Coupling metal–organic frameworks and g-C3N4 to derive Fe@N-doped graphene-like carbon for peroxymonosulfate activation: Upgrading framework stability and performance
[Display omitted] •A novel Fe@N-doped graphene-like carbon for activation PMS was synthesized.•Combined NH2 groups and g-C3N4 stabilized the framework morphology.•The degradation pathway of ABEE was first reported in the AOP field.•Fe@N-doped graphene-like carbon/PMS involved multi-oxidative pathway...
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Veröffentlicht in: | Applied catalysis. B, Environmental Environmental, 2019-10, Vol.255, p.1, Article 117763 |
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creator | Liu, Chao Liu, Liyuan Tian, Xing Wang, Yiping Li, Ruoyu Zhang, Yuting Song, Zilong Xu, Bingbing Chu, Wei Qi, Fei Ikhlaq, Amir |
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•A novel Fe@N-doped graphene-like carbon for activation PMS was synthesized.•Combined NH2 groups and g-C3N4 stabilized the framework morphology.•The degradation pathway of ABEE was first reported in the AOP field.•Fe@N-doped graphene-like carbon/PMS involved multi-oxidative pathways.•Nitrogen species and C = O contributed to the outstanding catalytic activity.
A highly active mediator (Fe@N-doped graphene-like carbon) for peroxymonosulfate (PMS) activation was prepared by employing g-C3N4 assisting NH2-MIL-53(Fe) as the precursor. The addition of combined nitrogen sources (g-C3N4 and NH2 groups) not only stabilized the phase composition and framework morphology, but also improved PMS activation performance significantly. In addition, the introduction of g-C3N4 increased the surface area. Electron paramagnetic resonance (EPR) spectroscopy and radical quenching experiments identified singlet oxygen (1O2), superoxide radicals (O2•−), hydroxyl radicals (•OH), and sulfate radicals (SO4•−) as the reactive oxygen species (ROS) in 4-aminobenzoic acid ethyl ether (ABEE) degradation via a combination process of nonradical and radical processes. The variable chemical valences of iron nanoparticles and quaternary-N, pyrrolic-N, pyridinic-N, and carbonyl (C=O) groups in the support contributed to the outstanding catalytic activity. A possible mechanism for PMS activation by Fe@N-doped graphene-like carbon for ABEE degradation was proposed, which involved sp2 hybridized carbon and electron-rich sp2 sites of the graphitic domain activating PMS via electron transfer. Intermediates were identified using liquid chromatography-quadrupole time-of-flight mass spectrometry (LC-Q-TOF-MS). The degradation pathway of ABEE was reported for the first time in the advanced oxidation process field. Based on intermediate identification of sulfamethoxazole (SMX) degradation, six intermediates were first reported and a new reaction pathway established. This work provides a promising approach to the rational design of high-performance active mediators for environmental remediation. |
doi_str_mv | 10.1016/j.apcatb.2019.117763 |
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•A novel Fe@N-doped graphene-like carbon for activation PMS was synthesized.•Combined NH2 groups and g-C3N4 stabilized the framework morphology.•The degradation pathway of ABEE was first reported in the AOP field.•Fe@N-doped graphene-like carbon/PMS involved multi-oxidative pathways.•Nitrogen species and C = O contributed to the outstanding catalytic activity.
