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用于将生物质衍生的木聚糖催化转化为糠醛的功能化共价有机框架。

Functionalized covalent organic frameworks for catalytic conversion of biomass-derived xylan to furfural.

作者信息

Ju Yuan, Zhang Kai, Gan Peng, Guo Baozhen, Xia Huanmei, Zhang Lilong, Wang Baobin, Zhang Lei, Chen Jiachuan

机构信息

State Key Laboratory of Biobased Materials and Green Papermaking/Key Laboratory of Pulp & Paper Science and Technology of Education Ministry, Qilu University of Technology (Shandong Academy of Sciences), Jinan 250353, China.

State Key Laboratory of Biobased Materials and Green Papermaking/Key Laboratory of Pulp & Paper Science and Technology of Education Ministry, Qilu University of Technology (Shandong Academy of Sciences), Jinan 250353, China.

出版信息

Int J Biol Macromol. 2025 Mar;294:139541. doi: 10.1016/j.ijbiomac.2025.139541. Epub 2025 Jan 6.

Abstract

A direct synthesis strategy was employed to prepare functionalized COFs enriched with acidic sites, using various precursor monomers. The functionalized COFs were applied in the catalytic conversion of biomass-derived xylan to furfural in the liquid phase. The study further assessed the recyclability and reusability of these COFs, explored the relationship between their structural features and catalytic performance, and investigated the reaction mechanism underlying the COF-catalyzed conversion of xylan to furfural. The results revealed the successful solvothermal synthesis of four COFs (COF-LZU1, TP-PA, TB-DAB, and TP-DAB). Among them, TP-DAB exhibited the highest acidity, reaching 2.092 mmol/g, due to its rich content of -OH and -COOH. Additionally, TP-DAB demonstrated a well-developed porous structure and excellent thermal stability, essential characteristics for a highly efficient solid acid catalyst. When employed as a catalyst in a mixed solvent system of HO/THF at 160 °C for 180 min, TP-DAB achieved complete xylan conversion with furfural yield of 63.49 %. Moreover, TP-DAB maintained good stability and reusability, being effective for at least five cycles. This study presents a novel and highly effective green catalyst for the sustainable conversion of biomass-derived sugars into furfural, providing new avenues for the efficient conversion of biomass into fine chemicals.

摘要

采用直接合成策略,使用各种前体单体来制备富含酸性位点的功能化共价有机框架(COFs)。将功能化COFs应用于生物质衍生的木聚糖在液相中催化转化为糠醛的反应。该研究进一步评估了这些COFs的可回收性和可重复使用性,探索了它们的结构特征与催化性能之间的关系,并研究了COF催化木聚糖转化为糠醛的反应机理。结果表明成功通过溶剂热合成法制备了四种COFs(COF-LZU1、TP-PA、TB-DAB和TP-DAB)。其中,TP-DAB由于其丰富的-OH和-COOH含量,表现出最高的酸度,达到2.092 mmol/g。此外,TP-DAB具有发达的多孔结构和优异的热稳定性,这是高效固体酸催化剂的基本特征。当在160°C的HO/THF混合溶剂体系中用作催化剂180分钟时,TP-DAB实现了木聚糖的完全转化,糠醛产率为63.49%。此外,TP-DAB保持了良好的稳定性和可重复使用性,至少可有效循环使用五次。本研究为生物质衍生糖可持续转化为糠醛提供了一种新型高效的绿色催化剂,为生物质高效转化为精细化学品提供了新途径。

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