Rational fabrication of Ti0.69Zr0.31O2 modified Au-loaded halloysite core-shell catalyst for highly efficient reduction of 4-nitrophenol and dye pollutants
Rational fabrication of Ti0.69Zr0.31O2 modified Au-loaded halloysite core-shell catalyst for highly efficient reduction of 4-nitrophenol and dye pollutants
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DOI：
10.1016/j.colsurfa.2023.132305
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发表时间：
2023-08
期刊：
影响因子：
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通讯作者：
Jiasheng Fang;Qiqi Diao;Ming Chen;Shuo Zhao;Yanliang Li;Kun Wei;Zhenting Huang;Q. Zhuo
中科院分区：
文献类型：
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作者：
Jiasheng Fang;Qiqi Diao;Ming Chen;Shuo Zhao;Yanliang Li;Kun Wei;Zhenting Huang;Q. Zhuo
催化还原法可以还原降解一些剧毒、有害的污染物，将其转化为低毒、易生物降解的有用化工资源，具有环境友好、经济有效、条件温和等优点。本文报道了HNTs-Au@Ti0.69Zr0.31O2hollow管状核壳催化剂的合理制备，用于4-硝基苯酚和偶氮染料污染物的易还原降解。催化剂采用以高岭土纳米管为核心的氨基丙基功能化界面反应策略，氨基静电吸附和原位还原具有良好分散性的超小Au纳米颗粒，溶胶-凝胶沉积ti0.69 zr0.31 o2壳层。得到的HNTs-Au@Ti0.69Zr0.31O2catalyst在还原4-硝基苯酚、亚甲基蓝和甲基橙方面表现出优异的催化性能和Au活性位点的原子利用效率。tio2和zro2在ti0.69 zr0.31 o2壳层内的整合使催化剂的孔隙度增加，并对Au NPs产生了非凡的界面化学效应，提高了表面电子态。层间嵌埋的Au纳米颗粒有效固化，避免了团聚和损失，提高了bh4到Au表面目标污染物的反应电子迁移速率，催化反应速率显著。催化剂组分独特的结构特征和协同增强效应，使其在金纳米颗粒周围的杂化界面处产生了过量的催化活性位点，从而构建了高性能的催化体系，使HNTs-Au@Ti0.69Zr0.31O2catalyst具有显著的催化性能、可重复使用性和结构稳定性。最后提出了反应机理和构效关系。
Catalytic reduction method can reductively degrade some highly toxic and harmful pollutants and transform them into useful chemical resources with low toxicity and easy biodegradability, owning the advantages of environmental friendliness, economic effectiveness and mild conditions. This study reported the rational fabrication of the HNTs-Au@Ti0.69Zr0.31O2hollow tubular core-shell catalyst for facile reductive degradation of aqueous 4-nitrophenol and azo dye pollutants. The catalyst employed the interfacial reaction strategy for aminopropyl-functionalization of halloysite nanotubes as core, amino electrostatic adsorption and in situ redction of ultrasmall Au nanoparticles with good dispersibility, and sol-gel deposition of Ti0.69Zr0.31O2shell. The obtained HNTs-Au@Ti0.69Zr0.31O2catalyst manifested superior catalytic performance and atom utilization efficiency of Au active sites for reduction of 4-nitrophenol, methylene blue and methyl orange in comparison to those control samples. The integration of TiO2and ZrO2within Ti0.69Zr0.31O2shell enriched the porosity of the catalyst, and generated the extraordinary interfacial chemical effect on Au NPs with improved surface electronic state. The interlayer-embedded Au nanoparticles were effectively solidified and avoided from agglomeration and loss, where the reactive electron migration rate from BH4-to target pollutants upon Au surfaces was elevated for prominent catalytic reaction rate. The unique structural characteristics and synergistic enhancement effect of catalyst components created excess catalytic active sites at the hybrid interface surrounded Au nanoparticles due to the strong metal-carrier chemical effect, and contributed to the construction of the high-performance catalytic system, which endowed the HNTs-Au@Ti0.69Zr0.31O2catalyst with remarkable catalytic capability, reusability and structural stability. The reaction mechanism and structure-property relationship were finally proposed.