A highly active mediator (Fe@N-doped graphene-like carbon) for peroxymonosulfate (PMS) activation was prepared by employing g-C3N4 assisting NH2-MIL-53(Fe) as the precursor. The addition of combined nitrogen sources (g-C3N4 and NH2 groups) not only stabilized the phase composition and framework morphology, but also improved PMS activation performance significantly. In addition, the introduction of g-C3N4 increased the surface area. Electron paramagnetic resonance (EPR) spectroscopy and radical quenching experiments identified singlet oxygen (1O2), superoxide radicals (O2•−), hydroxyl radicals (•OH), and sulfate radicals (SO4•−) as the reactive oxygen species (ROS) in 4-aminobenzoic acid ethyl ether (ABEE) degradation via a combination process of nonradical and radical processes. The variable chemical valences of iron nanoparticles and quaternary-N, pyrrolic-N, pyridinic-N, and carbonyl (C=O) groups in the support contributed to the outstanding catalytic activity. A possible mechanism for PMS activation by Fe@N-doped graphene-like carbon for ABEE degradation was proposed, which involved sp2 hybridized carbon and electron-rich sp2 sites of the graphitic domain activating PMS via electron transfer. Intermediates were identified using liquid chromatography-quadrupole time-of-flight mass spectrometry (LC-Q-TOF-MS). The degradation pathway of ABEE was reported for the first time in the advanced oxidation process field. Based on intermediate identification of sulfamethoxazole (SMX) degradation, six intermediates were first reported and a new reaction pathway established. This work provides a promising approach to the rational design of high-performance active mediators for environmental remediation.</description><identifier>ISSN: 0926-3373</identifier><identifier>EISSN: 1873-3883</identifier><identifier>DOI: 10.1016/j.apcatb.2019.117763</identifier><language>eng</language><publisher>Amsterdam: Elsevier B.V</publisher><subject>Activation ; Biodegradation ; Carbon ; Carbon nitride ; Carbonyls ; Catalysis ; Catalytic activity ; Degradation ; Electron paramagnetic resonance ; Electron transfer ; Electrons ; Fe@N-doped graphene-like carbon ; Free radicals ; g-C3N4 ; Graphene ; Hydroxyl radicals ; Intermediates ; Iron ; Liquid chromatography ; Mass spectrometry ; Mass spectroscopy ; Metal-organic frameworks ; metal–organic framework ; Morphology ; Nanoparticles ; Nitrogen ; Nitrogen sources ; Organic chemistry ; Oxidation ; Oxidation process ; peroxymonosulfate ; Phase composition ; Quadrupoles ; Reactive oxygen species ; Singlet oxygen ; Sulfamethoxazole ; sulfate radical ; Sulfates ; Superoxide</subject><ispartof>Applied catalysis. B, Environmental, 2019-10, Vol.255, p.1, Article 117763</ispartof><rights>2019 Elsevier B.V.</rights><rights>Copyright Elsevier BV Oct 15, 2019</rights><lds50>peer_reviewed</lds50><woscitedreferencessubscribed>false</woscitedreferencessubscribed></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><linktohtml>$$Uhttps://dx.doi.org/10.1016/j.apcatb.2019.117763$$EHTML$$P50$$Gelsevier$$H</linktohtml><link.rule.ids>314,780,784,3550,27924,27925,45995</link.rule.ids></links><search><creatorcontrib>Liu, Chao</creatorcontrib><creatorcontrib>Liu, Liyuan</creatorcontrib><creatorcontrib>Tian, Xing</creatorcontrib><creatorcontrib>Wang, Yiping</creatorcontrib><creatorcontrib>Li, Ruoyu</creatorcontrib><creatorcontrib>Zhang, Yuting</creatorcontrib><creatorcontrib>Song, Zilong</creatorcontrib><creatorcontrib>Xu, Bingbing</creatorcontrib><creatorcontrib>Chu, Wei</creatorcontrib><creatorcontrib>Qi, Fei</creatorcontrib><creatorcontrib>Ikhlaq, Amir</creatorcontrib><title>Coupling metal–organic frameworks and g-C3N4 to derive Fe@N-doped graphene-like carbon for peroxymonosulfate activation: Upgrading framework stability and performance</title><title>Applied catalysis. B, Environmental</title><description>[Display omitted]
•A novel Fe@N-doped graphene-like carbon for activation PMS was synthesized.•Combined NH2 groups and g-C3N4 stabilized the framework morphology.•The degradation pathway of ABEE was first reported in the AOP field.•Fe@N-doped graphene-like carbon/PMS involved multi-oxidative pathways.•Nitrogen species and C = O contributed to the outstanding catalytic activity.
