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通过吸附与光降解协同作用的原位快速微波合成 FeO@MIL-100(Fe) 用于去除水中的双氯芬酸钠。

Rapid in situ microwave synthesis of FeO@MIL-100(Fe) for aqueous diclofenac sodium removal through integrated adsorption and photodegradation.

机构信息

School of Pharmacy, Shenyang Pharmaceutical University, Shenyang, Liaoning Province, 110016, PR China.

School of Pharmaceutical Engineering, Shenyang Pharmaceutical University, Shenyang, Liaoning Province, 110016, PR China.

出版信息

J Hazard Mater. 2019 Jul 5;373:408-416. doi: 10.1016/j.jhazmat.2019.03.102. Epub 2019 Mar 25.

Abstract

Metal-Organic Frameworks (MOFs) are efficient adsorbent and catalyst, however, the prepare of MOFs can be extremely time consuming. The rapid in situ microwave synthesis process offers the possibility of MOFs to a large-scale application. In this study, FeO@MIL-100(Fe) was rapidly prepared via microwave in 30 min using FeO as metal precursor and applied as the adsorbent and photocatalyst to remove diclofenac sodium (DCF) from water. FeO@MIL-100(Fe) exhibited an excellent adsorption effect to DCF with the maximum adsorption capacities of 400 mg/L. The presence of HO could promote the removal of DCF during photocatalytic process. Approximately 99.4% of the DCF was removed in FeO@MIL-100(Fe)/vis/HO system via adsorption removal and consequent photocatalytic degradation. The high efficiency was attributed to the large BET surface area (1244.62 m/g) and abundant iron metal sites (Fe(III) and Fe(II)) of FeO@MIL-100(Fe). The adsorptive, photocatalytic property of FeO@MIL-100(Fe) and the Fenton-like reaction were the main mechanisms for DCF removal. TOC analyzer was served to assess the mineralization of solutions treated by FeO@MIL-100(Fe)/vis/HO in 12 h. High elimination of TOC (87.8%) was observed during the DCF mineralization process. In addition, the major products were illuminated using HPLC-Q-TOF-MS and DCF degradation pathways were also proposed.

摘要

金属-有机骨架(MOFs)是高效的吸附剂和催化剂,但 MOFs 的制备可能非常耗时。快速的原位微波合成过程为 MOFs 的大规模应用提供了可能性。在这项研究中,通过微波在 30 分钟内快速制备了 FeO@MIL-100(Fe),并将其用作吸附剂和光催化剂,从水中去除双氯芬酸钠(DCF)。FeO@MIL-100(Fe)对 DCF 具有优异的吸附效果,最大吸附容量为 400mg/L。HO 的存在可以促进光催化过程中 DCF 的去除。在 FeO@MIL-100(Fe)/vis/HO 体系中,通过吸附去除和随后的光催化降解,约有 99.4%的 DCF 被去除。高去除效率归因于 FeO@MIL-100(Fe)的大 BET 表面积(1244.62m/g)和丰富的铁金属位(Fe(III)和 Fe(II))。FeO@MIL-100(Fe)的吸附、光催化性能和类 Fenton 反应是去除 DCF 的主要机制。TOC 分析仪用于评估 FeO@MIL-100(Fe)/vis/HO 在 12 小时内处理的溶液的矿化程度。在 DCF 矿化过程中观察到 TOC 的高消除率(87.8%)。此外,使用 HPLC-Q-TOF-MS 照亮了主要产物,并提出了 DCF 降解途径。

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