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绿色合成 MIL-100(Fe) 衍生物并揭示其结构-活性关系用于 2,4-二氯苯酚的光降解。

Green synthesis of MIL-100(Fe) derivatives and revealing their structure-activity relationship for 2,4-dichlorophenol photodegradation.

机构信息

Faculty of Environmental Science and Engineering, Kunming University of Science and Technology, 650500, Kunming, China; Faculty of Chemical Engineering and Technology, Xinjiang University, 830046, Urumqi, China; College of Chemistry and Environmental Science, Qujing Normal University, 655011, Qujing, China.

Faculty of Environmental Science and Engineering, Kunming University of Science and Technology, 650500, Kunming, China.

出版信息

Chemosphere. 2022 Mar;291(Pt 3):132950. doi: 10.1016/j.chemosphere.2021.132950. Epub 2021 Nov 18.

Abstract

MIL-100(Fe), a kind of iron-based metal-organic framework materials (MOFs), can be synthesized at room temperature or hydrothermal conditions, which are promising precursor materials for preparing photocatalysts to degrade some recalcitrant chlorophenols in industrial wastewater. However, the relationship between the structural characterization of MIL-100(Fe) derivatives and their photodegradation behavior of chlorophenol pollutants is still unclear. Thus, in this work, a porous Z-scheme α-FeO/MIL-100(Fe) composite was successfully fabricated via partial-pyrolysis of MIL-100(Fe) precursor synthesized through green synthesis route, which was further used for degrading high-concentration of 2,4-dichlorophenol under visible-light illumination (λ > 420 nm). The effects of synthesis route and pyrolysis temperature of MIL-100(Fe) on the degradation efficiencies of as-derived materials for 2,4-dichlorophenol were investigated. The structure-activity relationship was illuminated in detail. Otherwise, the influence of several process factors, i.e., initial concentration and pH of the 2,4-dichlorophenol solution, catalyst dosage on the degradation efficiency of 2,4-dichlorophenol has also been performed. The removal efficiency of 2,4-dichlorophenol with the initial concentration of 100 mg L reached up to 87.65% under optimized conditions. Lastly, the possible mechanism was explored based on trapping experiments and some other characterization results. The study in this paper not only exhibited new insight into the modified α-FeO material with high photocatalytic activity but also provided a promising method for treating wastewater containing 2,4-dichlorophenol or other similar organic pollutants.

摘要

MIL-100(Fe),一种基于铁的金属有机骨架材料(MOFs),可以在室温或水热条件下合成,是制备光催化剂的有前途的前体材料,可以降解工业废水中一些难降解的氯苯酚。然而,MIL-100(Fe)衍生物的结构特征与其对氯苯酚污染物的光降解行为之间的关系仍不清楚。因此,在这项工作中,通过部分热解通过绿色合成路线合成的 MIL-100(Fe)前体,成功制备了多孔 Z 型 α-FeO/MIL-100(Fe)复合材料,进一步用于可见光照射下(λ>420nm)降解高浓度 2,4-二氯苯酚。研究了 MIL-100(Fe)的合成路线和热解温度对衍生材料降解 2,4-二氯苯酚效率的影响。详细阐明了结构-活性关系。此外,还研究了一些工艺因素,如 2,4-二氯苯酚溶液的初始浓度和 pH 值、催化剂用量对 2,4-二氯苯酚降解效率的影响。在优化条件下,初始浓度为 100mg/L 的 2,4-二氯苯酚的去除效率达到 87.65%。最后,根据捕获实验和其他一些表征结果探讨了可能的机制。本文的研究不仅为具有高光催化活性的改性α-FeO 材料提供了新的见解,而且为处理含有 2,4-二氯苯酚或其他类似有机污染物的废水提供了一种有前途的方法。

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