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Preparation of FeMn-ZSM-5/MOR composite molecular sieves: combination of adsorption/oxidation and Fenton-like reaction

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Abstract

In this paper, FeMn-ZSM-5/MOR(FeMn-Z/M) catalyst was synthesized through in-situ crystallization and wet impregnation method and used as heterogeneous Fenton-like catalyst for degradation of indigo carmine (IC) in aqueous solution. The catalysts were characterized using XRD, BET, SEM, EDS, FT-IR and XPS techniques. The experimental results showed that Fe and Mn were successfully doped onto the ZSM-5/MOR(Z/M) surface. The combination of ZSM-5 and mordenite (MOR) not only enhanced the adsorption capacity of contaminant, but also had more active sites. Degradation experiments and the valence variations indicated that Fe and Mn had a significant synergistic effect. The results of IC degradation experiments under different conditions showed that the optimum conditions (FeMn mass ratio = 1:2, FeMn-Z/M = 25 mg, H2O2 = 0.5 ml, pH = 3), the degradation rate of IC reaches 99% in 20 min. Reaction analyses showed that catalyst follow a first-order reaction kinetic. The degradation of IC could be divided into two stages: adsorption/oxidation (After adsorption, oxidative degradation begins) and Fenton-like reaction. Free radicals quenching studies analyzed verified that the dominant free radicals within FeMn-Z/M Fenton-like system were hydroxyl radical (·HO) and hydro-peroxy radical (·HO2), ·HO2 was the main free radical in the adsorption/oxidation stage. The possible catalytic mechanism was proposed. Finally, the synthesized FeMn-Z/M catalyst had better performance than other IC removal methods, and had good degradation efficiency and high reusability after multiple runs.

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Acknowledgements

This work was financially supported by the National Natural Science Foundation of China (No. 21371055) and the Open Fund Project of Key Laboratory of Fine Petrochemical Catalysis and Separation of Hunan Province (No. HNPCCS201904).

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Authors and Affiliations

  1. Department of Chemistry and Chemical Engineering, Hunan Institute of Science and Technology, Yueyang, China

    Zizhen Yang, Siya Wang, Ou Chen, Zhengwei Wang, Jundong Xu & Shuqin Zheng

  2. Key Laboratory of Fine Petrochemicals Catalysis and Separation of Hunan Province, Yueyang, China

    Shuqin Zheng

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  1. Zizhen Yang
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Yang, Z., Wang, S., Chen, O. et al. Preparation of FeMn-ZSM-5/MOR composite molecular sieves: combination of adsorption/oxidation and Fenton-like reaction. Res Chem Intermed 48, 4517–4536 (2022). https://doi.org/10.1007/s11164-022-04819-1

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