Investigating reaction mechanisms of base-catalyzed isomerization of aldoses into ketoses for developing efficient catalytic processes

研究醛糖碱催化异构化为酮糖的反应机制，以开发有效的催化过程

• 批准号: 397970309
• 负责人: Dr. Irina Delidovich, Ph.D.
• 金额: --
• 依托单位: Institut für Verfahrenstechnik, Umwelttechnik und Technische Biowissenschaften (E166)
• 依托单位国家: 德国
• 项目类别: Research Grants
• 财政年份: 2018
• 资助国家: 德国
• 起止时间: 2017-12-31 至 2021-12-31
• 项目状态: 已结题
• 来源: https://gepris.dfg.de/gepris/projekt/397970309?language=en
• 关键词: Investigating; reaction; mechanisms; base; catalyzed

Isomerization of aldoses into ketoses presents an industrially important reaction. It gives rise to keto-saccharides which are in high demand in food industry, manufacture of pharmaceuticals, synthesis of chiral organic compounds, and potentially for production of biofuels. Current industrial manufactures of ketoses rely on enzymatic processes, whereas chemo-catalytic methods present a number of advantages over biotechnological production. For example, the chemo-catalysts are of lower cost and less demanding to purity of feed. Moreover, thermostability of chemical catalysts typically excels the thermostability of enzymes, which enables operations at higher temperatures with a positive effect on the reaction rates and space-time-yields. Utilization of solid catalysts is especially beneficial considering ease of the catalyst separation and recycling. The current project focuses on investigating the base catalysts for isomerization of aldoses into ketoses with the ultimate goal to elaborate efficient tailor-made chemo-catalysts for these processes. Even though the isomerization over basic catalysts has been known for a long time, a molecular mechanism of this reaction is still poorly understood. At the same time, insight into the kinetics and mechanism of the isomerization (and of side reactions) should facilitate a knowledge-driven development of efficient catalysts.In this project the isomerization of glucose into fructose will be investigated in order to comprehend the kinetics and mechanism of the reaction depending on the nature of soluble and solid catalysts. The isomerization of other aldoses with various structures will be studied; and the dependence of the reaction efficiency on the structure of aldose will be obtained. Finally, stability of solid basic catalysts under the reaction conditions will be addressed. The correlations revealed in the study will provide fundamental understanding for a design of catalysts and catalytic processes for isomerization of aldoses into ketoses.

醛糖异构化为酮糖是工业上重要的反应。它产生酮糖，食品工业、药品制造、手性有机化合物的合成以及生物燃料生产中对酮糖的需求量很大。目前酮糖的工业生产依赖于酶促过程，而化学催化方法比生物技术生产具有许多优势。例如，化学催化剂成本较低，对原料纯度要求较低。此外，化学催化剂的热稳定性通常优于酶的热稳定性，这使得能够在更高的温度下操作，并对反应速率和时空产率产生积极影响。考虑到催化剂分离和回收的容易性，固体催化剂的利用特别有利。目前的项目重点是研究醛糖异构化为酮糖的基础催化剂，最终目标是为这些过程精心设计高效的定制化学催化剂。尽管碱性催化剂上的异构化早已为人所知，但对该反应的分子机制仍知之甚少。同时，对异构化（和副反应）的动力学和机制的深入了解应有助于知识驱动的高效催化剂的开发。在该项目中，将研究葡萄糖异构化为果糖，以了解动力学和异构化过程。反应机理取决于可溶性和固体催化剂的性质。研究其他各种结构醛糖的异构化；并得到反应效率对醛糖结构的依赖性。最后，将讨论反应条件下固体碱性催化剂的稳定性。研究中揭示的相关性将为醛糖异构化为酮糖的催化剂和催化过程的设计提供基本的理解。