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氧化铬改性介孔二氧化锆:用于合成 5-羟甲基糠醛的高效多相催化剂。

Chromium Oxide-modified Mesoporous Zirconium Dioxide: Efficient Heterogeneous Catalyst for the Synthesis of 5-Hydroxymethylfurfural.

机构信息

College of Energy Storage Technology, Shandong University of Science and Technology, Qianwangang Road 579, 266590, Qingdao, P. R. China.

出版信息

Chem Asian J. 2022 Oct 4;17(19):e202200653. doi: 10.1002/asia.202200653. Epub 2022 Aug 30.

Abstract

A highly efficient carbohydrate conversion to 5-hydroxymethylfurfural (5-HMF) is a promising method to achieve green and sustainable development. However, most currently reported strategies are energy consuming, and the 5-HMF yield is relatively lower in the aqueous phase. Herein, a facile method is reported to obtain effective Cr/ZrO catalysts with high acidity and their catalytic performances were investigated for catalyzing fructose to 5-HMF at different temperatures and times. With the catalysis of 15 % Cr/ZrO catalyst, the highest fructose conversion of 98 %, 5-HMF yield of 48.8 %, and 5-HMF selectivity of 49.8 % are achieved in green solvent with good recyclability. The possible reaction process of the improved catalysis performance is attributed to the highly crystalline and strong acidity of the Cr/ZrO catalyst. The Lewis acid sites could increase the overall rate of fructose conversion by promoting side reactions and might suppress fructose to glucose isomerization. In addition, Cr leakage during the reaction might act as the Bronsted acids to catalyze the fructose dehydration to 5-HMF. The reported method of introducing chromium oxides into ZrO catalyst will open a new avenue to promote the practical application of biomass and sustainable development in the future.

摘要

高效地将碳水化合物转化为 5-羟甲基糠醛(5-HMF)是实现绿色可持续发展的一种很有前途的方法。然而,目前大多数报道的策略都需要消耗大量能源,并且在水相中的 5-HMF 产率相对较低。在此,我们报道了一种简便的方法来获得具有高酸度的有效 Cr/ZrO 催化剂,并研究了它们在不同温度和时间下催化果糖转化为 5-HMF 的催化性能。在 15%Cr/ZrO 催化剂的催化作用下,在绿色溶剂中以良好的可回收性实现了最高的果糖转化率 98%、5-HMF 收率 48.8%和 5-HMF 选择性 49.8%。改进的催化性能的可能反应过程归因于 Cr/ZrO 催化剂的高结晶度和强酸度。路易斯酸位可以通过促进副反应来提高果糖转化的总速率,并可能抑制果糖向葡萄糖的异构化。此外,反应过程中 Cr 的泄漏可能作为布朗斯台德酸来催化果糖脱水生成 5-HMF。将氧化铬引入 ZrO 催化剂的方法将为未来促进生物质和可持续发展的实际应用开辟新途径。

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