金属多酚改性光催化膜原位去除水中四环素

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摘要通过层层自组装的方法,以聚偏二氟乙烯(PVDF)膜为基底,制备了金属多酚改性TiO₂光催化膜((TA-Fe³⁺)/TiO₂-PVDF),并搭建了一套原位光催化膜过滤系统以降解水中四环素.采用SEM、EDS、XRD、FTIR和接触角测量仪对光催化膜的结构进行了表征,表征结果均证明了(TA-Fe³⁺)/TiO₂的成功涂覆,且膜表面亲水性增强;选取四环素作为抗生素代表进行降解性能研究,在低剂量(50mg/L)过一硫酸盐(PMS),跨膜压5kPa,可见光光照强度250mW/cm²,运行过程1h中,四环素降解率始终保持80%,四环素平均去除速率7.34g/h,水通量较原始PVDF膜仅下降6%,适用于中性和弱酸性条件,基本不受水体中常见离子和天然有机物的影响;最后,通过活性物种捕获试验和EPR探究了(TA-Fe³⁺)/TiO₂-PVDF膜降解四环素的机理,发现光催化与PMS氧化协同产生的¹O₂、h⁺、O₂^-·和SO₄^·-为主要活性物种,并通过自由基和非自由基途径降解四环素.

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	侯俊
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关键词 ：金属多酚, 催化膜, 原位光催化, PMS, 高效瞬时降解

Abstract：A metal polyphenol-modified TiO₂ photocatalytic membrane ((TA-Fe³⁺)/TiO₂-PVDF) was prepared by a layer-by-layer self-assembly method using polyvinylidene difluoride (PVDF) membranes as the substrate, and an in situ photocatalytic membrane filtration system was constructed to degrade tetracycline in water. The structures of the photocatalytic membranes were characterized by SEM, EDS, XRD, FTIR and contact angle meter, and all the characterization results proved the successful coating of ((TA-Fe³⁺)/TiO₂-PVDF) and the enhanced hydrophilicity of the membrane surfaces; and tetracycline as a representative of the antibiotics was selected for the study of the degradation performance, which was achieved at a low dosage (50mg/L) of peroxydisulfate (PMS), a transmembrane pressure of 5 kPa, and an in situ photocatalytic membrane filtration system to degrade tetracycline in water. 250 mW/cm²visible light intensity, the tetracycline degradation rate was always maintained at 80% during 1h operation, the average removal rate of tetracycline was 7.34g/h, and the water flux only decreased by 6% compared with that of the original PVDF membranes, which is suitable for neutral and weakly acidic conditions, and basically unaffected by common ions in the water column and natural organic matter; finally, the mechanism of tetracycline degradation by (TA-Fe³⁺)/TiO₂-PVDF membranes was investigated by active species capture assay and EPR, and it was found that photocatalysis synergistically with PMS oxidation produced ¹O₂, h+, O₂^-· and SO₄^·- as the main active species, and degraded tetracycline by both the free radical and non-free radical pathways.

Key words： metal polyphenols catalytic membrane in situ photocatalysis permonosulfate efficient instantaneous degradation

收稿日期: 2024-08-24

PACS:

X703.1

基金资助:国家自然科学基金资助项目(U23A2058);中央高校优秀青年团队培育项目(B230201058);江苏省重点研发计划项目(BE2022834)

作者简介: 侯俊(1979-),男,湖北荆门人,教授,博士,主要从事水环境保护与生态修复、环境功能材料等方面研发.发表论文200余篇.20050036@hhu.edu.cn.

引用本文:

侯俊, 徐晓, 杨佳霖, 赵骁, 杨梓俊. 金属多酚改性光催化膜原位去除水中四环素[J]. 中国环境科学, 2025, 45(3): 1260-1271. HOU Jun, XU Xiao, YANG Jia-lin, ZHAO Xiao, YANG Zi-jun. In situ removal of tetracycline from water by metal polyphenol-modified photocatalytic membrane. CHINA ENVIRONMENTAL SCIENCECE, 2025, 45(3): 1260-1271.

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