 to generate reactive oxygen species (ROS, including 1O2, O2 –, and •OH), leading to superior ozonation activity to degrade toluene and intermediates. Meanwhile, free radical detection and scavenger tests indicated that •OH is the primary ROS during toluene ozonation rather than 1O2 or O2 –.</abstract><cop>Easton</cop><pub>American Chemical Society</pub><doi>10.1021/acs.est.2c07661</doi><tpages>10</tpages><orcidid>https://orcid.org/0000-0001-8476-8217</orcidid><orcidid>https://orcid.org/0000-0003-2124-0620</orcidid><orcidid>https://orcid.org/0000-0002-5258-906X</orcidid></addata></record> |
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subjects | Ambient temperature Catalysts Catalytic activity Density functional theory Electron paramagnetic resonance Electron spin Electron spin resonance Fine structure Free radicals Hydrothermal reactions Intermediates Manganese dioxide Morphology Oxygen Ozonation Ozone Positron annihilation Reactive oxygen species Scanning electron microscopy Spectroscopy Spin resonance Toluene Treatment and Resource Recovery Ultrastructure X ray absorption X-ray diffraction |
title | Effective Toluene Ozonation over δ‑MnO2: Oxygen Vacancy-Induced Reactive Oxygen Species |
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