CIESC Journal ›› 2022, Vol. 73 ›› Issue (4): 1743-1753.DOI: 10.11949/0438-1157.20211539

• Energy and environmental engineering • Previous Articles     Next Articles

Research of enhanced carbon nanotubes activated peroxymonosulfate by cerium doping

Xue HAN1,2(),Shengwang GAO2(),Guoying WANG1,Xunfeng XIA2   

  1. 1.College of Environmental Science and Engineering, Taiyuan University of Technology, Taiyuan 030024, Shanxi, China
    2.Chinese Research Academy of Environmental Sciences, Beijing 100012, China
  • Received:2021-10-28 Revised:2022-01-04 Online:2022-04-25 Published:2022-04-05
  • Contact: Shengwang GAO

铈掺杂强化碳纳米管活化过一硫酸盐实验研究

韩雪1,2(),高生旺2(),王国英1,夏训峰2   

  1. 1.太原理工大学环境科学与工程学院,山西 太原 030024
    2.中国环境科学研究院,北京 100012
  • 通讯作者: 高生旺
  • 作者简介:韩雪(1996—),女,硕士研究生,2934256424@qq.com
  • 基金资助:
    国家重点研发计划项目(2019YFD1100201)

Abstract:

Efficient and stable CeO2/CNT composites were prepared by impregnation-calcination method. The structure of the material was characterized by means of X-ray diffraction, X-ray photoelectron spectroscopy and Raman spectroscopy, and the degradation performance of sulfisoxazole(SIZ) by activated peroxymonosulfate(PMS) of the composite was studied. The introduction of CeO2 increases the defects content of carbon nanotubes, and the Ce3+/Ce4+ provides active sites for the reaction, which effectively improves the performance of carbon nanotube when activating PMS. The catalyst performance was studied by investigating the effects of CeO2 doping amount, catalysts dosage, PMS dosage and initial pH on the degradation system. The results show that when the dosage of catalysts is 75 mg·L-1, the dosage of PMS is 0.3 mmol·L-1 and the initial pH is 5.36, the removal rate of SIZ can reach more than 90% in 30 min and 100% in 50 min, and the reaction process conforms to the pseudo first-order reaction kinetic model. After 5 cycles, the catalyst can still maintain 77% degradation. Electron paramagnetic resonance experiments indicated that SO4?-, ?OH and 1O2 were produced in the degradation of SIZ. The surface defects of carbon nanotubes may be related to the formation of 1O2. At the same time, the direct electron transfer mediated by carbon nanotubes was existed in the system. The cycle of Ce3+/Ce4+ in the system promotes the activation of PMS.

Key words: CeO2, carbon nanotubes, composites, activation, peroxymonosulfate, sulfisoxazole, degradation

摘要:

采用浸渍-煅烧法制备了高效稳定的CeO2/CNT复合材料。利用X射线衍射、X射线光电子能谱和Raman光谱等手段对材料结构进行表征,并研究了复合材料活化过一硫酸盐(PMS)对磺胺异唑的降解性能。结果表明,在材料投加量为75 mg·L-1、PMS投加量为0.3 mmol·L-1、初始pH为5.36时,30 min降解率可达90%以上,50 min内可完全去除,反应过程符合伪一级反应动力学模型,活化剂使用5次后仍有77%的去除率。电子顺磁共振实验表明,SO4?-、?OH和1O2均参与了反应,碳纳米管表面缺陷可能与1O2的形成有关。CeO2的掺杂提高了碳纳米管中缺陷碳的含量,同时Ce3+/Ce4+为反应提供了更多活性位点,从而有效提升了碳纳米管活化PMS的性能,为铈基碳纳米管复合材料应用于过硫酸盐高级氧化技术提供了借鉴。

关键词: CeO2, 碳纳米管, 复合材料, 活化, 过一硫酸盐, 磺胺唑, 降解

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