高等学校化学学报2024,Vol.45Issue(9) :117-127.DOI:10.7503/cjcu20240247

Co基碳材料双功能催化剂在电芬顿体系中高效降解环丙沙星

Co Based Carbon Materials as Bifunctional Catalysts for Efficient Degradation of Ciprofloxacin in Electro-Fenton System

王爽 吕月琴 刘星宇 李轶
高等学校化学学报2024,Vol.45Issue(9) :117-127.DOI:10.7503/cjcu20240247

Co基碳材料双功能催化剂在电芬顿体系中高效降解环丙沙星

Co Based Carbon Materials as Bifunctional Catalysts for Efficient Degradation of Ciprofloxacin in Electro-Fenton System

王爽 1吕月琴 1刘星宇 2李轶1
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作者信息

  • 1. 天津大学理学院,天津 300072
  • 2. 天津工业大学环境科学与工程学院,天津 300387
  • 折叠

摘要

抗生素的大量使用导致了环丙沙星(CIP)及其降解中间体在环境中的累积,这对环境和人类健康都具有很大的危害.近年来,使用电芬顿技术降解CIP被认为是一种具有广阔应用前景的水污染控制方法.本文以有机金属骨架ZIF-67作为前驱体,在不同温度煅烧下合成了一系列的Co基碳材料电催化剂(Co-NC-T),并用于CIP的降解.采用扫描电子显微镜、高分辨透射电子显微镜以及X射线衍射仪对所合成催化剂进行了表征.X射线光电子能谱结果显示,性能最佳的Co-NC-900材料含有最高比例的石墨N,这有利于O2通过2e‒还原反应生成H2O2;Co的多重价态[Co(0),Co(Ⅱ)及Co(Ⅲ)]可以促进反应过程中的H2O2转化为多种活性氧物种.Co-NC-900催化剂可以同时促进H2O2的形成和活化,这有利于CIP的降解.猝灭实验和电子自旋共振实验结果表明,体系中主要的活性氧物种依次为·O2‒和·OH.活性氧物种可以协同参与污染物的降解,进而提高CIP的降解效果.CIP的降解性能测试结果显示,在pH=3的条件下,Co-NC-900对CIP的降解效率在120 min可以达到94.5%.

Abstract

The overuse of antibiotics has resulted in a significant accumulation of ciprofloxacin(CIP)and its degradation intermediates in the environment,posing a threat to the environment and human health.In recent years,it has been considered a promising method to use heterogeneous electron-Fenton technology for antibiotic pollution treatment.In this study,we used organic metal framework ZIF-67 as precursor,and prepared a series of Co based carbon electrocatalysts(Co-NC-T)under different temperatures.The successful formation of the catalysts was confirmed by morphology and crystal structure analysis,including scanning electron microscopy,high-resolution transmission electron microscopy and X-ray diffraction patterns.On the one hand,The results of X-ray photoelectron spectroscopy showed that Co-NC-900 contained the highest proportion of graphite N,which was beneficial for O2 to generate H2O2 through 2e‒ reduction reaction.On the other hand,the multiple valence states of Co[Co(0),Co(Ⅱ),Co(Ⅲ)]could promote the conversion of H2O2 into various reactive oxygen species during the reaction.The Co-NC-900 catalyst could simultaneously promote the formation and activation of H2O2,which was beneficial for the degradation of CIP.The quenching experiment and electron spin resonance experiment results indicated that the main reactive oxygen species in the system were·O2‒ and·OH.Reactive oxygen species could synergistically participate in the reaction,thereby improving the degradation efficiency of CIP.Under pH=3,the removal rate of Co-NC-900 to CIP was 94.5%in 120 min.This study provided theoretical guidance for the efficient degradation of CIP in wastewater.

关键词

电芬顿/环丙沙星/ZIF-67/Co基碳材料/活性氧物种

Key words

Electro-Fenton/Ciprofloxacin(CIP)/ZIF-67/Co based carbon material/Active oxygen species

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基金项目

国家自然科学基金(22376157)

国家自然科学基金(22176140)

出版年

2024
高等学校化学学报
中华人民共和国教育部委托 吉林大学和南开大学

高等学校化学学报

CSTPCDCSCD北大核心
影响因子:1.067
ISSN:0251-0790
参考文献量51
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