A highly active mediator (Fe@N-doped graphene-like carbon) for peroxymonosulfate (PMS) activation was prepared by employing g-C3N4 assisting NH2-MIL-53(Fe) as the precursor. The addition of combined nitrogen sources (g-C3N4 and NH2 groups) not only stabilized the phase composition and framework morphology, but also improved PMS activation performance significantly. In addition, the introduction of g-C3N4 increased the surface area. Electron paramagnetic resonance (EPR) spectroscopy and radical quenching experiments identified singlet oxygen (1O2), superoxide radicals (O2•−), hydroxyl radicals (•OH), and sulfate radicals (SO4•−) as the reactive oxygen species (ROS) in 4-aminobenzoic acid ethyl ether (ABEE) degradation via a combination process of nonradical and radical processes. The variable chemical valences of iron nanoparticles and quaternary-N, pyrrolic-N, pyridinic-N, and carbonyl (C=O) groups in the support contributed to the outstanding catalytic activity. A possible mechanism for PMS activation by Fe@N-doped graphene-like carbon for ABEE degradation was proposed, which involved sp2 hybridized carbon and electron-rich sp2 sites of the graphitic domain activating PMS via electron transfer. Intermediates were identified using liquid chromatography-quadrupole time-of-flight mass spectrometry (LC-Q-TOF-MS). The degradation pathway of ABEE was reported for the first time in the advanced oxidation process field. Based on intermediate identification of sulfamethoxazole (SMX) degradation, six intermediates were first reported and a new reaction pathway established. This work provides a promising approach to the rational design of high-performance active mediators for environmental remediation.</description><subject>Activation</subject><subject>Biodegradation</subject><subject>Carbon</subject><subject>Carbon nitride</subject><subject>Carbonyls</subject><subject>Catalysis</subject><subject>Catalytic activity</subject><subject>Degradation</subject><subject>Electron paramagnetic resonance</subject><subject>Electron transfer</subject><subject>Electrons</subject><subject>Fe@N-doped graphene-like carbon</subject><subject>Free radicals</subject><subject>g-C3N4</subject><subject>Graphene</subject><subject>Hydroxyl radicals</subject><subject>Intermediates</subject><subject>Iron</subject><subject>Liquid chromatography</subject><subject>Mass spectrometry</subject><subject>Mass spectroscopy</subject><subject>Metal-organic frameworks</subject><subject>metal–organic framework</subject><subject>Morphology</subject><subject>Nanoparticles</subject><subject>Nitrogen</subject><subject>Nitrogen sources</subject><subject>Organic chemistry</subject><subject>Oxidation</subject><subject>Oxidation process</subject><subject>peroxymonosulfate</subject><subject>Phase composition</subject><subject>Quadrupoles</subject><subject>Reactive oxygen species</subject><subject>Singlet oxygen</subject><subject>Sulfamethoxazole</subject><subject>sulfate radical</subject><subject>Sulfates</subject><subject>Superoxide</subject><issn>0926-3373</issn><issn>1873-3883</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2019</creationdate><recordtype>article</recordtype><recordid>eNo9kU1u2zAUhImiBeo6vUEXBLqWwx-JpLoIWhj5A4Jk06wJinxyqcikQtFOvMsdcomcKyepHAdZvcWbmW-AQegHJQtKqDjuFmawJjcLRmi9oFRKwT-hGVWSF1wp_hnNSM1EwbnkX9G3cewIIYwzNUMvy7gZeh9WeA3Z9K9PzzGtTPAWt8ms4SGmuxGb4PCqWPLrEueIHSS_BXwGv68LFweYfskM_yBA0fs7wNakJgbcxoQHSPFxt44hjpu-NRmwsdlvTfYx_MK3w2R0e_YHC4_ZNL73efcGnfxTzNoEC0foS2v6Eb6_3zm6PTv9u7worm7OL5d_rgpgssqFVaStFRWVpGVtiSyBlDWtJK84LaloBXNMOMmAWEmqhjemqoGa2inXONk4Pkc_D7lDivcbGLPu4iaFCakZE4QoRpSYVCcHFUxVth6SHq2HqabzCWzWLnpNid6vozt9WEfv19GHdfh_Ok6Jlw</recordid><startdate>20191015</startdate><enddate>20191015</enddate><creator>Liu, Chao</creator><creator>Liu, Liyuan</creator><creator>Tian, Xing</creator><creator>Wang, Yiping</creator><creator>Li, Ruoyu</creator><creator>Zhang, Yuting</creator><creator>Song, Zilong</creator><creator>Xu, Bingbing</creator><creator>Chu, Wei</creator><creator>Qi, Fei</creator><creator>Ikhlaq, Amir</creator><general>Elsevier