中国环境科学2024,Vol.44Issue(1) :193-201.

HNTs@CeO2-Au@Co3O4催化还原对硝基苯酚和染料污染物

HNTs@CeO2-Au@Co3O4 catalyst for catalytic reduction of 4-nitrophenol and dye pollutants

方嘉声 陈铭 刁琪琪 赵硕 黄振庭 卫昆 卓琼芳
中国环境科学2024,Vol.44Issue(1) :193-201.

HNTs@CeO2-Au@Co3O4催化还原对硝基苯酚和染料污染物

HNTs@CeO2-Au@Co3O4 catalyst for catalytic reduction of 4-nitrophenol and dye pollutants

方嘉声 1陈铭 2刁琪琪 2赵硕 3黄振庭 2卫昆 2卓琼芳1
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作者信息

  • 1. 东莞理工学院生态环境与建筑工程学院,广东东莞 523808;东莞市新污染物重点实验室,广东东莞 523808
  • 2. 东莞理工学院生态环境与建筑工程学院,广东东莞 523808
  • 3. 山东理工大学化学化工学院,山东淄博 255049
  • 折叠

摘要

制备了 HNTs@CeO2-Au@Co3O4核壳中空管状复合催化剂,用于还原降解水体中对硝基苯酚(4-NP)和染料(MB,MO)污染物.采用TEM,SEM,EDS,XRD,N2吸脱附,XPS等方法对催化剂微观结构和物化特征进行表征.结果表明,CeO2和Co3O4作为内外活性层较好地分散固载Au纳米颗粒,通过界面反应构筑于埃洛石纳米管中,形成CeO2/Co3O4叠层结构封装埃洛石载金核壳复合催化剂(HNTs@CeO2-Au@Co3O4).该催化剂分别在3.5,8和3min内可还原去除96%以上的4-NP,MB和MO污染物,其相应的一级反应动力学速率常数(0.856,0.370,1.337min-1)和转换频率(10.99,1.90,2.80min-1)均明显优于 HNTs-Au@Co3O4,HNTs@CeO2-Au 和 HNTs@CeO2@Co3O4 对照材料.HNTs@CeO2-Au@Co3O4 催化剂连续进行 6 次使用后,仍保持较高的4-NP,MB和MO污染物还原转化率(91.2%,87.3%,89.5%)和结构稳定性.独特的CeO2/Co3O4叠层结构特征和复合组分协同增强效应有效促进了高性能催化体系的构建,极大提升了 Au颗粒的催化活性和稳定性,使HNTs@CeO2-Au@Co3O4催化剂呈现较为优异的催化效能和循环使用性能.

Abstract

This paper reported the preparation of HNTs@CeO2-Au@Co3O4 core-shell hollow tubular composite catalyst for the reductive degradation of aqueous p-nitrophenol(4-NP)and dye(MB,MO)pollutants.The microstructure and physicochemical properties of the catalyst were characterized by the means of TEM,SEM,EDS,XRD,N2 adsorption-desorption,XPS,etc.The results showed that CeO2 and Co3O4 were used as internal and external active layers to well disperse and immobilize Au nanoparticles(NPs),which were constructed upon halloysite nanotubes(HNTs)via interfacial reaction.The formed core-shell composite catalyst(HNTs@CeO2-Au@Co3O4)was based on the HNTs carrier encapsulated by the CeO2/Co3O4 laminated structure with Au NPs.The catalyst can reduce over 96%of 4-NP,MB and MO pollutants within 3.5,8 and 3min respectively,in which the corresponding first-order kinetic rate constant(0.856,0.370,1.337min-1)and turnover frequency(10.99,1.90,2.80min-1)were significantly superior to the control materials including HNTs-Au@Co3O4,HNTs@CeO2-Au and HNTs@CeO2@Co3O4.Besides,HNTs@CeO2-Au@Co3O4 catalyst maintained high reduction conversion of 4-NP,MB and MO pollutants and good structural integrity after 6 consecutive uses.The unique CeO2/Co3O4 laminated structural feature and synergistic enhancement effect of composite components effectively promoted the construction of the high-performance catalytic system,greatly improved the catalytic activity and stability of Au NPs,which endowed the HNTs@CeO2-Au@Co3O4 catalyst with remarkable catalytic capability and recycling performance.

关键词

纳米金催化剂/埃洛石/核壳结构/对硝基苯酚/染料污染物/催化还原

Key words

Au nanocatalyst/halloysite/core-shell structure/p-nitrophenol/dye pollutants/catalytic reduction

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基金项目

国家自然科学基金资助项目(22008031)

广东省基础与应用基础研究基金资助项目(2019A1515110426)

广东省基础与应用基础研究基金资助项目(2020A1515110222)

山东省自然科学基金资助项目(ZR2021QB114)

东莞市科技特派员项目(20221800500622)

出版年

2024
中国环境科学
中国环境科学学会

中国环境科学

CSTPCDCSCDCHSSCD北大核心
影响因子:2.174
ISSN:1000-6923
参考文献量36
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