Au nanoparticles supported on piranha etched halloysite nanotubes for highly efficient heterogeneous catalysis

Au nanoparticles supported on piranha etched halloysite nanotubes for highly efficient heterogeneous catalysis
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DOI:
10.1016/j.apsusc.2021.149100
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发表时间:
2021-04
影响因子:
6.7
通讯作者:
Jiaying Yu;Woldemar Niedenthal;B. Smarsly;M. M. Natile-M.;Yuxing Huang;M. Carraro
Jiaying Yu;Woldemar Niedenthal;B. Smarsly;M. M. Natile-M.;Yuxing Huang;M. Carraro
中科院分区:
材料科学1区
文献类型:
--
作者:
Jiaying Yu;Woldemar Niedenthal;B. Smarsly;M. M. Natile-M.;Yuxing Huang;M. Carraro

文献摘要

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高岭土纳米管(HNTs)可以方便地用作负载催化单元的支架,以实现高效的多相催化过程。在这篇文章中,我们报告了一种简单的策略来制备基于金纳米粒子(NPs)的复合体系,该体系支持食人鱼蚀刻的HNTs。通过FTIR, XPS和氮气物理吸附等手段对纳米体系进行表征,以突出其表面性能和孔隙度。与未处理的参考HNTs相比,蚀刻的HNTs壁上羟基的增加允许接枝两倍量的3-氨基丙基硅烷(5.7 wt%比2.8 wt%),因此,负载15.5 wt%的金NPs。另一方面,氨基与Au NPs的相互作用稳定了带正电的NPs,从而导致了优异的催化活性和稳定性。该纳米杂化物能催化4-硝基苯酚还原为4-氨基苯酚,其动力学速率比参比反应高53%。此外,它可以重复使用8次而不会有明显的活性损失。该支撑体系还证明了其在糖源分子(即糠醛)氧化中的潜力,其转化为呋喃酸的转换频率(TOF)比参比物高25%。
Halloysite nanotubes (HNTs) can be conveniently used as scaffolds to load catalytic units, to enable efficient heterogeneous catalytic processes. In this contribution, we report a facile strategy to prepare a composite system based on Au nanoparticles (NPs) supported on piranha-etched HNTs. The resulting nano-system was characterized by FTIR, XPS and nitrogen physisorption to highlight its surface properties and porosity. Compared to the non-treated reference HNTs, the increase of hydroxyl groups on the etched HNTs walls allowed to graft a double amount of 3-aminopropyl silane (5.7 wt% vs. 2.8 wt%) and, consequently, to load 15.5 wt% more gold NPs. On the other hand, the interaction of the amino groups with Au NPs stabilizes positively charged NPs, thus leading to excellent catalytic activity and stability. The resulting nano-hybrid can catalyse the reduction of 4-nitrophenol to 4-aminophenol with a kinetic rate constant 53% higher than the reference reaction. In addition, it can be reused for 8 times without significant loss of activity. The supported system also demonstrates its potential in the oxidation of a sugar-derived molecule, i.e., furfural, which is converted into furoic acid with turnover frequency (TOF) 25% higher than the reference.