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Insights into the mechanism of persulfate activation with biochar composite loaded with Fe for 2,4-dinitrotoluene degradation

Iron in biochar composite loaded with Fe (Fex@biochar) is crucial for persulfate activation. However, the iron dosages-driven mechanism linked to the speciation, electrochemical property, and persulfate activation with Fex@biochar remains ambiguous. We synthesized and characterized a series of Fex@b...

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Published in:Journal of environmental management 2023-09, Vol.341, p.117955-117955, Article 117955
Main Authors: Li, Xiaodong, Cao, Huizhen, Cao, Yuan, Zhao, Yao, Zhang, Wenwen, Shen, Jialun, Sun, Zongquan, Ma, Fujun, Gu, Qingbao
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description Iron in biochar composite loaded with Fe (Fex@biochar) is crucial for persulfate activation. However, the iron dosages-driven mechanism linked to the speciation, electrochemical property, and persulfate activation with Fex@biochar remains ambiguous. We synthesized and characterized a series of Fex@biochar and evaluated its catalytic performance in 2,4-dinitrotoluene removal experiments. With increasing FeCl3 dosage, iron speciation in Fex@biochar changed from γ-Fe2O3 to Fe3O4, and the variation in functional groups was as follows: Fe–O, aliphatic C–O–H, O–H, aliphatic C–H, aromatic CC or CO, and C–N. The electron accepting capacity of Fex@biochar increased as the FeCl3 dosage increased from 10 to 100 mM but decreased at 300 and 500 mM FeCl3. 2,4-dinitrotoluene removal first increased and subsequently decreased, reaching 100% in the persulfate/Fe100@biochar system. The Fe100@biochar also showed good stability and reusability for PS activation, verified by five test cycles. The mechanism analysis indicated that the iron dosage altered the Fe (Ⅲ) content and electron accepting capacity of Fex@biochar during pyrolysis, further controlling persulfate activation and 2,4-dinitrotoluene removal. These results support the preparation of eco-friendly Fex@biochar catalysts. •Sequential response of functional groups to iron dosages was unraveled.•Iron dosage significantly altered electrochemical property of Fex@biochar.•Fex@biochar/persulfate system exhibited an excellent 2,4-DNT removal.•The EAC of Fex@biochar is a key factor affecting its catalytic performance.
doi_str_mv 10.1016/j.jenvman.2023.117955
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However, the iron dosages-driven mechanism linked to the speciation, electrochemical property, and persulfate activation with Fex@biochar remains ambiguous. We synthesized and characterized a series of Fex@biochar and evaluated its catalytic performance in 2,4-dinitrotoluene removal experiments. With increasing FeCl3 dosage, iron speciation in Fex@biochar changed from γ-Fe2O3 to Fe3O4, and the variation in functional groups was as follows: Fe–O, aliphatic C–O–H, O–H, aliphatic C–H, aromatic CC or CO, and C–N. The electron accepting capacity of Fex@biochar increased as the FeCl3 dosage increased from 10 to 100 mM but decreased at 300 and 500 mM FeCl3. 2,4-dinitrotoluene removal first increased and subsequently decreased, reaching 100% in the persulfate/Fe100@biochar system. The Fe100@biochar also showed good stability and reusability for PS activation, verified by five test cycles. The mechanism analysis indicated that the iron dosage altered the Fe (Ⅲ) content and electron accepting capacity of Fex@biochar during pyrolysis, further controlling persulfate activation and 2,4-dinitrotoluene removal. These results support the preparation of eco-friendly Fex@biochar catalysts. •Sequential response of functional groups to iron dosages was unraveled.•Iron dosage significantly altered electrochemical property of Fex@biochar.•Fex@biochar/persulfate system exhibited an excellent 2,4-DNT removal.•The EAC of Fex@biochar is a key factor affecting its catalytic performance.</description><identifier>ISSN: 0301-4797</identifier><identifier>EISSN: 1095-8630</identifier><identifier>DOI: 10.1016/j.jenvman.2023.117955</identifier><identifier>PMID: 37148765</identifier><language>eng</language><publisher>England: Elsevier Ltd</publisher><subject>Catalysis mechanism ; Charcoal - chemistry ; Electron transfer ; Engineered biochar ; Iron - chemistry ; Iron transformation ; Persulfate ; Water Pollutants, Chemical - chemistry</subject><ispartof>Journal of environmental management, 2023-09, Vol.341, p.117955-117955, Article 117955</ispartof><rights>2023 Elsevier Ltd</rights><rights>Copyright © 2023 Elsevier Ltd. 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However, the iron dosages-driven mechanism linked to the speciation, electrochemical property, and persulfate activation with Fex@biochar remains ambiguous. We synthesized and characterized a series of Fex@biochar and evaluated its catalytic performance in 2,4-dinitrotoluene removal experiments. With increasing FeCl3 dosage, iron speciation in Fex@biochar changed from γ-Fe2O3 to Fe3O4, and the variation in functional groups was as follows: Fe–O, aliphatic C–O–H, O–H, aliphatic C–H, aromatic CC or CO, and C–N. The electron accepting capacity of Fex@biochar increased as the FeCl3 dosage increased from 10 to 100 mM but decreased at 300 and 500 mM FeCl3. 2,4-dinitrotoluene removal first increased and subsequently decreased, reaching 100% in the persulfate/Fe100@biochar system. The Fe100@biochar also showed good stability and reusability for PS activation, verified by five test cycles. 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subjects Catalysis mechanism
Charcoal - chemistry
Electron transfer
Engineered biochar
Iron - chemistry
Iron transformation
Persulfate
Water Pollutants, Chemical - chemistry
title Insights into the mechanism of persulfate activation with biochar composite loaded with Fe for 2,4-dinitrotoluene degradation
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