Catalytic ozonation of bisphenol A by Cu/Mn@γ-Al2O3: Performance evaluation and mechanism insight

Herein, an alumina-based bimetallic catalyst (Cu1Mn7@γ-Al2O3) was synthesized for bisphenol A (BPA) degradation in the catalytic ozonation process. The catalytic ozonation system could degrade 93.9% of BPA within 30 min under the conditions of pH = 7.0, 10 mg L−1 O3 concentration, and 24 g L−1 catal...

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Veröffentlicht in:Journal of environmental management 2024-01, Vol.349, p.119403-119403, Article 119403
Hauptverfasser: Cao, Zhenhua, Long, Yuhan, Yang, Peizhen, Liu, Wenhao, Xue, Cheng, Wu, Weiran, Liu, Dongfang, Huang, Wenli
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container_end_page 119403
container_issue
container_start_page 119403
container_title Journal of environmental management
container_volume 349
creator Cao, Zhenhua
Long, Yuhan
Yang, Peizhen
Liu, Wenhao
Xue, Cheng
Wu, Weiran
Liu, Dongfang
Huang, Wenli
description Herein, an alumina-based bimetallic catalyst (Cu1Mn7@γ-Al2O3) was synthesized for bisphenol A (BPA) degradation in the catalytic ozonation process. The catalytic ozonation system could degrade 93.9% of BPA within 30 min under the conditions of pH = 7.0, 10 mg L−1 O3 concentration, and 24 g L−1 catalyst dosage compared to ozone alone (21.0%). The enhanced BPA degradation efficiency was attributed to the abundant catalytic sites and synergistic effects of Cu and Mn. The results revealed that the synergistic interaction between Cu and Mn effectively accelerated the electron transfer process on the catalyst surface, thus promoting the generation of reactive oxygen species (ROS). Further studies indicated that the BPA degradation in Cu1Mn7@γ-Al2O3/O3 system predominantly followed the ·OH and O2·- oxidation pathway. Based on the density functional theory (DFT) calculations and intermediates detected by LC-MS analysis, two pathways for BPA degradation in the Cu1Mn7@γ-Al2O3/O3 system were proposed. The toxicity estimation illustrated that the toxicity of BPA and its byproducts was effectively reduced in the Cu1Mn7@γ-Al2O3/O3 system. This work provides a new protocol for O3 activation and pollutant elimination through a novel bimetallic catalyst during water purification. [Display omitted] •Cu1Mn7@γ-Al2O3/O3 enhanced BPA degradation up to 93.9% within 30 min.•The Cu–Mn synergistic interaction significantly promoted ROS generation.•·OH and O2·- were the dominant reactive species in BPA degradation.•DFT calculation was employed to speculate the attacking sites of BPA.
doi_str_mv 10.1016/j.jenvman.2023.119403
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The catalytic ozonation system could degrade 93.9% of BPA within 30 min under the conditions of pH = 7.0, 10 mg L−1 O3 concentration, and 24 g L−1 catalyst dosage compared to ozone alone (21.0%). The enhanced BPA degradation efficiency was attributed to the abundant catalytic sites and synergistic effects of Cu and Mn. The results revealed that the synergistic interaction between Cu and Mn effectively accelerated the electron transfer process on the catalyst surface, thus promoting the generation of reactive oxygen species (ROS). Further studies indicated that the BPA degradation in Cu1Mn7@γ-Al2O3/O3 system predominantly followed the ·OH and O2·- oxidation pathway. Based on the density functional theory (DFT) calculations and intermediates detected by LC-MS analysis, two pathways for BPA degradation in the Cu1Mn7@γ-Al2O3/O3 system were proposed. The toxicity estimation illustrated that the toxicity of BPA and its byproducts was effectively reduced in the Cu1Mn7@γ-Al2O3/O3 system. This work provides a new protocol for O3 activation and pollutant elimination through a novel bimetallic catalyst during water purification. [Display omitted] •Cu1Mn7@γ-Al2O3/O3 enhanced BPA degradation up to 93.9% within 30 min.•The Cu–Mn synergistic interaction significantly promoted ROS generation.•·OH and O2·- were the dominant reactive species in BPA degradation.•DFT calculation was employed to speculate the attacking sites of BPA.