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一种新型钴基非均相催化剂的结构:以磷酸锰为载体,有效活化过一硫酸盐以促进磺胺类药物的降解

Structure of a novel Co-based heterogeneous catalyst via Mn(PO) as a carrier to efficiently activate peroxymonosulfate for improving degradation of sulfonamides.

作者信息

Li Yuxin, Jiang Zhuo-Rui, Yang Xiaoli, Lan Yeqing, Guo Jing

机构信息

College of Resources and Environmental Sciences, Nanjing Agricultural University, Nanjing, 210095, PR China.

Anhui Conch Cement Co., Ltd., Wuhu, 241011, PR China.

出版信息

Chemosphere. 2023 Jun;325:138337. doi: 10.1016/j.chemosphere.2023.138337. Epub 2023 Mar 10.

Abstract

Effective degradation of sulfonamides (SAs) in water is of global importance for decreasing its pathogenicity and bioaccumulation. In this study, Mn(PO) was used as a carrier to fabricate a novel and high-efficient catalyst with CoO anchored (CoO@Mn(PO)) for the activation of peroxymonosulfate (PMS) to degrade SAs. Surprisingly, the catalyst exhibited superior performance, and nearly 100% of SAs (10 mg L) including sulfamethazine (SMZ), sulfadimethoxine (SDM), sulfamethoxazole (SMX), and sulfisoxazole (SIZ) was degraded by CoO@Mn(PO)-activated PMS within 10 min. A series of characterization of the CoO@Mn(PO) composite were conducted and the main operational parameters of SMZ degradation were investigated. SO, •OH, and O were determined to be the dominating reactive oxygen species (ROS) responsible for the degradation of SMZ. CoO@Mn(PO) also exhibited excellent stability and the removal rate of SMZ still maintained over 99% even in the fifth cycle. The plausible pathways and mechanisms of SMZ degradation in the system of CoO@Mn(PO)/PMS were deduced on the basis of the analyses of LCMS/MS and XPS. This is the first report on high-efficient heterogeneous activating PMS by mooring CoO on Mn(PO) to degrade SAs, which provides us with a strategy to structure novel bimetallic catalysts for PMS activation.

摘要

有效降解水中的磺胺类药物(SAs)对于降低其致病性和生物累积性具有全球重要意义。在本研究中,以Mn(PO)为载体,制备了一种新型高效的负载CoO的催化剂(CoO@Mn(PO)),用于活化过一硫酸盐(PMS)以降解SAs。令人惊讶的是,该催化剂表现出优异的性能,CoO@Mn(PO)活化的PMS在10分钟内可降解近100%的SAs(10 mg L),包括磺胺二甲嘧啶(SMZ)、磺胺二甲氧嘧啶(SDM)、磺胺甲恶唑(SMX)和磺胺异恶唑(SIZ)。对CoO@Mn(PO)复合材料进行了一系列表征,并研究了SMZ降解的主要操作参数。确定SO、•OH和O为负责降解SMZ的主要活性氧物种(ROS)。CoO@Mn(PO)还表现出优异的稳定性,即使在第五个循环中,SMZ的去除率仍保持在99%以上。基于LCMS/MS和XPS分析,推导了CoO@Mn(PO)/PMS体系中SMZ降解的可能途径和机制。这是首次报道通过将CoO锚定在Mn(PO)上高效非均相活化PMS来降解SAs,为我们构建用于PMS活化的新型双金属催化剂提供了一种策略。

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