Cu(Fe)/Pd-In/TiO<sub>2</sub>催化剂直接合成过氧化氢及原位活化降解四环素的性能研究

吕志文; 宋文佳; 苏敏; 高嘉诚; 贺嘉熙; 欧阳李科

doi:10.12434/j.issn.2097-2547.20240212

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Cu(Fe)/Pd-In/TiO₂催化剂直接合成过氧化氢及原位活化降解四环素的性能研究

绿色低碳化工技术

- Cu(Fe)/Pd-In/TiO₂催化剂直接合成过氧化氢及原位活化降解四环素的性能研究
- Study on performances of Cu(Fe)/Pd-In/TiO₂ catalysts for direct synthesis to hydrogen peroxide and in situ activation degradation of tetracycline
- 低碳化学与化工 2024, 49(12): 103-111.
- 作者机构：
  
  1.四川大学化学工程学院，四川成都 610207
  2.西南化工研究设计院有限公司，四川成都 610225
- 作者简介：
  
  吕志文（1994—），硕士研究生，研究方向为药物制剂工程，E-mail：2221486267@qq.com。
  欧阳李科（1987—），博士，副教授，研究方向为绿色化工、能源与环境催化反应工程，E-mail：Like.ouyang@scu.edu.cn。
- 基金信息：
  
  国家自然科学基金青年基金(22008158);四川省区域创新合作项目(2023YFQ0086)
- DOI：10.12434/j.issn.2097-2547.20240212
  中图分类号： TQ085;TQ426
- 纸质出版日期：2024-12-25，
  
  收稿日期：2024-05-14，
  
  修回日期：2024-05-27，
- 稿件说明：
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吕志文,宋文佳,苏敏等.Cu(Fe)/Pd-In/TiO₂催化剂直接合成过氧化氢及原位活化降解四环素的性能研究[J].低碳化学与化工,2024,49(12):103-111.

LV Zhiwen,SONG Wenjia,SU Min,et al.Study on performances of Cu(Fe)/Pd-In/TiO₂ catalysts for direct synthesis to hydrogen peroxide and in situ activation degradation of tetracycline[J].Low-carbon Chemistry and Chemical Engineering,2024,49(12):103-111.
吕志文,宋文佳,苏敏等.Cu(Fe)/Pd-In/TiO₂催化剂直接合成过氧化氢及原位活化降解四环素的性能研究[J].低碳化学与化工,2024,49(12):103-111. DOI： 10.12434/j.issn.2097-2547.20240212.

LV Zhiwen,SONG Wenjia,SU Min,et al.Study on performances of Cu(Fe)/Pd-In/TiO₂ catalysts for direct synthesis to hydrogen peroxide and in situ activation degradation of tetracycline[J].Low-carbon Chemistry and Chemical Engineering,2024,49(12):103-111. DOI： 10.12434/j.issn.2097-2547.20240212.

摘要

传统均相芬顿工艺处理废水中的四环素存在需要外加H

消耗大量铁离子、pH适用范围窄以及产生大量铁污泥等问题。通过设计

Cu(Fe)/Pd-In/TiO

系列双功能催化剂，构建了H

直接合成-芬顿（类芬顿）反应耦合体系，实现了H

高效合成及原位活化降解废水中四环素。采用XRD、TEM和EPR等表征技术对催化剂的晶体结构和微观形貌进行了分析，探究了pH值、四环素溶液初始质量浓度、催化剂质量浓度和共存离子等工艺条件对催化剂四环素去除性能的影响。结果表明，在温度为25 ℃、pH值为7、四环素溶液初始质量浓度为30 mg/L、催化剂质量浓度为0.2 g/L和无共存离子的最适宜反应条件下反应90 min后，2Fe/Pd-In/TiO

催化剂的四环素去除率最高（88.1%）；在上述条件下，pH值为3时，1Cu/Pd-In/TiO

催化剂的四环素去除率最高（80.3%）。

Fe/Pd-In/TiO

催化剂的四环素去除能力整体强于

Cu/Pd-In/TiO

催化剂，这主要是由于Fe在催化剂表面分散更加均匀，且催化剂粒径相对更小。自由基捕获实验和EPR分析结果表明，·O

https://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=71247571&type=

3.89466691

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1.10066664

和·OH为氧化降解四环素的主要活性氧物种，其中·O

https://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=71247563&type=

3.89466691

https://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=71247573&type=

1.10066664

起主导作用。

Abstract

The traditional homogeneous Fenton process has some problems

such as requiring the addition of H

to consume a large amount of iron ions

the narrow pH applicatio

n range and the generation of a large amount of iron sludge. Through designing a series of

Cu(Fe)/Pd-In/TiO

bifunctional catalysts

a coupling H

direct synthesis-Fenton (Fenton like) reaction system was constructed to achieve efficient synthesis of H

and in-situ activation degradation of tetracycline in wastewater. XRD

TEM and EPR characterization techniques were used to analyze the crystal structure and microscopic topography of the catalysts

and the effects of pH value

initial mass concentration of tetracycline solution

mass concentration of catalysts and coexisting ions on the tetracycline removal performances of the catalysts were investigated. The results show that the tetracycline removal rate of 2Fe/Pd-In/TiO

catalyst is the highest (88.1%) after 90 min of reaction under the optimal reaction conditions of temperature of 25 ℃

pH value of 7

initial mass concentration of tetracycline solution of 30 mg/L

catalyst mass concentration of 0.2 g/L and no coexisting ions. Under the above conditions

the tetracycline removal rate of the 1Cu/Pd-In/TiO

catalyst is the highest (80.3%) at pH value of 3. The tetracycline removal ability of

Fe/Pd-In/TiO

catalyst is better than that of

Cu/Pd-In/TiO

catalyst. This is mainly due to the more uniform dispersion of Fe on the catalyst surfaces and the relatively small particle size of the catalysts. The results of free radical capture experiment and EPR analysis show that ·O

https://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=71247584&type=

3.64066648

https://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=71247586&type=

1.10066664

and ·OH are the main active oxygen species for oxidative degradation of tetracycline

in which ·O

https://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=71247584&type=

3.64066648

https://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=71247586&type=

1.10066664

plays a leading role.

关键词

四环素去除芬顿反应活性氧物种去除效率

Keywords

tetracycline removalFenton reactionactive oxygen speciesremoval efficiency

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Cu(Fe)/Pd-In/TiO2催化剂直接合成过氧化氢及原位活化降解四环素的性能研究

Study on performances of Cu(Fe)/Pd-In/TiO2 catalysts for direct synthesis to hydrogen peroxide and in situ activation degradation of tetracycline

DOI：10.12434/j.issn.2097-2547.20240212

摘要

Abstract

关键词

Keywords

references

Cu(Fe)/Pd-In/TiO₂催化剂直接合成过氧化氢及原位活化降解四环素的性能研究

Study on performances of Cu(Fe)/Pd-In/TiO₂ catalysts for direct synthesis to hydrogen peroxide and in situ activation degradation of tetracycline