One-pot cascade conversion of fructose to 2,5-diformylfuran enabled by a polyionic liquid-based porous catalyst†

IF 6.4 1区 化学 Q1 CHEMISTRY, INORGANIC & NUCLEAR Inorganic Chemistry Frontiers Pub Date : 2025-04-08 DOI:10.1039/D5QI00135H
Gang Liu, Jun Zheng, Xianqiang Huang, Shiqi Fu, Shiqi Xi, Yalin Zhang, Zhen Li, Fei Yu and Yifa Chen
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Abstract

One-pot direct conversion of cheap and abundant fructose to 2,5-diformylfuran (DFF) is highly desirable to achieve hundreds-fold value-increase and high atomic economy, yet it is still challenging due to the lack of suitable catalysts with cascade conversion ability. In this work, we developed a porous hybrid catalyst (i.e. PMo10V2@2Br-PIL) based on the assembly of polyoxometalates and porous polyionic liquids that can be applied in the one-pot conversion of fructose to DFF. The integration of PMo10V2 with 2Br-PIL can impart both Brønsted acid and oxidation sites in the porous structure, thereby enabling the one-pot cascade conversion. As a result, PMo10V2@2Br-PIL demonstrated a remarkable DFF yield (95% yield), satisfying stability, recyclability and scale-up production ability (≈12.3 g in a batch experiment), demonstrating great potential for industrial production of DFF from fructose. Theoretical calculations revealed a synergistic effect of Brønsted acid sites and oxidation sites in PMo10V2@2Br-PIL, which promoted the one-pot conversion of fructose to DFF. This study enhances the understanding of biomass transformation over hybrid catalysts through synergetic acidic/oxidative catalysis, contributing to the development of highly active, selective, and multifunctional catalysts for one-pot biomass conversion.

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多离子液体多孔催化剂催化果糖一锅级联转化为2,5-二甲酰呋喃
廉价而丰富的果糖一锅直接转化为2,5-二甲酰呋喃(DFF)是实现百倍增值和高原子经济性的迫切需要,但由于缺乏合适的具有级联转化能力的催化剂,仍然具有挑战性。在这项工作中,我们开发了一种基于多金属氧酸盐和多孔多离子液体组装的多孔杂化催化剂(即PMo10V2@2Br-PIL),可用于一锅转化果糖为DFF。PMo10V2与2Br-PIL的集成可以在多孔结构中同时赋予Brönsted酸位点和氧化位点,从而实现一锅级联转化。结果表明,PMo10V2@2Br-PIL具有显著的DFF产率(95%产率),具有良好的稳定性、可回收性和规模化生产能力(批量实验≈12.3 g),具有从果糖中提取DFF的工业生产潜力。理论计算表明PMo10V2@2Br-PIL中Brönsted酸位点和氧化位点的协同作用可以促进果糖一锅转化为DFF。本研究加深了对酸性/氧化协同催化混合催化剂转化生物质的认识,为设计高效、选择性和多功能的一锅生物质转化催化剂做出了贡献。
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来源期刊
Inorganic Chemistry Frontiers
Inorganic Chemistry Frontiers CHEMISTRY, INORGANIC & NUCLEAR-
CiteScore
10.40
自引率
7.10%
发文量
587
审稿时长
1.2 months
期刊介绍: The international, high quality journal for interdisciplinary research between inorganic chemistry and related subjects
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