| 刘峻豪,李树奎,李富让,耿旭超,吕玉超,付建冶,马丽爽,刘欣梅.化学通报,2026,89(6):700-708,750. |
| 不同拓扑结构锡基分子筛的构筑及其对木糖制糠醛催化反应的调控 |
| Construction of Tin-Based Zeolites with Varied Topological Structures for Regulating the Catalytic Conversion of Xylose to Furfural |
| 投稿时间：2026-03-09 修订日期：2026-03-23 |
| DOI： |
| 中文关键词: 木糖 糠醛 含锡分子筛 拓扑结构 酸性质 |
| 英文关键词:Xylose Furfural Tin-containing zeolite Topological structure Acid property |
| 基金项目:山东省重点科技项目(2024CXPT078)和国家自然科学基金项目(U24B20200,22378427)资助 |
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| 中文摘要: |
| 糠醛作为最具价值的生物质衍生平台分子之一,其工业生产长期受限于均相酸催化剂所导致的收率低、设备腐蚀及废污排放等问题,因此开发高效分子筛基固体酸催化剂具有重要的工业应用前景。本研究采用类固相法,以锡酸钠为金属前驱体,在无氟介质中一步将Sn(IV)和Al(III)中心同时引入分子筛骨架,成功制备出了四种不同拓扑结构的含锡分子筛催化剂(Sn, Al)-Beta、(Sn, Al)-MOR、(Sn, Al)-ZSM-5和(Sn, Al)-ZSM-22。利用分子筛骨架中四配位的Sn(IV)和Al(III)分别作为Lewis酸位点和Br?nsted酸位点,协同催化木糖高效转化制备糠醛。骨架Sn物种的引入显著增加了Lewis酸量,同时小幅提升Br?nsted酸量,成功构建了双酸协同催化中心,使含锡分子筛样品的木糖转化率与糠醛选择性显著提升。构效关系分析进一步揭示,含锡分子筛的催化性能是酸性质与扩散性能协同作用的结果：Beta和Mor分子筛的十二元环孔道结构有利于反应物和产物在催化剂内的快速扩散；而Beta分子筛丰富的Lewis酸位点和低强酸含量则可在促进木糖异构的同时,有效抑制糠醛的聚合副反应,提高糠醛选择性；与之相比,ZSM-5和ZSM-22分子筛则因十元环孔道扩散受限及强酸主导的副反应加剧,催化性能相对较低。其中,(Sn, Al)-Beta催化剂的性能最优,拥有93.3%的木糖转化率和最高56.2%的糠醛选择性。本研究通过揭示含锡分子筛酸性质、拓扑结构对催化性能的影响机制,为设计用于糠醛生产的高效工业分子筛催化剂提供了理论依据与实验支撑。 |
| 英文摘要: |
| Furfural is a valuable biomass-derived platform chemical, but its industrial production suffers from low yield and environmental issues due to homogeneous acid catalysts. Here, we report four stannosilicate zeolites with different topologies: (Sn, Al)-Beta, (Sn, Al)-Mor, (Sn, Al)-ZSM-5 and (Sn, Al)-ZSM-22. These materials were synthesized via a solvent-free method, achieving one-step incorporation of Sn(IV) and Al(III) into the framework. Framework Sn(IV) and Al(III) act as Lewis and Br?nsted acid sites, respectively, forming dual acid cooperative centers that enhance xylose conversion and furfural selectivity. Structure-performance analysis shows that catalytic efficiency arises from the synergy between acidity and diffusion properties. The 12-membered ring channels of Beta and MOR enable rapid mass transfer, while abundant Lewis acid sites and low strong acid content of Beta zeolite promote xylose isomerization and suppress furfural polymerization. In contrast, ZSM-5 and ZSM-22 suffer from diffusion constraints due to their 10-membered ring channels and severe side reactions dominated by strong acid sites. (Sn, Al)-Beta achieves the best performance, with 93.3% xylose conversion and 56.2% furfural selectivity. This work provides insights for designing efficient industrial zeolite catalysts for furfural production. |
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