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Zr-TUD-1: A lewis acidic, three-dimensional, mesoporous, zirconium-containing catalyst

机译:Zr-TUD-1:刘易斯酸性,三维,介孔,含锆催化剂

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摘要

A three-dimensional, mesoporous, silicate containing zirconium, Zr-TUD-1, was synthesized by a direct hydrothermal treatment method with triethanolamine as a complexing and templating reagent to ensure that zirconium was incorporated as isolated atoms. The mesoporosity of Zr-TUD-1 was confirmed by X-ray diffraction (XRD), N-2 sorption and high-resolution transmission electron micrograph (HR-TEM) studies. The nature and strength of the Lewis acid sites present in Zr-TUD-1 were evaluated by FTIR studies of pyridine adsorption and temperature-programmed desorption of ammonia. FTIR, X-ray photoelectron spectroscopic (XPS) and UV/Vis spectroscopic studies showed that, at Si/Zr ratios of 25 and higher, all the zirconium was tetrahedrally incorporated into the mesoporous framework, while at low Si/Zr ratios, a small part of the zirconium was present as ZrO2 nanoparticles. Zr-TUD-1 is a Lewis acidic, stable and recyclable catalyst for the Meerwein-Ponndorf-Verley (MPV) reaction and for the Prins reaction.
机译:通过直接水热处理方法,以三乙醇胺为络合剂和模板剂,合成了含锆的介孔硅酸盐三维晶体Zr-TUD-1,以确保锆作为分离的原子掺入。通过X射线衍射(XRD),N-2吸附和高分辨率透射电子显微照片(HR-TEM)研究证实了Zr-TUD-1的介孔性。通过FTIR研究吡啶吸附和程序升温氨的脱附,对Zr-TUD-1中存在的路易斯酸位点的性质和强度进行了评估。 FTIR,X射线光电子能谱(XPS)和UV / Vis光谱研究表明,在Si / Zr比为25或更高时,所有锆都以四面体形式掺入中孔骨架,而在低Si / Zr比时,则很小锆的一部分以ZrO2纳米颗粒的形式存在。 Zr-TUD-1是路易斯酸性,稳定且可回收的路易斯催化剂,用于Meerwein-Ponndorf-Verley(MPV)反应和Prins反应。

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