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构建三维互连通“陷阱-捕获”β-CDPs/Fe-g-CN 催化剂用于高效过一硫酸盐活化降解磺胺甲恶唑:性能、机制、中间产物和毒性。

Constructing a 3D interconnected "trap-zap" β-CDPs/Fe-g-CN catalyst for efficient sulfamethoxazole degradation via peroxymonosulfate activation: Performance, mechanism, intermediates and toxicity.

机构信息

Key Laboratory of Agro-Forestry Environmental Processes and Ecological Regulation of Hainan Province, School of Ecological and Environmental Sciences, Hainan University, Haikou, 570228, China.

Key Laboratory of Agro-Forestry Environmental Processes and Ecological Regulation of Hainan Province, School of Ecological and Environmental Sciences, Hainan University, Haikou, 570228, China.

出版信息

Chemosphere. 2022 May;294:133780. doi: 10.1016/j.chemosphere.2022.133780. Epub 2022 Jan 29.

DOI:10.1016/j.chemosphere.2022.133780
PMID:35104553
Abstract

A novel and high-efficiency catalyst Fe doped g-CN (Fe-g-CN) composited with β-cyclodextrin polymers (β-CDPs) was synthesized for activating peroxymonosulfate (PMS). The scanning electron microscopy (SEM) and transmission electron microscopy (TEM) results showed that the catalyst was 3D interconnected porous structure. The degradation rate constant of sulfamethoxazole (SMX) in β-CDPs/Fe-g-CN+PMS system was estimated to be 0.132 min, which was 14.7 times and 2.2 times that of g-CN+PMS and Fe-g-CN+PMS system, respectively. In addition, the β-CDPs/Fe-g-CN exhibited superior degradation performance in a wide pH range (3.0-9.0) and good selectivity in the presence of other inorganic anions and natural organics. Radical scavenging, electron paramagnetic resonance (EPR) and electrochemical measurements indicated that O and Fe(V)O were the main active species for SMX degradation in β-CDPs/Fe-g-CN+PMS system. Moreover, β-CDPs accelerated electron transfer between catalyst and PMS and promoted the generation of reactive oxygen species (ROS) during PMS activation. The loading of β-CDPs increased the yields of Fe(V)O and O in the system and limited the leaching of Fe. In addition, the possible degradation pathways of SMX were described based on the intermediates detected by liquid chromatography-mass spectrometry (LC-MS), and the toxicity of the intermediates was also evaluated. This work investigate the role of β-CDPs in PMS activation for the first time and develop a promising material with potential for water treatment.

摘要

一种新型高效催化剂 Fe 掺杂 g-CN(Fe-g-CN)与β-环糊精聚合物(β-CDPs)复合,用于激活过一硫酸盐(PMS)。扫描电子显微镜(SEM)和透射电子显微镜(TEM)结果表明,催化剂为 3D 相互连接的多孔结构。β-CDPs/Fe-g-CN+PMS 体系中磺胺甲恶唑(SMX)的降解速率常数估计为 0.132 min-1,分别是 g-CN+PMS 和 Fe-g-CN+PMS 体系的 14.7 倍和 2.2 倍。此外,β-CDPs/Fe-g-CN 在较宽的 pH 值范围(3.0-9.0)内表现出优异的降解性能,并且在存在其他无机阴离子和天然有机物时有良好的选择性。自由基清除、电子顺磁共振(EPR)和电化学测量表明,O 和 Fe(V)O 是β-CDPs/Fe-g-CN+PMS 体系中 SMX 降解的主要活性物质。此外,β-CDPs 加速了催化剂和 PMS 之间的电子转移,并在 PMS 激活过程中促进了活性氧物质(ROS)的生成。β-CDPs 的负载增加了体系中 Fe(V)O 和 O 的产率,并限制了 Fe 的浸出。此外,根据液相色谱-质谱(LC-MS)检测到的中间产物描述了 SMX 的可能降解途径,并评估了中间产物的毒性。这项工作首次研究了β-CDPs 在 PMS 激活中的作用,并开发了一种具有水处理潜力的有前途的材料。

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