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Assembly of Zr-based coordination polymer over USY zeolite as a highly efficient and robust acid catalyst for one-pot transformation of fructose into 2,5-bis(isopropoxymethyl)furan
Journal of Catalysis ( IF 7.3 ) Pub Date : 2020-05-26 , DOI: 10.1016/j.jcat.2020.05.020
Junnan Wei , Ting Wang , Huai Liu , Yiqiang Liu , Xing Tang , Yong Sun , Xianhai Zeng , Tingzhou Lei , Shijie Liu , Lu Lin

It is highly desirable but challenging to develop a one-pot process for the transformation of fructose into 2,5-bis(isopropoxymethyl)furan (BPMF), a promising biofuel component, because a cascade sequence involving dehydration, reduction, and etherification requires multifunctional acid catalysts. Herein, we propose a facile and firm assembly of Zr/2-methylimidazole (2-MeIM) coordination polymer over USY zeolite (USY@ZrCP) through N-Al bonds formed by the condensation of 2-MeIM and the hydroxyls on USY surface at room temperature. USY@ZrCP possesses an abundance of strong Lewis acid sites with suitable amount of Bronsted acid sites, which are mainly attributed to the highly dispersed Zr(IV) species and the hydroxyls over USY@ZrCP, respectively. Unexpectedly, USY@ZrCP could offer BPMF yield up to 82.6% from fructose in isopropanol by the integration of dehydration, Meerwein–Ponndorf–Verley reduction and etherification in a one-pot strategy. This work proposes a novel approach to prepare highly efficient and robust solid acid catalyst for the catalytic valorization of biomass-derived carbohydrates and their derivatives.



中文翻译:

Zr基配位聚合物在USY沸石上的组装作为一种高效强健的酸催化剂,用于将果糖一锅转化为2,5-双(异丙氧基甲基)呋喃

开发一锅法将果糖转化为2,5-双(异丙氧基甲基)呋喃(BPMF)(一种有前途的生物燃料成分)非常需要,但具有挑战性,因为涉及脱水,还原和醚化的级联序列需要多功能酸催化剂。本文中,我们提出了一种通过Zr / 2-甲基咪唑(2-MeIM)配位聚合物在USY沸石(USY @ ZrCP)上通过N-Al键(由2-MeIM和USY表面上的羟基缩合而形成的N-Al键)的牢固组装的方法。室内温度。USY @ ZrCP具有丰富的强路易斯酸位点和适量的布朗斯台德酸位点,这分别归因于高度分散的Zr(IV)物种和USY @ ZrCP上的羟基。出乎意料的是,USY @ ZrCP可能会将BPMF的收益率提高到82。通过一锅法将脱水,Meerwein-Ponndorf-Verley还原和醚化相结合,从果糖在异丙醇中提取6%。这项工作提出了一种新颖的方法来制备高效,坚固的固体酸催化剂,用于生物质衍生的碳水化合物及其衍生物的催化增值。

更新日期:2020-05-26
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