期刊
CHEMICAL ENGINEERING JOURNAL
卷 378, 期 -, 页码 -出版社
ELSEVIER SCIENCE SA
DOI: 10.1016/j.cej.2019.05.031
关键词
Wet impregnation; Cerium oxide; Catalytic ozonation; Ceramic membrane; Advanced oxidation; Reactive oxygen species
资金
- Ministry of Education, Singapore [RG96/16]
- Nanyang Technological University, Singapore
This study investigated the degradation of three micropollutants (MPs), namely bisphenol A (BPA), benzotriazole (BTZ) and clofibric acid (CA) by a novel hybrid catalytic ozonation-membrane filtration process. The catalytic ceramic membranes (CCMs) were fabricated via citrate sol-gel assisted wet impregnation method. The surface morphologies and elemental distributions across the CCMs were characterized by FESEM-EDX and AFM. The characterization results suggested that the metal oxides were successfully impregnated throughout the porous structure of the CCMs. The performance of the CCMs was evaluated by a custom-made Hybrid Oxidation Separation Technology (HOST) system. Results indicated that CeOx-impregnated CCM (Ce-CCM) exhibited higher MPs mineralization ability with a 2.1 mg O-3(aq) mg(-1) TOC removal, as compared to that of MnOx-impregnated CCM (Mn-CCM). The CeOx loading in Ce-CCM could be increased by multiple impregnation cycles, at the expense of decrease in its water permeability. The effect of hydraulic retention time (HRT) towards the hybrid process was further investigated, whereby a higher HRT of 13.7 s was able to achieve up to 38% TOC removal. The quantification of reactive oxygen species (ROS) revealed that the O-3(aq) decomposition and ROS generation were enhanced by Ce-CCM, with 0.14 mu mol HO center dot L-1 and 8.78 mu mol O-2(center dot-) L-1 detected. The intermediate by-products of the hybrid process were detected by LC-MS/MS and the MPs degradation pathways via catalytic ozonation were identified. The mechanism of heterogenous catalytic ozonation by Ce-CCM was proposed, based on the presence of surface hydroxyl groups as catalytic sites and involvement of Ce( III/IV) redox pair for electron transfer facilitation in ROS generation. The CCM pores could act as microreactors for effective MPs mineralization in the hybrid process.
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