B.V</general><general>Elsevier BV</general><scope>7SR</scope><scope>7ST</scope><scope>7U5</scope><scope>8BQ</scope><scope>8FD</scope><scope>C1K</scope><scope>FR3</scope><scope>JG9</scope><scope>KR7</scope><scope>L7M</scope><scope>SOI</scope></search><sort><creationdate>20191015</creationdate><title>Coupling metal–organic frameworks and g-C3N4 to derive Fe@N-doped graphene-like carbon for peroxymonosulfate activation: Upgrading framework stability and performance</title><author>Liu, Chao ; Liu, Liyuan ; Tian, Xing ; Wang, Yiping ; Li, Ruoyu ; Zhang, Yuting ; Song, Zilong ; Xu, Bingbing ; Chu, Wei ; Qi, Fei ; Ikhlaq, Amir</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-e275t-c80f981657149c074e0491573531416f62d26d72e0c705b3ba59e1a9d8dbd7bd3</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2019</creationdate><topic>Activation</topic><topic>Biodegradation</topic><topic>Carbon</topic><topic>Carbon nitride</topic><topic>Carbonyls</topic><topic>Catalysis</topic><topic>Catalytic activity</topic><topic>Degradation</topic><topic>Electron paramagnetic resonance</topic><topic>Electron transfer</topic><topic>Electrons</topic><topic>Fe@N-doped graphene-like carbon</topic><topic>Free radicals</topic><topic>g-C3N4</topic><topic>Graphene</topic><topic>Hydroxyl radicals</topic><topic>Intermediates</topic><topic>Iron</topic><topic>Liquid chromatography</topic><topic>Mass spectrometry</topic><topic>Mass spectroscopy</topic><topic>Metal-organic frameworks</topic><topic>metal–organic framework</topic><topic>Morphology</topic><topic>Nanoparticles</topic><topic>Nitrogen</topic><topic>Nitrogen sources</topic><topic>Organic chemistry</topic><topic>Oxidation</topic><topic>Oxidation process</topic><topic>peroxymonosulfate</topic><topic>Phase composition</topic><topic>Quadrupoles</topic><topic>Reactive oxygen species</topic><topic>Singlet oxygen</topic><topic>Sulfamethoxazole</topic><topic>sulfate radical</topic><topic>Sulfates</topic><topic>Superoxide</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Liu, Chao</creatorcontrib><creatorcontrib>Liu, Liyuan</creatorcontrib><creatorcontrib>Tian, Xing</creatorcontrib><creatorcontrib>Wang, Yiping</creatorcontrib><creatorcontrib>Li, Ruoyu</creatorcontrib><creatorcontrib>Zhang, Yuting</creatorcontrib><creatorcontrib>Song, Zilong</creatorcontrib><creatorcontrib>Xu, Bingbing</creatorcontrib><creatorcontrib>Chu, Wei</creatorcontrib><creatorcontrib>Qi, Fei</creatorcontrib><creatorcontrib>Ikhlaq, Amir</creatorcontrib><collection>Engineered Materials Abstracts</collection><collection>Environment Abstracts</collection><collection>Solid State and Superconductivity Abstracts</collection><collection>METADEX</collection><collection>Technology Research Database</collection><collection>Environmental Sciences and Pollution Management</collection><collection>Engineering Research Database</collection><collection>Materials Research Database</collection><collection>Civil Engineering Abstracts</collection><collection>Advanced Technologies Database with Aerospace</collection><collection>Environment Abstracts</collection><jtitle>Applied catalysis. B, Environmental</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Liu, Chao</au><au>Liu, Liyuan</au><au>Tian, Xing</au><au>Wang, Yiping</au><au>Li, Ruoyu</au><au>Zhang, Yuting</au><au>Song, Zilong</au><au>Xu, Bingbing</au><au>Chu, Wei</au><au>Qi, Fei</au><au>Ikhlaq, Amir</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Coupling