研究报告

  • 秦航道,肖榕,成昊,冷森林,吴思展.羧基功能化磁性纳米MnFe2O4非均相Fenton氧化降解水中头孢噻肟钠的研究[J].环境科学学报,2022,42(9):71-80

  • 羧基功能化磁性纳米MnFe2O4非均相Fenton氧化降解水中头孢噻肟钠的研究
  • Heterogeneous Fenton degradation of cefotaxime sodium in water catalyzed by carboxyl-functionalized MnFe2O4 magnetic nanoparticles
  • 基金项目:国家自然科学基金(No.22166031);贵州省科技计划项目(No.黔科合基础-ZK[2021]一般071);贵州省教育厅拔尖人才项目(No.黔教合KY字[2020]042);贵州省教育厅创新团队项目(No.KY[2018]030)
  • 作者
  • 单位
  • 秦航道
  • 铜仁学院材料与化学工程学院,铜仁 554300
  • 肖榕
  • 铜仁职业技术学院,铜仁 554300
  • 成昊
  • 铜仁学院材料与化学工程学院,铜仁 554300
  • 冷森林
  • 铜仁学院材料与化学工程学院,铜仁 554300
  • 吴思展
  • 铜仁学院材料与化学工程学院,铜仁 554300
  • 摘要:成功制备出羧基功能化的MnFe2O4磁性催化剂(MnFe2O4-COOH),采用X射线衍射(XRD)、N2吸附-脱附、振动样品磁强计(VSM)、红外光谱(FT-IR)、透射电子显微镜(TEM)、H2-程序升温还原(TPR)及X-射线光电子能谱(XPS)等技术对其理化性质进行了表征,并通过非均相Fenton氧化降解水中头孢噻肟钠抗生素对MnFe2O4和MnFe2O4-COOH的催化性能进行了考查.结果表明,经过表面修饰之后的MnFe2O4-COOH比MnFe2O4的催化活性高,头孢噻肟钠的去除率可以达到85.5%,TOC的去除率达到58.1%.同时,对溶液pH的影响、Fe的流失、主要的活性物种及羧基修饰基团的作用进行了研究.结果表明,羟基自由基(?OH)是非均相Fenton氧化过程中的主要活性物种,羧基修饰后催化活性的提高主要归因于团聚的抑制、活性组分Fe流失的降低及还原能力的提高.此外,稳定性和重复使用性的研究结果表明,MnFe2O4-COOH经过3次 循环使用后,仍能保持较高的催化活性.
  • Abstract:Carboxyl-functionalized MnFe2O4 (MnFe2O4-COOH) was successfully obtained and well characterized by X-ray diffraction (XRD), N2 adsorption-desorption, vibrating sample magnetometer (VSM), infrared spectrum (FT-IR), transmission electron microscopy (TEM), H2-temperature programmed reduction (H2-TPR) and X-ray photoelectron spectroscopy (XPS). MnFe2O4 and MnFe2O4-COOH were tested as heterogeneous Fenton catalysts for the degradation of cefotaxime sodium antibiotic. After surface functionalization, MnFe2O4-COOH showed superior catalytic activity than that of MnFe2O4, achieving 85.5% of azithromycin removal and 58.1% of TOC removal. Effect of solution pH, iron leaching, primary reactive oxidizing species, and the role of carboxyl surface groups were also investigated. The results showed that ?OH radicals are the main reactive oxidizing species in the heterogeneous Fenton degradation of cefotaxime sodium. The enhanced catalytic activity after carboxyl functionalization may be attributed to the reduction of aggregation, the decrease of iron leaching and the enhancement of reduction capacity. Besides, the study of the stability and reusability of MnFe2O4-COOH indicated it presented a high catalytic performance even after three consecutive runs.

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