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水热炭负载钴铁氧体通过过一硫酸盐产生的自由基途径同时降解氯苯和对氯苯胺

Significant roles of surface functional groups and Fe/Co redox reactions on peroxymonosulfate activation by hydrochar-supported cobalt ferrite for simultaneous degradation of monochlorobenzene and p-chloroaniline.

机构信息

Key Laboratory of Soil Environment and Pollution Remediation, Institute of Soil Science, Chinese Academy of Sciences, Nanjing 210008, China; University of Chinese Academy of Sciences, Beijing 100049, China.

Key Laboratory of Soil Environment and Pollution Remediation, Institute of Soil Science, Chinese Academy of Sciences, Nanjing 210008, China; Jiangsu Engineering Laboratory for Soil and Groundwater Remediation of Contaminated Sites, Institute of Soil Science, Chinese Academy of Sciences, Nanjing 210008, China; Lier Chemical Co Ltd, Mianyang 621020, China.

出版信息

J Hazard Mater. 2023 Mar 5;445:130588. doi: 10.1016/j.jhazmat.2022.130588. Epub 2022 Dec 9.

Abstract

CoFeO/hydrochar composites (FeCo@HC) were synthesized via a facile one-step hydrothermal method and utilized to activate peroxymonosulfate (PMS) for simultaneous degradation of monochlorobenzene (MCB) and p-chloroaniline (PCA). Additionally, the effects of humic acid, Cl, HCO, HPO HPO and water matrices were investigated and degradation pathways of MCB and PCA were proposed. The removal efficiencies of MCB and PCA were higher in FeCo@HC140-10/PMS system obtained under hydrothermal temperature of 140 °C than FeCo@HC180-10/PMS and FeCo@HC220-10/PMS systems obtained under higher temperatures. Radical species (i.e., SO, •OH) and nonradical pathways (i.e., O, Fe (IV)/Co (IV) and electron transfer through surface FeCo@HC140-10/PMS* complex) co-occurred in the FeCo@HC140-10/PMS system, while radical and nonradical pathways were dominant in degrading MCB and PCA respectively. The surface functional groups (i.e., C-OH and CO) and Fe/Co redox cycles played crucial roles in the PMS activation. MCB degradation was significantly inhibited in the mixed MCB/PCA solution over that in the single MCB solution, whereas PCA degradation was slightly promoted in the mixed MCB/PCA solution. These findings are significant for the provision of a low-cost and environmentally-benign synthesis of bimetal-hydrochar composites and more detailed understanding of the related mechanisms on PMS activation for simultaneous removal of the mixed contaminants in groundwater.

摘要

CoFeO/水凝胶复合材料(FeCo@HC)通过简便的一步水热法合成,并用于激活过一硫酸盐(PMS)以同时降解单氯苯(MCB)和对氯苯胺(PCA)。此外,还考察了腐殖酸、Cl、HCO、HPO 和 HPO 等共存物质以及水基质的影响,并提出了 MCB 和 PCA 的降解途径。在水热处理温度为 140°C 下获得的 FeCo@HC140-10/PMS 体系中,MCB 和 PCA 的去除效率高于在较高温度下获得的 FeCo@HC180-10/PMS 和 FeCo@HC220-10/PMS 体系。在 FeCo@HC140-10/PMS 体系中,同时存在自由基物种(如 SO、•OH)和非自由基途径(如 O、Fe(IV)/Co(IV)和通过表面 FeCo@HC140-10/PMS*复合物的电子转移),而在降解 MCB 和 PCA 时,自由基和非自由基途径分别占主导地位。表面官能团(如 C-OH 和 CO)和 Fe/Co 氧化还原循环在 PMS 活化中起着关键作用。在混合 MCB/PCA 溶液中,MCB 的降解明显受到抑制,而在混合 MCB/PCA 溶液中,PCA 的降解略有促进。这些发现对于提供一种低成本和环境友好的双金属-水凝胶复合材料的合成以及更详细地了解相关机制,即 PMS 激活用于同时去除地下水中的混合污染物具有重要意义。

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