pH adjustable MgAl@LDH-coated MOFs-derived Co2.25Mn0.75O4 for SMX degradation in PMS activated system

Sulfate radical-based advanced oxidation processes (SR-AOPs) is considered as one of the most promising technologies for antibiotic pollution. In this study, a core-shell catalyst of cobalt-manganese oxide derived from CoMn-MOFs coating by MgAl-LDH (Co/Mn@LDH) was synthesized for peroxymonosulfate (...

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Veröffentlicht in:Chemosphere (Oxford) 2023-10, Vol.339, p.139672-139672, Article 139672
Hauptverfasser: Su, Chenxin, Zhang, Nizi, Zhu, Xiaobiao, Sun, Zhirong, Hu, Xiang
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Zhang, Nizi
Zhu, Xiaobiao
Sun, Zhirong
Hu, Xiang
description Sulfate radical-based advanced oxidation processes (SR-AOPs) is considered as one of the most promising technologies for antibiotic pollution. In this study, a core-shell catalyst of cobalt-manganese oxide derived from CoMn-MOFs coating by MgAl-LDH (Co/Mn@LDH) was synthesized for peroxymonosulfate (PMS) activation to degrade sulfamethoxazole (SMX). Degradation efficiency of nearly 100% and a mineralization efficiency of 68.3% for SMX were achieved in Co/Mn@LDH/PMS system. Mn species and out shell MgAl-LDH greatly suppressed the cobalt ions leaching, which only 23 μg/L Co ions were detected by ICP after the reaction. SO4·- was identified as dominant reactive species in the system. Furthermore, the possible reactive sites of SMX were predicted by the density functional theory (DFT) calculations. And the intermediates of SMX were detected by LC-MS and the degradation pathway was proposed based on the results above. The ECOSAR results suggested the intermediates of SMX showed a relatively low toxicity compared to SMX, indicating huge potential of utilization of Co/Mn@LDH in SR-AOPs system. [Display omitted] •Core-shell Co/Mn@LDH exhibited an excellent performance on activating PMS.•The outer LDH shell can maintain system pH at neutral during the reaction process.•The Co ions leaching was only 23 μg/L in Co/Mn@LDH/PMS system.•Co/Mn@LDH/PMS/SMX system showed a low risk for environment according to the ECOSAR.
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In this study, a core-shell catalyst of cobalt-manganese oxide derived from CoMn-MOFs coating by MgAl-LDH (Co/Mn@LDH) was synthesized for peroxymonosulfate (PMS) activation to degrade sulfamethoxazole (SMX). Degradation efficiency of nearly 100% and a mineralization efficiency of 68.3% for SMX were achieved in Co/Mn@LDH/PMS system. Mn species and out shell MgAl-LDH greatly suppressed the cobalt ions leaching, which only 23 μg/L Co ions were detected by ICP after the reaction. SO4·- was identified as dominant reactive species in the system. Furthermore, the possible reactive sites of SMX were predicted by the density functional theory (DFT) calculations. And the intermediates of SMX were detected by LC-MS and the degradation pathway was proposed based on the results above. The ECOSAR results suggested the intermediates of SMX showed a relatively low toxicity compared to SMX, indicating huge potential of utilization of Co/Mn@LDH in SR-AOPs system. [Display omitted] •Core-shell Co/Mn@LDH exhibited an excellent performance on activating PMS.•The outer LDH shell can maintain system pH at neutral during the reaction process.•The Co ions leaching was only 23 μg/L in Co/Mn@LDH/PMS system.•Co/Mn@LDH/PMS/SMX system showed a low risk for environment according to the ECOSAR.</description><identifier>ISSN: 0045-6535</identifier><identifier>EISSN: 1879-1298</identifier><identifier>DOI: 10.1016/j.chemosphere.2023.139672</identifier><language>eng</language><publisher>Elsevier Ltd</publisher><subject>Low Co leaching ; Magnesium-aluminum hydrotalcite ; MOF-derived cobalt-manganese oxide ; pH adjustable ; SMX degradation</subject><ispartof>Chemosphere (Oxford), 2023-10, Vol.339, p.139672-139672, Article 139672</ispartof><rights>2023</rights><lds50>peer_reviewed</lds50><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-c269t-1e39c63d26971036a556d67491ae3dd09bf6c851a09a5c4e00416514c11eb1d93</citedby><cites>FETCH-LOGICAL-c269t-1e39c63d26971036a556d67491ae3dd09bf6c851a09a5c4e00416514c11eb1d93</cites><orcidid>0000-0001-6529-0182 ; 0000-0003-4699-7136</orcidid></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><linktohtml>$$Uhttps://dx.doi.org/10.1016/j.chemosphere.2023.139672$$EHTML$$P50$$Gelsevier$$H</linktohtml><link.rule.ids>314,780,784,3550,27924,27925,45995</link.rule.ids></links><search><creatorcontrib>Su, Chenxin</creatorcontrib><creatorcontrib>Zhang, Nizi</creatorcontrib><creatorcontrib>Zhu, Xiaobiao</creatorcontrib><creatorcontrib>Sun, Zhirong</creatorcontrib><creatorcontrib>Hu, Xiang</creatorcontrib><title>pH adjustable MgAl@LDH-coated MOFs-derived Co2.25Mn0.75O4 for SMX degradation in PMS activated system</title><title>Chemosphere (Oxford)</title><description>Sulfate radical-based advanced oxidation processes (SR-AOPs) is considered as one of the most promising technologies for antibiotic pollution. 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In this study, a core-shell catalyst of cobalt-manganese oxide derived from CoMn-MOFs coating by MgAl-LDH (Co/Mn@LDH) was synthesized for peroxymonosulfate (PMS) activation to degrade sulfamethoxazole (SMX). Degradation efficiency of nearly 100% and a mineralization efficiency of 68.3% for SMX were achieved in Co/Mn@LDH/PMS system. Mn species and out shell MgAl-LDH greatly suppressed the cobalt ions leaching, which only 23 μg/L Co ions were detected by ICP after the reaction. SO4·- was identified as dominant reactive species in the system. Furthermore, the possible reactive sites of SMX were predicted by the density functional theory (DFT) calculations. And the intermediates of SMX were detected by LC-MS and the degradation pathway was proposed based on the results above. The ECOSAR results suggested the intermediates of SMX showed a relatively low toxicity compared to SMX, indicating huge potential of utilization of Co/Mn@LDH in SR-AOPs system. [Display omitted] •Core-shell Co/Mn@LDH exhibited an excellent performance on activating PMS.•The outer LDH shell can maintain system pH at neutral during the reaction process.•The Co ions leaching was only 23 μg/L in Co/Mn@LDH/PMS system.•Co/Mn@LDH/PMS/SMX system showed a low risk for environment according to the ECOSAR.</abstract><pub>Elsevier Ltd</pub><doi>10.1016/j.chemosphere.2023.139672</doi><tpages>1</tpages><orcidid>https://orcid.org/0000-0001-6529-0182</orcidid><orcidid>https://orcid.org/0000-0003-4699-7136</orcidid></addata></record>
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subjects Low Co leaching
Magnesium-aluminum hydrotalcite
MOF-derived cobalt-manganese oxide
pH adjustable
SMX degradation
title pH adjustable MgAl@LDH-coated MOFs-derived Co2.25Mn0.75O4 for SMX degradation in PMS activated system
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