Fe_(2)O_(3)/MIL-53（Al）催化类芬顿氧化性能及其作用机制研究  

Study on efficiency and mechanism of Fe_(2)O_(3)/MIL-53（Al） catalytic Fenton-like oxidation

作　　者：任逸 施梦琦 尹越 张炜铭[1,2,3,4] 吕路 柏益尧[1,3,4] REN Yi;SHI Mengqi;YIN Yue;ZHANG Weiming;LV Lu;BAI Yiyao(State Key Laboratory of Pollution Control and Resource Reuse,School of the Environment,Nanjing University,Nanjing 210023;Research Center for Environmental Nanotechnology(ReCENT),Nanjing University,Nanjing 210023;State Environmental Protection Engineering Center for Organic Chemical Wastewater Treatment and Resource Reuse,Nanjing 210046;Nanjing University-International Research Institute of Environmental Industries,Changzhou 213125)

机构地区：[1]污染控制与资源化研究国家重点实验室,南京大学环境学院,南京210023 [2]南京大学环境纳米技术研究中心,南京大学,南京210023 [3]国家环境保护有机化工废水处理与资源化工程技术中心,南京210046 [4]南京大学常高新国际环保产业技术研究院,常州213125

出　　处：《环境科学学报》2019年第8期2508-2516,共9页Acta Scientiae Circumstantiae

基　　金：国家重点研发计划(No.2017YFE0107200);江苏省研究生科研与实践创新计划项目(No.KYCN10-0050)

摘　　要：以MIL-53(Al)和铁盐为原料,采用浸渍-焙烧的方法,制备了Fe2O3/MIL-53(Al)类芬顿催化剂.通过扫描电子显微镜(SEM)、射透射电子显微镜(TEM)、X射线衍射仪(XRD)、傅里叶变换红外光谱仪(FTIR)及X射线光电子能谱仪(XPS),对Fe2O3/MIL-53(Al)、MIL-53(Al)及Fe2O3 3种材料的理化性质进行了表征.以亚甲基蓝为相关材料催化类芬顿反应氧化性能的指示剂,考察了Fe2O3/MIL-53(Al)、MIL-53(Al)及Fe2O3 3种材料催化类芬顿反应的活性.探讨了Fe2O3/MIL-53(Al)催化活性强化的相关作用机制.研究结果表明,Fe2O3/MIL-53(Al)的物化结构特征是以赤铁矿为主的纳米Fe2O3颗粒均匀、离散地分布在MIL-53(Al)之上,纳米Fe2O3颗粒尺寸大多集中在1~5 nm.与未负载纳米Fe2O3相比,其分散性和颗粒尺寸都展现出潜在优越性.Fe2O3/MIL-53(Al)材料催化类芬顿反应降解水溶液中亚甲基蓝的效果是未负载纳米Fe2O3的4.8倍(以反应速率常数计),且TOC去除率亦有明显优势.自由基猝灭实验结果表明Fe2O3/MIL-53(Al)催化类芬顿降解污染物的主要活性氧类物质为羟基自由基.MIL-53(Al)孔结构发达、孔分布均匀及孔尺寸较小且均一等结构特征,导致负载其中的Fe2O3具有孔道负载量大、颗粒分布离散且均匀、颗粒粒径小且均一等特点,从而强化了纳米Fe2O3催化类芬顿反应氧化降解水中污染物的性能.Fe2O3/MIL?53(Al)for Fenton catalysis was prepared by impregnation?calcination with MIL?53(Al)and ferric salt.First of all,the Fe2O3/MIL?53(Al),MIL?53(Al)and Fe2O3 particles were characterized by scanning electron microscope(SEM),transmission electron microscope(TEM),X?ray diffraction(XRD),fourier transform infrared spectrometer(FTIR)and X?ray photoelectron spectroscopy(XPS).To further illustrate the advantage of this new catalyst for Fenton?like catalysis,methylene blue(MB)was chosen as a model pollutant to evaluate the catalytic activity of Fe2O3/MIL?53(Al),MIL?53(Al)and Fe2O3 in Fenton?like process.The results indicated that nano?Fe2O3,mainly consisted of hematite,were distributed on the MIL?53(Al)uniformly and discretely with the particle size of 1~5 nm.Compared with unsupported nano?Fe2O3,Fe2O3/MIL?53(Al)showed potential advantages of dispersity and particle size.The constant rate of Fe2O3/MIL?53(Al)catalyzing Fenton?like for MB removal was 4.8 times higher than that of Fe2O3/H2O2 system as well.Results of Quenching experiments suggest that the main reactive oxygen species for the pollutant degradation is hydroxyl radical.Due to the developed pore structure,uniform pore distribution,small pore size and uniform pore size of MIL?53(Al),supported Fe2O3 particles has more pore loading and better dispersity,as well as smaller and more uniform particle size,which would strengthen Fenton?like performance of nano Fe2O3 for pollutants degradation in aqueous solution.

关 键 词：Fe_(2)O_(3)/MIL-53(Al) 非均相类芬顿反应 废水处理 亚甲基蓝 

分 类 号：X703[环境科学与工程—环境工程]