Fe2O3/改性沸石催化剂的制备及其催化臭氧氧化对氯苯酚

doi:10.16085/j.issn.1000-6613.2019-1735

摘要/Abstract

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。

关键词: 沸石, 催化臭氧氧化, 自由基, 对氯苯酚

Abstract:

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 (4CP) 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), X-ray 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 12.776m²/g, 0.042cm³/g and 3.932nm, respectively. The removal efficiencies of 4CP and COD were 87.26% and 48.83% when the initial concentration of 4CP, O₃ concentration, temperature and pH were 100mg/L, 2.6mg/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 4CP. So, the reaction followed the mechanism of hydroxyl radical.

Key words: zeolite, catalytic ozonation, radical, 4-chlorophenol

中图分类号:

X703

张兰河, 郭琳, 李佳宁, 陈子成, 贾艳萍, 李正, 关晓辉. Fe₂O₃/改性沸石催化剂的制备及其催化臭氧氧化对氯苯酚[J]. 化工进展, 2020, 39(8): 3086-3094.

Lanhe ZHANG, Lin GUO, Jianing LI, Zicheng CHEN, Yanping JIA, Zheng LI, Xiaohui GUAN. Preparation of Fe₂O₃/modified natural zeolite catalyst and mechanism study on catalytic ozonation of 4-chlorophenol[J]. Chemical Industry and Engineering Progress, 2020, 39(8): 3086-3094.

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Fe₂O₃/改性沸石催化剂的制备及其催化臭氧氧化对氯苯酚

Preparation of Fe₂O₃/modified natural zeolite catalyst and mechanism study on catalytic ozonation of 4-chlorophenol

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