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使用负载型四氧化三铁磁性纳米粒子作为高效非均相催化剂的类芬顿体系降解 3,4-二氯三氟甲苯。

Degradation of 3,4-dichlorobenzotrifluoride by the Fenton-like process using zirconia-coated magnetite magnetic nanoparticles as an effective heterogeneous catalyst.

机构信息

School of Water Resources and Environment, Beijing Key Laboratory of Water Resources & Environmental Engineering, China University of Geosciences (Beijing), Beijing, 100083, People's Republic of China.

Laboratory of Environmental Technology, INET, and State Key Joint Laboratory of Environment Simulation and Pollution Control, Tsinghua University, Beijing, 100084, People's Republic of China.

出版信息

Environ Sci Pollut Res Int. 2017 Aug;24(22):18575-18584. doi: 10.1007/s11356-017-9552-x. Epub 2017 Jun 24.

Abstract

In this study, zirconia-coated magnetite magnetic nanoparticles (ZrO/FeO MNPs) were prepared, characterized, and used as an effective and reusable heterogeneous catalyst for 3,4-dichlorobenzotrifluoride (3,4-DCBTE) degradation. The catalytic potential of the FeO/ZrO-HO system for the removal of 3,4-DCBTE was tested in comparison with several other systems, and the effects of various operating parameters, including initial solution pH, catalyst addition, HO concentrations, and reaction temperature, were also evaluated with respect to the degradation efficiency of 3,4-DCBTE. Results showed that the FeO/ZrO composite could effectively enhance the oxidation of 3,4-DCBTE by the Fenton-like process, and there might be a synergetic effect in the FeO/ZrO composite. When the mass ratio of FeO and ZrO was 1:1, the FeO/ZrO exhibited the best catalytic activity, and the catalyst-driven Fenton process achieved high removal of 3,4-DCBTE (98.5%) and total organic carbon (TOC) (52.7%) at the operating conditions: pH 3.0, catalyst 2.0 g/L, HO 30 mM, temperature 30 °C, and reaction time 1 h. Furthermore, five successive runs of the Fenton oxidation using the same FeO/ZrO composite resulted in the steady removal of 3,4-DCBTE, further confirming the high stability of the catalyst. In addition, the possible catalytic mechanism and degradation pathways of 3,4-DCBTE were also investigated.

摘要

在这项研究中,制备了氧化锆包覆磁铁矿磁性纳米颗粒(ZrO/FeO MNPs),并将其用作 3,4-二氯三氟甲苯(3,4-DCBTE)降解的有效且可重复使用的多相催化剂。与其他几种体系相比,测试了 FeO/ZrO-HO 体系对去除 3,4-DCBTE 的催化潜力,还评估了各种操作参数(包括初始溶液 pH 值、催化剂添加量、HO 浓度和反应温度)对 3,4-DCBTE 降解效率的影响。结果表明,FeO/ZrO 复合材料可以有效地增强类 Fenton 过程中 3,4-DCBTE 的氧化,并且在 FeO/ZrO 复合材料中可能存在协同效应。当 FeO 和 ZrO 的质量比为 1:1 时,FeO/ZrO 表现出最佳的催化活性,催化剂驱动的 Fenton 过程在操作条件下实现了 3,4-DCBTE 的高去除率(98.5%)和总有机碳(TOC)(52.7%):pH 值 3.0、催化剂 2.0 g/L、HO 30 mM、温度 30°C、反应时间 1 h。此外,在相同的 FeO/ZrO 复合材料上进行五次连续的 Fenton 氧化实验,实现了 3,4-DCBTE 的稳定去除,进一步证实了催化剂的高稳定性。此外,还研究了 3,4-DCBTE 的可能催化机制和降解途径。

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