Abstract
Heterogeneous Fenton oxidation using traditional catalysts with H2O2 for the degradation of 1,4-dioxane (1,4-DX) still presents challenge. In this study, we explored the potential of Fe-ZSM-5 zeolites (Fe-zeolite) with three Si/Al ratios (25, 100, 300) as heterogeneous Fenton catalysts for the removal of 1,4-DX from aqueous solution. Fe2O3 or ZSM-5 alone provided ineffective in degrading 1,4-DX when combined with H2O2. However, the efficient removal of 1,4-DX using H2O2 was observed when Fe2O3 was loaded on ZSM-5. Notably, the Brønsted acid sites of Fe-zeolite played a crucial role during the degradation of 1,4-DX. Fe-zeolites, in combination with H2O2, effectively removed 1,4-DX via a combination of adsorption and oxidation. Initially, Fe-zeolites demonstrated excellent affinity for 1,4-DX, achieving adsorption equilibrium rapidly in about 10 min, followed by effective catalytic oxidative degradation. Among the Fe-ZSM-5 catalysts, Fe-ZSM-5 (25) exhibited the highest catalytic activity and degraded 1,4-DX the fastest. We identified hydroxyl radicals (·OH) and singlet oxygen (1O2) as the primary reactive oxygen species (ROS) responsible for 1,4-DX degradation, with superoxide anions (HO2·/O2·−) mainly converting into 1O2 and ·OH. The degradation primarily occurred at the Fe-zeolite interface, with the degradation rate constants proportional to the amount of Brønsted acid sites on the Fe-zeolite. Fe-zeolites were effective over a wide working pH range, with alkaline pH conditions favoring 1,4-DX degradation. Overall, our study provides valuable insights into the selection of suitable catalysts for effective removal of 1,4-DX using a heterogeneous Fenton technology.
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Funding
This work was supported by the National Natural Science Foundation of China (41825021, 41877504), Science and Technology Innovation Special Foundation for Carbon Peak and Carbon Neutrality of Jiangsu Province (BK20220004), and the Open Fund of National Engineering Laboratory for Site Remediation Technologies (NELSRT201902).
National Natural Science Foundation of China,41825021,41877504,Yun Liu,Science and Technology Innovation Special Foundation for Carbon Peak and Carbon Neutrality of Jiangsu Province,BK20220004,Yun Liu,the Open Fund of National Engineering Laboratory for Site Remediation Technologies,NELSRT201902,Yun Liu
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Kun Tian: conceptualization, methodology, investigation, data curation, and writing original draft. Jie Pan: conceptualization, methodology, investigation, data curation, and writing original draft. Yun Liu: supervision, conceptualization, methodology, data curation and data analysis, writing-reviewed & editing, and resources. Ping Wang: reviewed and edited the manuscript. Ming Zhong: methodology, investigation, data curation. Yuanhua Dong: reviewed and edited the manuscript. Meng Wang: supervision, conceptualization, methodology, reviewed and edited the manuscript.
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Tian, K., Pan, J., Liu, Y. et al. Fe-ZSM-5 zeolite catalyst for heterogeneous Fenton oxidation of 1,4-dioxane: effect of Si/Al ratios and contributions of reactive oxygen species. Environ Sci Pollut Res 31, 19738–19752 (2024). https://doi.org/10.1007/s11356-024-32287-0
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DOI: https://doi.org/10.1007/s11356-024-32287-0