</description><identifier>ISSN: 0301-4797</identifier><identifier>EISSN: 1095-8630</identifier><identifier>DOI: 10.1016/j.jenvman.2023.119403</identifier><language>eng</language><publisher>Elsevier Ltd</publisher><subject>Bimetallic catalyst ; bisphenol A ; catalysts ; density functional theory ; DFT calculation ; electron transfer ; environmental management ; oxidation ; ozonation ; ozone ; pollutants ; protocols ; reactive oxygen species ; synergism ; Synergistic effect ; Toxicity ; water purification</subject><ispartof>Journal of environmental management, 2024-01, Vol.349, p.119403-119403, Article 119403</ispartof><rights>2023 Elsevier Ltd</rights><lds50>peer_reviewed</lds50><oa>free_for_read</oa><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-c422t-a5c5e010e845cdc9f8bd3f82b56fffdcccbb06d3323eb18fcdc0b2a29d487b803</citedby><cites>FETCH-LOGICAL-c422t-a5c5e010e845cdc9f8bd3f82b56fffdcccbb06d3323eb18fcdc0b2a29d487b803</cites><orcidid>0000-0002-2584-6841</orcidid></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><linktohtml>$$Uhttps://www.sciencedirect.com/science/article/pii/S0301479723021916$$EHTML$$P50$$Gelsevier$$H</linktohtml><link.rule.ids>314,776,780,3537,27901,27902,65306</link.rule.ids></links><search><creatorcontrib>Cao, Zhenhua</creatorcontrib><creatorcontrib>Long, Yuhan</creatorcontrib><creatorcontrib>Yang, Peizhen</creatorcontrib><creatorcontrib>Liu, Wenhao</creatorcontrib><creatorcontrib>Xue, Cheng</creatorcontrib><creatorcontrib>Wu, Weiran</creatorcontrib><creatorcontrib>Liu, Dongfang</creatorcontrib><creatorcontrib>Huang, Wenli</creatorcontrib><title>Catalytic ozonation of bisphenol A by Cu/Mn@γ-Al2O3: Performance evaluation and mechanism insight</title><title>Journal of environmental management</title><description>Herein, an alumina-based bimetallic catalyst (Cu1Mn7@γ-Al2O3) was synthesized for bisphenol A (BPA) degradation in the catalytic ozonation process. The catalytic ozonation system could degrade 93.9% of BPA within 30 min under the conditions of pH = 7.0, 10 mg L−1 O3 concentration, and 24 g L−1 catalyst dosage compared to ozone alone (21.0%). The enhanced BPA degradation efficiency was attributed to the abundant catalytic sites and synergistic effects of Cu and Mn. The results revealed that the synergistic interaction between Cu and Mn effectively accelerated the electron transfer process on the catalyst surface, thus promoting the generation of reactive oxygen species (ROS). Further studies indicated that the BPA degradation in Cu1Mn7@γ-Al2O3/O3 system predominantly followed the ·OH and O2·- oxidation pathway. Based on the density functional theory (DFT) calculations and intermediates detected by LC-MS analysis, two pathways for BPA degradation in the Cu1Mn7@γ-Al2O3/O3 system were proposed. The toxicity estimation illustrated that the toxicity of BPA and its byproducts was effectively reduced in the Cu1Mn7@γ-Al2O3/O3 system. This work provides a new protocol for O3 activation and pollutant elimination through a novel bimetallic catalyst during water purification. [Display omitted] •Cu1Mn7@γ-Al2O3/O3 enhanced BPA degradation up to 93.9% within 30 min.•The Cu–Mn synergistic interaction significantly promoted ROS generation.•·OH and O2·- were the dominant reactive species in BPA degradation.•DFT calculation was employed to speculate the attacking sites of BPA.</description><subject>Bimetallic catalyst</subject><subject>bisphenol A</subject><subject>catalysts</subject><subject>density functional theory</subject><subject>DFT calculation</subject><subject>electron transfer</subject><subject>environmental management</subject><subject>oxidation</subject><subject>ozonation</subject><subject>ozone</subject><subject>pollutants</subject><subject>protocols</subject><subject>reactive oxygen species</subject><subject>synergism</subject><subject>Synergistic effect</subject><subject>Toxicity</subject><subject>water purification</subject><issn>0301-4797</issn><issn>1095-8630</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2024</creationdate><recordtype>article</recordtype><recordid>eNqFkM1OGzEUha2qlZpCH6GSl91MuLbnx8OmRBF_EoguytqyPdfE0Ywd7Emk9LV4D56JQcOe1d185xzdj5BfDJYMWH22XW4xHAYdlhy4WDLWliC-kAWDtipkLeArWYAAVpRN23wnP3LeAoDgrFkQs9aj7o-jtzT-j0GPPgYaHTU-7zYYYk9X1Bzpen92Hy5eX4pVzx_EOf2LycU0TVqkeND9fg7q0NEB7UYHnwfqQ_ZPm_GUfHO6z_jz456Qx6vLf-ub4u7h-na9uitsyflY6MpWCAxQlpXtbOuk6YST3FS1c66z1hoDdScEF2iYdBMDhmvedqVsjARxQn7PvbsUn_eYRzX4bLHvdcC4z0pACSVnohKfolxKUcm6LZsJrWbUpphzQqd2yQ86HRUD9a5fbdWHfvWuX836p9yfOYfTywePSWXrcfLV-YR2VF30nzS8Afsjkjw</recordid><startdate>20240101</startdate><enddate>20240101</enddate><creator>Cao, Zhenhua</creator><creator>Long, Yuhan</creator><creator>Yang, Peizhen</creator><creator>Liu, Wenhao</creator><creator>Xue, Cheng</creator><creator>Wu, Weiran</creator><creator>Liu, Dongfang</creator><creator>Huang, Wenli</creator><general>Elsevier