摘要
为了提高非均相催化臭氧氧化体系处理难降解有机废水的效率,分别以十六烷基三甲基溴化铵(CTMAB)改性的天然沸石和Fe(NO3)3·9H2O溶液作为载体和活性组分前体,采用浸渍法制备Fe2O3/改性天然沸石催化剂(MNZ),利用能谱仪(EDS)、扫描电镜(SEM)、傅里叶变换红外光谱仪(FTIR)、X射线衍射仪(XRD)、X射线光电子能谱仪(XPS)、N2-吸附/脱附等方法分析催化剂的结构和组成,研究其催化臭氧氧化对氯苯酚的效果和催化机制。结果表明:Fe2O3/MNZ催化剂保持了天然沸石的表面结构。Fe2O3均匀负载在沸石表面,属于典型的分子筛结构,比表面积、孔容和孔径分别为12.776m2/g、0.042cm3/g和3.932nm。在对氯苯酚初始浓度为100mg/L、臭氧浓度为2.6mg/L、温度为25℃、pH为7.0±0.2的条件下,对氯苯酚和化学需氧量(COD)去除率分别为87.26%和48.83%。天然沸石与Fe2O3共同促进臭氧分解生成强氧化能力的羟基自由基(·OH),提高了对氯苯酚的去除率,反应体系遵循羟基自由基作用机理。
In order to improve the efficiency of heterogeneous catalytic ozonation of refractory organic wastewater,Fe2O3/modified natural zeolite(MNZ) catalyst was prepared by impregnation method,in which the hexadecyl trimethyl ammonium bromide(CTMAB) modified natural zeolite and Fe(NO3)3·9H2O solution were used as the carrier and a precursor of active components,respectively.The structure and constituent of the catalyst were analyzed and the catalytic ozonation performance of 4-chlorophenol(4 CP)as well as the catalytic mechanisms were studied by using energy dispersive spectrometer(EDS),scanning electron microscope(SEM),Fourier transform infrared spectroscopy(FTIR),X-ray diffraction(XRD),Xray photoelectron spectroscopy(XPS) and N2 adsorption/desorption,respectively.The results showed that the Fe2O3/MNZ catalyst maintained the surface structure of natural zeolite and Fe2O3 was uniformly deposited on the surface of zeolite,which confirmed the catalyst had typical molecular sieve structure.The special surface area,pore volume and pore size of the catalyst were 12.776 m2/g,0.042 cm3/g and 3.932 nm,respectively.The removal efficiencies of 4 CP and COD were 87.26% and 48.83% when the initial concentration of 4 CP,O3 concentration,temperature and pH were 100 mg/L,2.6 mg/L,25℃ and 7.0±0.2,respectively.MNZ and Fe2O3 synthetically promoted the decomposition of ozone into hydroxyl radical(·OH) with high oxidation capacity and thus improved the removal efficiency of 4 CP.So,the reaction followed the mechanism of hydroxyl radical.
作者
张兰河
郭琳
李佳宁
陈子成
贾艳萍
李正
关晓辉
ZHANG Lanhe;GUO Lin;LI Jianing;CHEN Zicheng;JIA Yanping;LI Zheng;GUAN Xiaohui(School of Chemical Engineering,Northeast Electric Power University,Jilin 132012,Jilin,China;Key Laboratory of Songliao Aquatic Environment,Ministry of Education,Jilin Jianzhu University,Changchun 130118,Jilin,China)
出处
《化工进展》
EI
CAS
CSCD
北大核心
2020年第8期3086-3094,共9页
Chemical Industry and Engineering Progress
基金
吉林省科技发展计划(20180201016SF,20180101309JC)。