metal–organic frameworks and g-C3N4 to derive Fe@N-doped graphene-like carbon for peroxymonosulfate activation: Upgrading framework stability and performance</atitle><jtitle>Applied catalysis. B, Environmental</jtitle><date>2019-10-15</date><risdate>2019</risdate><volume>255</volume><spage>1</spage><pages>1-</pages><artnum>117763</artnum><issn>0926-3373</issn><eissn>1873-3883</eissn><abstract>[Display omitted]
•A novel Fe@N-doped graphene-like carbon for activation PMS was synthesized.•Combined NH2 groups and g-C3N4 stabilized the framework morphology.•The degradation pathway of ABEE was first reported in the AOP field.•Fe@N-doped graphene-like carbon/PMS involved multi-oxidative pathways.•Nitrogen species and C = O contributed to the outstanding catalytic activity.
A highly active mediator (Fe@N-doped graphene-like carbon) for peroxymonosulfate (PMS) activation was prepared by employing g-C3N4 assisting NH2-MIL-53(Fe) as the precursor. The addition of combined nitrogen sources (g-C3N4 and NH2 groups) not only stabilized the phase composition and framework morphology, but also improved PMS activation performance significantly. In addition, the introduction of g-C3N4 increased the surface area. Electron paramagnetic resonance (EPR) spectroscopy and radical quenching experiments identified singlet oxygen (1O2), superoxide radicals (O2•−), hydroxyl radicals (•OH), and sulfate radicals (SO4•−) as the reactive oxygen species (ROS) in 4-aminobenzoic acid ethyl ether (ABEE) degradation via a combination process of nonradical and radical processes. The variable chemical valences of iron nanoparticles and quaternary-N, pyrrolic-N, pyridinic-N, and carbonyl (C=O) groups in the support contributed to the outstanding catalytic activity. A possible mechanism for PMS activation by Fe@N-doped graphene-like carbon for ABEE degradation was proposed, which involved sp2 hybridized carbon and electron-rich sp2 sites of the graphitic domain activating PMS via electron transfer. Intermediates were identified using liquid chromatography-quadrupole time-of-flight mass spectrometry (LC-Q-TOF-MS). The degradation pathway of ABEE was reported for the first time in the advanced oxidation process field. Based on intermediate identification of sulfamethoxazole (SMX) degradation, six intermediates were first reported and a new reaction pathway established. This work provides a promising approach to the rational design of high-performance active mediators for environmental remediation.</abstract><cop>Amsterdam</cop><pub>Elsevier B.V</pub><doi>10.1016/j.apcatb.2019.117763</doi></addata></record> |
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subjects | Activation Biodegradation Carbon Carbon nitride Carbonyls Catalysis Catalytic activity Degradation Electron paramagnetic resonance Electron transfer Electrons Fe@N-doped graphene-like carbon Free radicals g-C3N4 Graphene Hydroxyl radicals Intermediates Iron Liquid chromatography Mass spectrometry Mass spectroscopy Metal-organic frameworks metal–organic framework Morphology Nanoparticles Nitrogen Nitrogen sources Organic chemistry Oxidation Oxidation process peroxymonosulfate Phase composition Quadrupoles Reactive oxygen species Singlet oxygen Sulfamethoxazole sulfate radical Sulfates Superoxide |
title | Coupling metal–organic frameworks and g-C3N4 to derive Fe@N-doped graphene-like carbon for peroxymonosulfate activation: Upgrading framework stability and performance |
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