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Degradation of Diclofenac by Loaded Solid Superbase-Activated Persulfate

Alkali-activated persulfate (PS) is widely used in situ in chemical oxidation processes; however, studies on the innovation of the alkali activation process are very limited. Two supported solid superbases, namely KNO(3)/γ-Al(2)O(3) (KAl) and KNO(3)/SBA-15/MgO (KSM), respectively, were prepared and...

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Autores principales: Shi, Jiaqi, Wang, Lei, Gao, Shang, Huang, Jianbo, Yang, Hao, Lu, Hao, Cao, Shaohua
Formato: Online Artículo Texto
Lenguaje:English
Publicado: MDPI 2023
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10531577/
https://www.ncbi.nlm.nih.gov/pubmed/37762616
http://dx.doi.org/10.3390/ijms241814313
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author Shi, Jiaqi
Wang, Lei
Gao, Shang
Huang, Jianbo
Yang, Hao
Lu, Hao
Cao, Shaohua
author_facet Shi, Jiaqi
Wang, Lei
Gao, Shang
Huang, Jianbo
Yang, Hao
Lu, Hao
Cao, Shaohua
author_sort Shi, Jiaqi
collection PubMed
description Alkali-activated persulfate (PS) is widely used in situ in chemical oxidation processes; however, studies on the innovation of the alkali activation process are very limited. Two supported solid superbases, namely KNO(3)/γ-Al(2)O(3) (KAl) and KNO(3)/SBA-15/MgO (KSM), respectively, were prepared and used to activate persulfate to degrade DCF in this work. The results showed that the superbases elevated the solution pH once added and thus could catalyze persulfate to degrade diclofenac efficiently above pH 10.5. The catalytic efficiency of KAl was close to that of sodium hydroxide, and that of KSM was the highest. The mechanism might be that, in addition to raising the solution pH, some potassium existed as K(2)O(2), which had a strong oxidizing effect and was conducive to DCF removal. Hydroxyl, sulfate and superoxide radicals were all found in the reaction system, among which hydroxyl might play the most important role. The material composition ratio, common anion and humic acid all had some influences on the catalytic efficiency. A total of five intermediates were found in the KSM/PS oxidation system, and six oxidation pathways, which were hydroxylation, dehydrogen, dechlorination, dehydration, decarboxylation, and C-N bond breakage, might be involved in the reaction process. Several highly toxic oxidation products that should be paid attention to were also proposed.
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spelling pubmed-105315772023-09-28 Degradation of Diclofenac by Loaded Solid Superbase-Activated Persulfate Shi, Jiaqi Wang, Lei Gao, Shang Huang, Jianbo Yang, Hao Lu, Hao Cao, Shaohua Int J Mol Sci Article Alkali-activated persulfate (PS) is widely used in situ in chemical oxidation processes; however, studies on the innovation of the alkali activation process are very limited. Two supported solid superbases, namely KNO(3)/γ-Al(2)O(3) (KAl) and KNO(3)/SBA-15/MgO (KSM), respectively, were prepared and used to activate persulfate to degrade DCF in this work. The results showed that the superbases elevated the solution pH once added and thus could catalyze persulfate to degrade diclofenac efficiently above pH 10.5. The catalytic efficiency of KAl was close to that of sodium hydroxide, and that of KSM was the highest. The mechanism might be that, in addition to raising the solution pH, some potassium existed as K(2)O(2), which had a strong oxidizing effect and was conducive to DCF removal. Hydroxyl, sulfate and superoxide radicals were all found in the reaction system, among which hydroxyl might play the most important role. The material composition ratio, common anion and humic acid all had some influences on the catalytic efficiency. A total of five intermediates were found in the KSM/PS oxidation system, and six oxidation pathways, which were hydroxylation, dehydrogen, dechlorination, dehydration, decarboxylation, and C-N bond breakage, might be involved in the reaction process. Several highly toxic oxidation products that should be paid attention to were also proposed. MDPI 2023-09-20 /pmc/articles/PMC10531577/ /pubmed/37762616 http://dx.doi.org/10.3390/ijms241814313 Text en © 2023 by the authors. https://creativecommons.org/licenses/by/4.0/Licensee MDPI, Basel, Switzerland. This article is an open access article distributed under the terms and conditions of the Creative Commons Attribution (CC BY) license (https://creativecommons.org/licenses/by/4.0/).
spellingShingle Article
Shi, Jiaqi
Wang, Lei
Gao, Shang
Huang, Jianbo
Yang, Hao
Lu, Hao
Cao, Shaohua
Degradation of Diclofenac by Loaded Solid Superbase-Activated Persulfate
title Degradation of Diclofenac by Loaded Solid Superbase-Activated Persulfate
title_full Degradation of Diclofenac by Loaded Solid Superbase-Activated Persulfate
title_fullStr Degradation of Diclofenac by Loaded Solid Superbase-Activated Persulfate
title_full_unstemmed Degradation of Diclofenac by Loaded Solid Superbase-Activated Persulfate
title_short Degradation of Diclofenac by Loaded Solid Superbase-Activated Persulfate
title_sort degradation of diclofenac by loaded solid superbase-activated persulfate
topic Article
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10531577/
https://www.ncbi.nlm.nih.gov/pubmed/37762616
http://dx.doi.org/10.3390/ijms241814313
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