Constructing fast mass-transfer channels with efficient catalytic ozonation activity in 2D manganese dioxide membranes by intercalating Fe/Mn bimetallic MOF  

作　　者：Dandan Zhou Shilong Li Luyi Chai Jian Lu Tianxiang Yu Yuqing Sun Wenheng Jing 

机构地区：[1]State Key Laboratory of Materials-Oriented Chemical Engineering,Nanjing Tech University,Nanjing 210009,China [2]Nanjing Fu Ding New Energy Technology Co.Ltd.,Nanjing 210023,China

出　　处：《Chinese Journal of Chemical Engineering》2024年第10期272-286,共15页中国化学工程学报（英文版）

基　　金：supported by the National Key Research and Development Program(2021YFB3801303);the National Natural Science Foundation of China(22408161,21921006);the Key Research and Development Program of Jiangsu Provincial Department of Science and Technology(BE2022033-3);the State Key Laboratory of Materials-Oriented Chemical Engineering(SKL-MCE-22A03).

摘　　要：Two-dimensional(2D)catalytic ozonation membranes are promising for the treatment of micropollutants in wastewater due to simultaneous ozone-catalyzed degradation and membrane filtration processes.However,it remains challenging for 2D catalytic ozonation membranes to efficiently degrade micropollutants due to low mass-transfer efficiency and poor catalytic activity.Herein,Fe/Mn bimetallic metal-organic framework(MOF)intercalated lamellar MnO_(2) membranes with fast and robust ozone-catalyzed mass-transfer channels were developed on the surface of the hollow fiber ceramic membrane(HFCM)to obtain 2D Fe/Mn-MOF@MnO_(2)-HFCM for efficiently degrading micropollutants in wastewater.The intercalation of Fe/Mn-MOF expanded the interlayer spacing of the MnO_(2) membrane,thereby providing abundant transport channels for rapid passage of water.More notably,the Fe/Mn-MOF provided enriched reactive sites as well as high electron transfer efficiency based on the redox cycling between Mn^(3+)/Mn^(4+) and Fe^(2+)/Fe^(3+),ensuring the effective catalytic oxidative degradation of micropollutants including tetracycline hydrochloride(TCH),methylene blue,and methyl blue.Moreover,the carboxyl groups on the MOF formed covalent bonds(-COO-)with the hydroxyl groups in MnO_(2) between layers,which increased the interaction between MnO_(2) nanosheets to form stable interlayer channels.Specifically,the optimal composite membrane achieved a high removal rate of TCH micropollutant(93.4%),high water treatment capacity(282 L·m^(-2)·h^(-1)·MPa^(-1)),and excellent longterm stability(1200 min).This study provides a simple and easily scalable strategy to construct fast,efficient,and stable 2D catalytic mass-transfer channels for the efficient treatment of micropollutants in wastewater.

关 键 词：Catalytic ozonation Two-dimensional ceramic membranes Fe/Mn bimetallic MOF MICROPOLLUTANTS 

分 类 号：X703[环境科学与工程—环境工程] TQ426[化学工程]