Novel visible-light activated photocatalytic ultrafiltration membrane for simultaneous separation and degradation of emerging contaminants.

Journal of hazardous materials Pub Date : 2024-10-05 Epub Date: 2024-08-24 DOI:10.1016/j.jhazmat.2024.135634
Ran Li, Zhidong Wei, Peng Li, Yangbo Qiu, Chengyi Wang, Chao Wang, Long-Fei Ren, Jiahui Shao, Yiliang He
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Abstract

Emerging contaminants (ECs) in secondary effluent of wastewater treatment plants (WWTPs) have received increasing attention due to their adverse effects on aquatic ecosystems and human health. Herein, visible-light responsive photocatalyst TM (TiO2 @NH2-MIL-101(Fe)) and resultant photocatalytic ultrafiltration (PUF, PVDF/TM) membrane were prepared to remove 32 typical compounds of antibiotics, 296 compounds of antibiotic resistance genes (ARGs), and their corresponding bacterial hosts. The construction of heterojunction photocatalyst promoted the electron transfer from NH2-MIL-101(Fe) to TiO2 and the formation of N-TiO2, enhancing visible-light (λ ≥ 420 nm) photocatalytic activity. With highly-hydrophilic surface and delicately-regulated pore structure, the initial water permeance of optimal PUF membrane significantly increased to 3912.2 L/m2/h at 1.0 bar. Meanwhile, membrane retention (via adsorption, electrostatic interaction, and steric hindrance) was improved due to the narrowed pore size, highly-negative surface charge and abundant functional groups. Additionally, hydroxyl radical (•OH) was the dominant active reactive oxygen species (ROS) for ECs degradation, and the narrowed pore structure could serve as microreactors to increase ROS concentration and reduce migration distance. Consequently, the removal efficiencies of antibiotics, bacteria and ARGs were 86.5 %, 91.4 % and 91.8 %, respectively. Overall, this novel visible-light-activated PUF membrane expands membrane application, and has great potential in ECs treatment.

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用于同时分离和降解新兴污染物的新型可见光激活光催化超滤膜。
由于对水生生态系统和人类健康的不利影响,污水处理厂(WWTPs)二级出水中的新污染物(ECs)日益受到关注。本文制备了可见光响应光催化剂TM(TiO2 @NH2-MIL-101(Fe))及其光催化超滤膜(PUF,PVDF/TM),用于去除32种典型的抗生素化合物、296种抗生素耐药基因(ARGs)化合物及其相应的细菌宿主。异质结光催化剂的构建促进了 NH2-MIL-101(Fe)向 TiO2 的电子转移和 N-TiO2 的形成,提高了可见光(λ ≥ 420 nm)下的光催化活性。最佳 PUF 膜具有高亲水性表面和微调的孔隙结构,在 1.0 巴的条件下,其初始透水量显著增加到 3912.2 L/m2/h。同时,由于孔径变窄、表面电荷呈高负值和功能基团丰富,膜的截留能力(通过吸附、静电作用和立体阻碍)也得到了改善。此外,羟基自由基(-OH)是降解 ECs 的主要活性氧(ROS),而狭窄的孔隙结构可作为微反应器,增加 ROS 浓度并缩短迁移距离。因此,抗生素、细菌和 ARGs 的去除率分别为 86.5%、91.4% 和 91.8%。总之,这种新型可见光激活 PUF 膜扩大了膜的应用范围,在治疗心血管疾病方面具有巨大潜力。
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