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Insight into the roles of HEPES and ethanol in one-pot preparation of ZrO2@Pt catalyst for efficient selective hydrogenation of nitrobenzene

Journal 2024 · IF 13.3 · 发表于 2024 年 7 月 14 日
作者: Yaqi Qu,Hualiang An,Xinqiang Zhao,Yanji Wang
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摘要

High dispersion of active metal is an inevitable requirement to improve the catalytic performance of supported metal catalysts and achieving this goal always requires the support with a large specific surface area. Here we innovatively prepared a ZrO 2 @Pt catalyst using ZrO 2 with a small specific surface area as the core which is coated with highly dispersed Pt nanoclusters (<2 nm). In this process, the surface of ZrO 2 was firstly functionalized to increase the number of hydroxyl group, Pt nanoclusters were formed simultaneously and uniformly coated on the ZrO 2 surface. In this work, much attention was paid to the role of 2-[4-(2-hydroxyethyl)-1-piperazinyl] ethanesulfonic acid (HEPES) and ethanol in the one-pot preparation process. The results showed that HEPES acted as a reductant, while treatment with ethanol promoted both the generation of hydroxyl groups on ZrO 2 surface and the reduction of Pt precursor under mild conditions. As-prepared ZrO 2 @Pt catalyst showed excellent catalytic performance in the selective hydrogenation of nitrobenzene; nitrobenzene was completely converted to aniline with 100 % selectivity at room temperature and 8 bar H 2 pressure within 30 min, and the TOF reached as high as 3304 h −1 . Moreover, ZrO 2 @Pt also exhibited a good reusability and a broad substrate applicability. The results of both DRIFTS analysis and DFT calculation demonstrated that the hydrogenation of nitrobenzene on ZrO 2 @Pt catalyst followed the condensation reaction pathway. Our findings can provide a new approach to obtaining highly dispersed metal nanoparticles on the support with a small specific surface area.

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