Ltd</general><scope>AAYXX</scope><scope>CITATION</scope><scope>7X8</scope><scope>7S9</scope><scope>L.6</scope><orcidid>https://orcid.org/0000-0002-2584-6841</orcidid></search><sort><creationdate>20240101</creationdate><title>Catalytic ozonation of bisphenol A by Cu/Mn@γ-Al2O3: Performance evaluation and mechanism insight</title><author>Cao, Zhenhua ; Long, Yuhan ; Yang, Peizhen ; Liu, Wenhao ; Xue, Cheng ; Wu, Weiran ; Liu, Dongfang ; Huang, Wenli</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-c422t-a5c5e010e845cdc9f8bd3f82b56fffdcccbb06d3323eb18fcdc0b2a29d487b803</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2024</creationdate><topic>Bimetallic catalyst</topic><topic>bisphenol A</topic><topic>catalysts</topic><topic>density functional theory</topic><topic>DFT calculation</topic><topic>electron transfer</topic><topic>environmental management</topic><topic>oxidation</topic><topic>ozonation</topic><topic>ozone</topic><topic>pollutants</topic><topic>protocols</topic><topic>reactive oxygen species</topic><topic>synergism</topic><topic>Synergistic effect</topic><topic>Toxicity</topic><topic>water purification</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Cao, Zhenhua</creatorcontrib><creatorcontrib>Long, Yuhan</creatorcontrib><creatorcontrib>Yang, Peizhen</creatorcontrib><creatorcontrib>Liu, Wenhao</creatorcontrib><creatorcontrib>Xue, Cheng</creatorcontrib><creatorcontrib>Wu, Weiran</creatorcontrib><creatorcontrib>Liu, Dongfang</creatorcontrib><creatorcontrib>Huang, Wenli</creatorcontrib><collection>CrossRef</collection><collection>MEDLINE - Academic</collection><collection>AGRICOLA</collection><collection>AGRICOLA - Academic</collection><jtitle>Journal of environmental management</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Cao, Zhenhua</au><au>Long, Yuhan</au><au>Yang, Peizhen</au><au>Liu, Wenhao</au><au>Xue, Cheng</au><au>Wu, Weiran</au><au>Liu, Dongfang</au><au>Huang, Wenli</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Catalytic ozonation of bisphenol A by Cu/Mn@γ-Al2O3: Performance evaluation and mechanism insight</atitle><jtitle>Journal of environmental management</jtitle><date>2024-01-01</date><risdate>2024</risdate><volume>349</volume><spage>119403</spage><epage>119403</epage><pages>119403-119403</pages><artnum>119403</artnum><issn>0301-4797</issn><eissn>1095-8630</eissn><abstract>Herein, an alumina-based bimetallic catalyst (Cu1Mn7@γ-Al2O3) was synthesized for bisphenol A (BPA) degradation in the catalytic ozonation process. The catalytic ozonation system could degrade 93.9% of BPA within 30 min under the conditions of pH = 7.0, 10 mg L−1 O3 concentration, and 24 g L−1 catalyst dosage compared to ozone alone (21.0%). The enhanced BPA degradation efficiency was attributed to the abundant catalytic sites and synergistic effects of Cu and Mn. The results revealed that the synergistic interaction between Cu and Mn effectively accelerated the electron transfer process on the catalyst surface, thus promoting the generation of reactive oxygen species (ROS). Further studies indicated that the BPA degradation in Cu1Mn7@γ-Al2O3/O3 system predominantly followed the ·OH and O2·- oxidation pathway. Based on the density functional theory (DFT) calculations and intermediates detected by LC-MS analysis, two pathways for BPA degradation in the Cu1Mn7@γ-Al2O3/O3 system were proposed. The toxicity estimation illustrated that the toxicity of BPA and its byproducts was effectively reduced in the Cu1Mn7@γ-Al2O3/O3 system. This work provides a new protocol for O3 activation and pollutant elimination through a novel bimetallic catalyst during water purification. [Display omitted] •Cu1Mn7@γ-Al2O3/O3 enhanced BPA degradation up to 93.9% within 30 min.•The Cu–Mn synergistic interaction significantly promoted ROS generation.•·OH and O2·- were the dominant reactive species in BPA degradation.•DFT calculation was employed to speculate the attacking sites of BPA.</abstract><pub>Elsevier Ltd</pub><doi>10.1016/j.jenvman.2023.119403</doi><tpages>1</tpages><orcidid>https://orcid.org/0000-0002-2584-6841</orcidid><oa>free_for_read</oa></addata></record>
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subjects Bimetallic catalyst
bisphenol A
catalysts
density functional theory
DFT calculation
electron transfer
environmental management
oxidation
ozonation
ozone
pollutants
protocols
reactive oxygen species
synergism
Synergistic effect
Toxicity
water purification
title Catalytic ozonation of bisphenol A by Cu/Mn@γ-Al2O3: Performance evaluation and mechanism insight
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