Fe-SBA-15强化H2O2/O3耦合氧化高浓度苯酚的矿化性能研究
Enhanced Mineralization of High-Concentration Phenol by an Fe-SBA-15-Assisted H2O2/O3 Oxidation Process
DOI: 10.12677/wpt.2026.144022, PDF,    科研立项经费支持
作者: 周杨群*, 狄学梦, 王 勇, 姜乾坤:阜阳师范大学化学与材料工程学院,安徽 阜阳
关键词: Fe-SBA-15;H2O2/O3;催化氧化;苯酚;矿化;Fe-SBA-15; H2O2/O3; Catalytic Oxidation; Phenol; Mineralization
摘要: 为提高高浓度有机污染物在臭氧氧化过程中的深度矿化效率,采用水热共缩合法制备Fe-SBA-15介孔催化材料,并通过X射线衍射(XRD)、扫描电子显微镜(SEM)、N2吸附–脱附和紫外–可见漫反射光谱(UV-vis DRS)对其结构和Fe物种状态进行表征。结果表明,Fe的引入未破坏SBA-15的典型介孔结构,Fe-SBA-15的比表面积、平均孔径和孔容分别达到716 m2/g、6.3 nm和1.12 cm3/g;约250 nm处的特征吸收带支持Fe以高分散骨架型物种存在。以250 mg/L苯酚为模型污染物,考察不同氧化体系的矿化性能。在60 min内,Fe-SBA-15/O3和Fe-SBA-15/H2O2体系的TOC去除率分别仅约10%和16%,H2O2/O3体系约为35%;当Fe-SBA-15与H2O2/O3耦合后,TOC去除率提高至约60%,为无催化剂H2O2/O3体系的约1.7倍。结果表明,Fe-SBA-15对单一O3或H2O2的促进作用有限,但能够显著强化H2O2/O3耦合氧化过程。该增强效应可能与骨架Fe位点促进H2O2/O3界面反应以及提高活性氧物种利用效率有关。本研究为介孔Fe基材料强化peroxone过程处理高有机负荷废水提供了实验依据。
Abstract: Fe-SBA-15 mesoporous material was synthesized by a hydrothermal co-condensation route and characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM), N2 adsorption-desorption, and UV-vis diffuse reflectance spectroscopy (UV-vis DRS). The incorporation of Fe preserved the mesoporous structure of SBA-15, while the Fe-SBA-15 sample exhibited a specific surface area of 716 m2/g, an average pore size of 6.3 nm, and a pore volume of 1.12 cm3/g. A characteristic absorption band around 250 nm supported the presence of highly dispersed framework-like Fe species. Using phenol (250 mg/L) as a model pollutant, the mineralization performances of different oxidation systems were compared. After 60 min, TOC removal was only approximately 10% for Fe-SBA-15/O3 and 16% for Fe-SBA-15/H2O2, whereas the conventional H2O2/ O3 process achieved approximately 35%. In contrast, the coupled Fe-SBA-15/H2O2/O3 system increased TOC removal to approximately 60%, corresponding to about 1.7 times that of H2O2/O₃ without the catalyst. These results indicate that Fe-SBA-15 shows limited promotion toward either O3 or H2O2 alone but markedly enhances the coupled H2O2/O3 oxidation process. The enhanced performance may be associated with the ability of framework Fe sites to facilitate interfacial H2O2/O3 reactions and improve the utilization efficiency of reactive oxygen species. This work provides a simple strategy for strengthening peroxone treatment under high organic loading.
文章引用:周杨群, 狄学梦, 王勇, 姜乾坤. Fe-SBA-15强化H2O2/O3耦合氧化高浓度苯酚的矿化性能研究[J]. 水污染及处理, 2026, 14(4): 209-217. https://doi.org/10.12677/wpt.2026.144022

参考文献

[1] Mahmood, Z., Yuan, Y., Garg, S. and Waite, T.D. (2026) Catalytic versus Pure Ozonation: Insights from Real Wastewater Treatment Performance. Environmental Science & Technology, 60, 4440-4448.
https://doi.org/10.1021/acs.est.5c15666
[2] Guo, Y., Zhao, E.Z., Wang, J., Zhang, X.Y., Huang, H.O., Yu, G., et al. (2020) Comparison of Emerging Contaminant Abatement by Conventional Ozonation, Catalytic Ozonation, O3/H2O2 and Electro-Peroxone Processes. Journal of Hazardous Materials, 389, Article ID: 121829.
https://doi.org/10.1016/j.jhazmat.2019.121829
[3] Wang, J. and Bai, Z. (2017) Fe-Based Catalysts for Heterogeneous Catalytic Ozonation of Emerging Contaminants in Water and Wastewater. Chemical Engineering Journal, 312, 79-98.
https://doi.org/10.1016/j.cej.2016.11.118
[4] Zhao, D.Y., Feng, J.L., Huo, Q.S., Melosh, N., Fredrickson, G.H., Chmelka, B.F., et al. (1998) Triblock Copolymer Syntheses of Mesoporous Silica with Periodic 50 to 300 Angstrom Pores. Science, 279, 548-552.
https://doi.org/10.1126/science.279.5350.548
[5] Verma, P., Kuwahara, Y., Mori, K., Raja, R. and Yamashita, H. (2020) Functionalized Mesoporous SBA-15 Silica: Recent Trends and Catalytic Applications. Nanoscale, 12, 11333-11363.
