吉林大学学报(理学版) ›› 2023, Vol. 61 ›› Issue (3): 707-716.

• • 上一篇    

水热法制备MnO2活化过硫酸盐降解水中的四环素

杜蕊含1, 尚丹1, 蒋欣1, 王洋2, 康春莉1   

  1. 1. 吉林大学 新能源与环境学院, 长春 130012;
    2. 中国科学院东北地理与农业生态研究所 湿地生态与环境重点实验室, 长春 130102
  • 收稿日期:2022-07-11 出版日期:2023-05-26 发布日期:2023-05-26
  • 通讯作者: 康春莉 E-mail:kangcl@jlu.edu.cn

Preparation of MnO2 Activated  Persulfate by Hydrothermal Method  for Degradation of Tetracycline in Water

DU Ruihan1, SHANG Dan1, JIANG Xin1, WANG Yang2, KANG Chunli1   

  1. 1. College of New Energy and Environment,  Jilin University,  Changchun 130012,  China; 
    2. Key Laboratory of Wetland Ecology and Environment,  Northeast Institute of Geography and Agroecology,  Chinese Academy of Sciences,  Changchun 130102,  China
  • Received:2022-07-11 Online:2023-05-26 Published:2023-05-26

摘要: 基于过硫酸盐的高级氧化技术在抗生素污染治理方面重要的应用价值, 分别以MnSO4,MnCl2和Mn(NO3)2为原料, 采用水热法制备3种MnO2,  并利用X射线衍射仪(XRD)、 扫描电子显微镜(SEM)和X射线光电子能谱(XPS)对制备的MnO2进行表征, 对比分析3种MnO2催化过氧单硫酸盐(peroxymonosulfate,  PMS)去除四环素的效果, 通过猝灭实验研究催化作用的机理. 结果表明: 以MnSO4制备的MnO2具有纳米棒结构, 对PMS表现出最佳催化效果, 60 min内对50 mg/L四环素去除率为56.8%; 催化过程中存在Mn(Ⅳ)/Mn(Ⅲ)循环, SO-4.,.OH和1O2对去除四环素均有贡献; MnO2/PMS体系的pH>7时对四环素具有较高的去除率, 10 mmol/L NO-3和 Cl-对四环素降解效率基本无影响, 10 mmol/L HCO-3可促进四环素降解; 该方法对3种四环素类抗生素去除的大小顺序为金霉素>四环素>土霉素, 可用于抗生素污染的治理. 

关键词: 二氧化锰, 过氧单硫酸盐, 高级氧化, 四环素

Abstract: Advanced oxidation technology based on persulfate had important potential value in treating antibiotic pollution. We  used MnSO4,  MnCl2  and Mn(NO3)2 as raw materials to prepare three kinds of MnO2 by hydrothermal method. The prepared MnO2 was characterized by an X-ray diffractometer (XRD),  scanning electron microscope (SEM)  and X-ray photoelectron spectroscopy (XPS). The effects of three kinds of MnO2  catalysts on the removal of tetracycline (TC)  by peroxymonosulfate (PMS) were compared and analyzed, and  the catalytic mechanism was studied by quenching experiments. The results show that the MnO2 prepared by MnSO4 has a nanorod structure and the best catalytic effect on PMS. The removal rate of 50 mg/L TC is 56.8% within 60 min. There is an Mn(Ⅳ)/Mn(Ⅲ) cycle in the catalytic process,  and SO-4..OH,  and 1O2 all contribute to the removal of TC. The MnO2/PMS system has a high removal rate for  tetracycline when   pH>7,  10 mmol/L NO-3 and Clhave no affect on the  degradation efficiency of TC,  and 10 mmol/L HCO-3  can promote the  degradation of TC. The order of removal  of three tetracycline antibiotics by this method is  chlortetracycline>TC>oxytetracycline,  which  can be used for the treatment of antibiotic pollution.

Key words: manganese bioxide,  , peroxymonosulfate,  , advanced oxidation,  , tetracycline

中图分类号: 

  • X131