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Enhanced degradation of tetrabromobisphenol A by magnetic Fe3O4@ZIF-67 composites as a heterogeneous Fenton-like catalyst
Chemical Engineering Journal ( IF 15.1 ) Pub Date : 2020-11-01 , DOI: 10.1016/j.cej.2020.127539
Mantang Chen , Nan Wang , Xiaobo Wang , Yu Zhou , Lihua Zhu

Magnetic Fe3O4@ZIF-67 composites were prepared, characterized, and used as heterogeneous catalysts to activate peroxymonosulfate (PMS) for the degradation of tetrabromobisphenol A (TBBPA). It was observed that all the added TBBPA (40 mg L−1) was completely degraded in 3 min in the Fe3O4@ZIF-67 (0.1 g L−1) + PMS (0.1 g L−1) system with a pseudo second-order degradation rate constant (k) of 110.3 L g−1 min−1, being nearly 10 times that (11.8 L g−1 min−1) in the ZIF-67 + PMS system and 2000 times that (0.06 L g−1 min−1) in the Fe3O4 + PMS system. The observed synergistic catalysis between Fe3O4 and ZIF-67 in Fe3O4@ZIF-67 enhanced not only the degradation of TBBPA, but also the TOC removal and the release of Br during the degradation of TBBPA. Multiple reactive species including •OH, SO4•− and 1O2 were responsible for the degradation of TBBPA, but 1O2 was the dominant one. The synergistic catalytic mechanism of PMS activation by Fe3O4@ZIF-67 was proposed, which mainly involved the electron donating ability of Fe2+ in Fe3O4 for enhancing the Co3+/Co2+ cycle. Moreover, Fe3O4@ZIF-67 showed good recyclability and could be easily recycled by magnetic separation. This work provides an opportunity to construct highly efficient catalysts with magnetic recycling capability.



中文翻译:

Fe 3 O 4 @ ZIF-67磁性复合材料作为非均相Fenton催化剂增强了四溴双酚A的降解

制备了磁性Fe 3 O 4 @ ZIF-67复合材料,对其进行了表征,并将其用作非均相催化剂来活化过氧单硫酸盐(PMS)以降解四溴双酚A(TBBPA)。观察到在Fe 3 O 4 @ ZIF-67(0.1 g L -1)+ PMS(0.1 g L -1)系统中,所有添加的TBBPA(40 mg L -1)在3分钟内被完全降解。伪二级降解速率常数(k)为110.3 L g -1 min -1,几乎是ZIF-67 + PMS系统中(11.8 L g -1 min -1)的10倍,是(0.06 L g -1Fe 3 O 4 + PMS系统中的min -1)。铁之间所观察到的协同催化3 ö 4中Fe和ZIF-67 3 ö 4 @ ZIF-67增强不仅TBBPA的降解,而且去除TOC和Br的释放- TBBPA的降解期间。包括•OH,SO 4 •-1 O 2在内的多种反应性物质是导致TBBPA降解的原因,而1 O 2是主要的降解物质。Fe 3 O 4激活PMS的协同催化机理提出了@ ZIF-67,其主要涉及Fe 3 O 4中Fe 2+的给电子能力以增强Co 3+ / Co 2+循环。而且,Fe 3 O 4 @ ZIF-67具有良好的可回收性,并且可以通过磁分离容易地回收。这项工作为构建具有磁性回收能力的高效催化剂提供了机会。

更新日期:2020-11-02
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