https://doi.org/10.1039/d0nr00732c
[6] Taguchi, A. and Schüth, F. (2005) Ordered Mesoporous Materials in Catalysis. Microporous and Mesoporous Materials, 77, 1-45.
https://doi.org/10.1016/j.micromeso.2004.06.030
[7] Cornu, C., Bonardet, J.L., Casale, S., Davidson, A., Abramson, S., André, G., et al. (2012) Identification and Location of Iron Species in Fe/SBA-15 Catalysts: Interest for Catalytic Fenton Reactions. The Journal of Physical Chemistry C, 116, 3437-3448.
https://doi.org/10.1021/jp2038625
[8] Li, Y., Feng, Z.C., Lian, Y.X., Sun, K.Q., Zhang, L., Jia, G.Q., et al. (2005) Direct Synthesis of Highly Ordered Fe-SBA-15 Mesoporous Materials under Weak Acidic Conditions. Microporous and Mesoporous Materials, 84, 41-49.
https://doi.org/10.1016/j.micromeso.2005.05.021
[9] Xu, Z.H., Yin, K.X., Zhang, L., Tian, Q.B., Wang, J., Wang, Y.F., et al. (2026) Interfacial Electron Modulation and Molecular Passivation: Suppression Mechanisms of Microplastics on Dual Oxidation Pathways in Peroxone Reaction. Water Research, 301, Article ID: 126022.
https://doi.org/10.1016/j.watres.2026.126022
[10] Li, S.Y., Huang, J., Ye, Z.X., Wang, Y.Z., Li, X.K., Wang, J., et al. (2021) The Mechanism of Metal-H2O2 Complex Immobilized on MCM-48 and Enhanced Electron Transfer for Effective Peroxone Ozonation of Sulfamethazine. Applied Catalysis B: Environmental, 280, Article ID: 119453.
https://doi.org/10.1016/j.apcatb.2020.119453
[11] Staehelin, J. and Hoigne, J. (1982) Decomposition of Ozone in Water: Rate of Initiation by Hydroxide Ions and Hydrogen Peroxide. Environmental Science & Technology, 16, 676-681.
https://doi.org/10.1021/es00104a009
[12] Chen, F., Zhang, Y.S., Bai, C.W., Huang, X.T., Sun, Y.J. and Chen, X.J. (2024) Ozone Meets Peroxides: A Symphony of Hybrid Techniques in Wastewater Treatment. Chemical Engineering Journal, 483, Article ID: 149129.
https://doi.org/10.1016/j.cej.2024.149129
[13] Merényi, G., Lind, J., Naumov, S. and Sonntag, C.V. (2010) Reaction of Ozone with Hydrogen Peroxide (Peroxone Process): A Revision of Current Mechanistic Concepts Based on Thermokinetic and Quantum-Chemical Considerations. Environmental Science & Technology, 44, 3505-3507.
https://doi.org/10.1021/es100277d
[14] Shukla, P., Wang, S., Sun, H., Ang, H. and Tadé, M. (2010) Adsorption and Heterogeneous Advanced Oxidation of Phenolic Contaminants Using Fe Loaded Mesoporous SBA-15 and H2O2. Chemical Engineering Journal, 164, 255-260.
https://doi.org/10.1016/j.cej.2010.08.061
[15] Singh, A. and Majumder, S.K. (2026) Integrated Peroxone Advanced Oxidation for Efficient Treatment of Refractory Organic Pollutants in Petroleum Refinery Wastewater. Journal of Environmental Chemical Engineering, 14, Article ID: 123907.
https://doi.org/10.1016/j.jece.2026.123907
[16] Wang, Y.S., Qiu, W., Yu, Y.B. and Ma, J. (2026) Electron Transfer Drives Hydroxyl Radical Formation in Peroxone Reactions. Environmental Science and Ecotechnology, 31, Article ID: 100704.
https://doi.org/10.1016/j.ese.2026.100704
[17] Chen, W.R., Xie, J.X., Li, X.K. and Li, L.S. (2021) Oxygen Vacancies and Lewis Sites Activating O3/H2O2 at Wide Ph Range via Surface Electron Transfer over CeOx@SiO2 for Nitrobenzene Mineralization. Journal of Hazardous Materials, 406, Article ID: 124766.
https://doi.org/10.1016/j.jhazmat.2020.124766
[18] Zhang, Y.S., Chen, X.J., Huang, X.T., Bai, C.W., Duan, P.J., Zhang, Z.Q., et al. (2025) Enhanced Peroxone Reaction with Amphoteric Oxide Modulation for Efficient Decontamination of Challenging Wastewaters: Comparative Performance, Economic Evaluation, and Pilot-Scale Implementation. Water Research, 274, Article ID: 123058.
https://doi.org/10.1016/j.watres.2024.123058
[19] Yan, H.H., Chen, W.R., Liao, G.Z., Li, X.K., Ma, S.S. and Li, L.S. (2016) Activity Assessment of Direct Synthesized Fe-SBA-15 for Catalytic Ozonation of Oxalic Acid. Separation and Purification Technology, 159, 1-6.
https://doi.org/10.1016/j.seppur.2015.12.055
[20] Chen, W.R., He, H.X., Zou, R.N., Chen, Y.D., Li, X.K., Wang, J., et al. (2021) Unravelling the Facets-Dependent Behavior among H2O2, O3 and Oxygen Vacancies on CeOx and the Promotion of Peroxone Reaction at under Acidic Conditions. Environmental Science: Nano, 8, 3138-3152.
https://doi.org/10.1039/d1en00716e