欢迎访问过程工程学报, 今天是

过程工程学报 ›› 2021, Vol. 21 ›› Issue (7): 857-864.DOI: 10.12034/j.issn.1009-606X.220135

• 环境与能源 • 上一篇    

电芬顿体系中铁铈双金属催化剂降解邻苯二甲酸二丁酯研究

郑应俊1(), 孟海玲1,2(), 刘再亮1, 周晗1, 朱俊杰1   

  1. 1.安徽工业大学能源与环境学院,安徽 马鞍山 243002
    2.生物膜法水质净化及利用技术教育部工程研究中心,安徽 马鞍山 243002
  • 收稿日期:2020-04-20 修回日期:2020-08-04 出版日期:2021-07-28 发布日期:2021-07-27
  • 通讯作者: 孟海玲 1766920868@qq.com;menghlahut@163.com
  • 作者简介:郑应俊(1995-),男,安徽省六安市人,硕士研究生,环境工程专业,E-mail: 1766920868@qq.com
    孟海玲,通讯联系人,E-mail: menghlahut@163.com.
  • 基金资助:
    安徽工业大学大学生科研训练计划项目资助;安徽工业大学省级大学生创新创业训练计划项目资助(S201910360323)

Study on the catalytic degradation of dibutyl phthalate by ferric cerium bimetal in electric-Fenton system

Yingjun ZHENG1(), Hailing MENG1,2(), Zailiang LIU1, Han ZHOU1, Junjie ZHU1   

  1. 1.School of Energy and Environment, Anhui University of Technology, Ma′anshan, Anhui 243002, China
    2.Ministry of Education Biofilm Process Water Purification and Utilization Technology Engineering Research Center, Ma′anshan, Anhui 243002, China
  • Received:2020-04-20 Revised:2020-08-04 Online:2021-07-28 Published:2021-07-27
  • Contact: Hailing MENG 1766920868@qq.com;menghlahut@163.com

摘要:

以MCM-41为载体,采用水热-焙烧法制备了Al修饰双金属催化剂Fe-Ce/Al-MCM-41并进行了XRD、BET和FT-IR表征;以水体中的邻苯二甲酸二丁酯(DBP)为处理对象,在铂丝-碳毡电芬顿体系中研究了催化氧化降解DBP的效果和影响因素,探讨了降解机理。结果表明,铁、铈双金属催化剂在电芬顿体系降解邻苯二甲酸二丁酯中具有良好的催化活性,铝离子的加入能够提高催化剂的催化性能;最佳实验条件为pH=3、催化剂投加量0.5 g/L、电流强度I=0.15 A、通氧流量0.2 L/min、反应120 min、初始浓度10 mg/L,此时DBP去除率为97.1%,在酸性或中性条件下去除率稳定在92.1%以上,碱性条件下DBP去除率降低,电流强度和通氧量达到饱和后对DBP降解率影响很小,并且催化剂投加过量会导致催化效果降低。此电芬顿体系中·OH的氧化反应是降解DBP的主要途径。

关键词: 邻苯二甲酸二丁酯, 电芬顿, 双金属催化剂, 降解条件

Abstract:

Dibutyl phthalate as a plasticizer is widely used in all walks of life. As an endocrine interferon, the pollution caused by it cannot be ignored, and it will harm the health of biology and human body. Because it is difficult to degrade effectively in common wastewater treatment processes, it is urgent to find effective treatment methods. As one of the advanced oxidation technologies, electro-Fenton has great advantages in treating refractory wastewater and has made many achievements. But the difficulty of electro-Fenton technology is to find an efficient and reusable catalyst. In this work, an efficient bimetal catalyst for the treatment of dibutyl phthalate in electro-Fenton system was studied. Aluminum modified bimetallic catalyst Fe-Ce/Al-MCM-41, was prepared by hydrothermal-calcination method using MCM-41 as template and characterized by XRD, BET and FT-IR. Taking dibutyl phthalate simulated wastewater as the treatment object, the effects of four different conditions, such as initial pH, catalyst dosage, current intensity and oxygen flux, on the degradation efficiency of Perth-carbon felt electro-Fenton system were discussed, and the best operation conditions were found. The characterization results showed that the loading of metal ions did not change the mesoporous structure of MCM-41, which provided sufficient active sites for the follow-up reaction. Under the best experimental conditions, the removal rate of 10 mg/L DBP was 97.1%, the removal rate under acidic and neutral conditions was more than 92.1%, and the removal rate of DBP was reduced under alkaline conditions. Through the comparative experimental analysis of the degradation mechanism, it was found that the iron and cerium bimetallic catalyst had good catalytic activity for the degradation of dibutyl phthalate in electric-Fenton system. Among them, iron ion and cerium ion participated in the catalytic reaction and had synergistic effect, while aluminum ion did not directly participate in the catalytic reaction, but the addition of aluminum ion can improve the catalytic performance of the catalyst. In addition, carbon felt as a cathode had a certain adsorption effect. The main active substance in the electro-Fenton system for the degradation of DBP was ·OH, degrades the target pollutants by the oxidation of ·OH.