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纳米Fe3O4/CeO2-H2O2非均相类Fenton体系对3,4-二氯三氟甲苯的降解
引用本文:孙正男,杨琦,纪冬丽,郑琳.纳米Fe3O4/CeO2-H2O2非均相类Fenton体系对3,4-二氯三氟甲苯的降解[J].环境科学,2015,36(6):2154-2160.
作者姓名:孙正男  杨琦  纪冬丽  郑琳
作者单位:中国地质大学 北京 水资源与环境学院,北京水资源与环境工程重点实验室,北京 100083
基金项目:北京市产学研项目(51900265005);国家水体污染控制与治理科技重大专项(2009ZX07207-008,2009ZX07419-002,2009ZX07207-001,2015ZX07406005);中央高校基本科研业务费专项(2652013101,2652013086,2652013087,2652015118,2652015005,2652015006);重点防控重金属汞、铬、铅、镉、砷便携/车载/在线监测仪器开发与应用示范项目(2012YQ060115)
摘    要:以浸渍法制备的新型纳米Fe3O4/Ce O2为催化剂,3,4-二氯三氟甲苯(3,4-DCBTE)为目标污染物,在Fe3O4/Ce O2-H2O2非均相类Fenton体系中对目标污染物的降解进行研究,考察催化剂的催化效果和温度、p H、H2O2投加量等因素对催化剂催化效果的影响.结果表明,以纳米Fe3O4/Ce O2作为催化剂的非均相类Fenton体系对3,4-二氯三氟甲苯的处理效果极佳;随着温度的升高,纳米Fe3O4/Ce O2的催化效果不断提高;在偏酸性环境中,p H越低催化效果越好,p H=2时反应去除效率可达96.67%;随着H2O2投加量的增加,3,4-二氯三氟甲苯的降解效率先提高后降低,投加量为15 mg·L-1时去除效果最好可达99.47%;随着催化剂投加量的增加,同样出现了处理效果先升高后降低的现象,投加量为0.5 g·L-1时催化效果最好可达99.64%.在以纳米Fe3O4/Ce O2为催化剂的非均相类Fenton体系中,3,4-二氯三氟甲苯的降解符合一级反应动力学,反应所需活化能较低只需30.26 k J·mol-1.

关 键 词:纳米Fe3O4/CeO2  影响因素  非均相类  Fenton  体系  3  4-二氯三氟甲苯(3  4-DCBTE)
收稿时间:2014/11/28 0:00:00
修稿时间:2015/1/25 0:00:00

Degradation of 3,4-Dichlorobenzotrifluoride by Fe3O4/CeO2-H2O2 Heterogeneous Fenton-Like Systems
SUN Zheng-nan,YANG Qi,JI Dong-li and ZHENG Lin.Degradation of 3,4-Dichlorobenzotrifluoride by Fe3O4/CeO2-H2O2 Heterogeneous Fenton-Like Systems[J].Chinese Journal of Environmental Science,2015,36(6):2154-2160.
Authors:SUN Zheng-nan  YANG Qi  JI Dong-li and ZHENG Lin
Institution:Key Laboratory of Water Resources and Environmental Engineering, Institute of Water Resources and Environment, China University of Geosciences(Beijing), Beijing 100083, China;Key Laboratory of Water Resources and Environmental Engineering, Institute of Water Resources and Environment, China University of Geosciences(Beijing), Beijing 100083, China;Key Laboratory of Water Resources and Environmental Engineering, Institute of Water Resources and Environment, China University of Geosciences(Beijing), Beijing 100083, China;Key Laboratory of Water Resources and Environmental Engineering, Institute of Water Resources and Environment, China University of Geosciences(Beijing), Beijing 100083, China
Abstract:The 3,4-Dichlorobenzotrifluoride (3,4-DCBTE) was dehalogenated with oxidation treatment by heterogeneous Fenton-like system, using nanoscale Fe3O4/CeO2 as a catalyst. This nanoscale catalyst was prepared by the impregnated method. As a highly active new heterogeneous Fenton-like catalyst, nanoscale Fe3O4/CeO2 not only has the characteristics of the traditional Fenton-like catalyst but also can prevent the secondary pollution which caused by Fe2+. To find the optimum catalytic conditions for nanoscale Fe3O4/CeO2, the influence factors were investigated. The results indicated that the degradation ratio of 3,4-DCBTE was significantly improved by adding nanoscale Fe3O4/CeO2, with the removal ratio reaching 97.76% in 120 minutes and 79.85% in 20 minutes. As the temperature increasing, the catalytic effect of nanoscale Fe3O4/CeO2 catalyst had been constantly improved obviously. As the pH decreased, the degradation ratio of 3,4-DCBTE increased. With the increase of dosage of hydrogen peroxide (H2O2), the degradation efficiency of 3,4-DCBTE initially increased and then decreased, because oxygen (O2) was generated in preferential self-reaction when an excess of (H2O2) was added. The optimum removal efficiency was observed with the dosage of 15 mg·L-1. With the increased amount of catalyst, there was a same trend as dosage of hydrogen peroxide (H2O2). The degradation ratio of 3,4-DCBTE initially increased and then decreased, the optimum amount of catalyst was 0.5 g·L-1. The results also suggested that the reaction process followed the first-order kinetics and the thermodynamic analysis demonstrated that the reaction was only needed low reaction activation energy.
Keywords:nanoscale Fe3O4/CeO2  influence factor  heterogeneous Fenton-like system  3  4-Dichlorobenzotrifluoride (3  4-DCBTE)
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