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Enhanced photocatalysis using metal–organic framework MIL-101(Fe) for organophosphate degradation in water

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Metal–organic frameworks (MOFs) are attractive novel classes of porous materials with diverse potentiality and easily tailored structures. It is desirable to evaluate the performance of MOFs as photocatalysts for organic contaminant removal in aqueous matrixes. In this study, iron-based MIL-101(Fe) was synthesized and a photo-Fenton reaction system (multiple wavelength light + MIL-101(Fe) + H2O2) was developed for elimination of tris(2-chloroethyl) phosphate (TCEP). Degradation pattern of TCEP followed an S-shape curve, which included a slow induction period and a rapid radical oxidation process. Transport of reactants into MIL-101(Fe) and the activation of electron transport within Fe–O clusters of MIL-101(Fe) may be the dominant mechanisms in the induction period, while a pseudo-first-order kinetics was observed in the hydroxyl radical oxidation process. Removal efficiencies in these two stages highly depended on the reaction conditions. Irradiation at 420 nm and acid condition were conductive, while high temperature and high [H2O2]:[MIL-101(Fe)] mass ratio accelerated the reaction. Before complete mineralization, eleven degradation products were generated, and the dominant degradation pathways included cleavage, hydroxylation, carbonylation, and carboxylation. Under acid condition (pH = 3), only 1% mass loss was observed after 60-min reaction, but the iron leakage was aggravated when pH increased. Furthermore, this MOF-photo-Fenton system demonstrated a robust performance on TCEP degradation in actual wastewater matrixes under acid condition. Generally, the MOF-photo-Fenton system is a potential technology for elimination of organic pollutants in aqueous solution.

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Funding

This project was supported by the National Natural Science Foundation of China (Grant No. 51778270) and the Fundamental Research Funds for the Central Universities (Grant Nos. 21617448, 17817020).

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Authors and Affiliations

  1. School of Environment, Guangdong Key Laboratory of Environmental Pollution and Health, Jinan University, Guangzhou, 510632, China

    Han Hu, Haixuan Zhang, Yujia Chen & Huase Ou

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  1. Han Hu
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  2. Haixuan Zhang
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  3. Yujia Chen
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  4. Huase Ou
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Correspondence to Huase Ou.

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Hu, H., Zhang, H., Chen, Y. et al. Enhanced photocatalysis using metal–organic framework MIL-101(Fe) for organophosphate degradation in water. Environ Sci Pollut Res 26, 24720–24732 (2019). https://doi.org/10.1007/s11356-019-05649-2

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