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通过 TiO@MIL-101(Fe) 激活过硫酸钠:通过界面电荷转移增强类 Fenton 过程。

Activation of sodium persulfate by TiO@MIL-101(Fe): Boosting the Fenton-like process by interfacial charge transfer.

机构信息

College of Chemistry and Environmental Engineering, Shenzhen University, Shenzhen, 518052, People's Republic of China.

College of Chemistry and Environmental Engineering, Shenzhen University, Shenzhen, 518052, People's Republic of China.

出版信息

Chemosphere. 2022 Feb;288(Pt 3):132666. doi: 10.1016/j.chemosphere.2021.132666. Epub 2021 Oct 25.

Abstract

Advanced oxidation processes based on sulfate radicals are considered as a promising approach for environmental remediation. In this study, TiO@MIL-101(Fe) is successfully fabricated by a facile impregnation method and is used for sodium persulfate (SPS) activation. TiO@MIL-101@SPS combines the advantages of photocatalysis and SPS activation, which shows high removal efficiency for nitrobenzene and methyl orange. In addition, the effect of multiple factors, including light source, SPS amount and catalyst amount, on nitrobenzene degradation have been investigated. Results show that the nitrobenzene degradation efficiency is up to 66.53 % while that of TOC removal is 32.21 % under 4-h visible light irradiation with 30 mg catalyst and 1.6 mM SPS. Moreover, LC-MS have been carried out to study the route of nitrobenzene degradation. Besides, ESR analysis reveals that both SO and OH radicals are generated sustainably under visible light irradiation, and more OH radicals can be detected owing to the synergic effect of photocatalysis and SPS activation. Interfacial charge transfer effect provides photoinduced electrons for the Fe/Fe cycle in MIL-101(Fe), which boosts the SPS activation process, resulting in high photocatalytic activity.

摘要

基于硫酸根自由基的高级氧化工艺被认为是一种很有前途的环境修复方法。在本研究中,通过简便的浸渍法成功制备了 TiO@MIL-101(Fe),并将其用于过一硫酸盐(SPS)的活化。TiO@MIL-101@SPS 结合了光催化和 SPS 活化的优点,对硝基苯和甲基橙表现出高去除效率。此外,还研究了多种因素,包括光源、SPS 用量和催化剂用量对硝基苯降解的影响。结果表明,在可见光照射 4 小时、催化剂用量为 30mg 和 SPS 用量为 1.6mM 的条件下,硝基苯的降解效率高达 66.53%,TOC 去除率为 32.21%。此外,还进行了 LC-MS 研究了硝基苯降解的途径。此外,ESR 分析表明,在可见光照射下可持续生成 SO 和 OH 自由基,由于光催化和 SPS 活化的协同作用,可以检测到更多的 OH 自由基。界面电荷转移效应为 MIL-101(Fe)中的 Fe/Fe 循环提供了光诱导电子,从而促进了 SPS 的活化过程,导致了高的光催化活性。

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