温和条件下生物基碳水化合物新型氢解催化体系的构建与选择性调控

项目名称： 温和条件下生物基碳水化合物新型氢解催化体系的构建与选择性调控

项目编号： No.21273260

项目类型： 面上项目

立项/批准年度： 2013

项目学科： 数理科学和化学

项目作者： 牟新东

作者单位： 中国科学院青岛生物能源与过程研究所

项目金额： 82万元

中文摘要： 二元醇是重要的工业大宗化学品，可由石化原料或生物质原料制备。然而，在生物基碳水化合物的催化氢解反应过程中，高温和高氢压的强反应条件通常是不可避免的，而这常常导致对目标产物的选择性下降。 针对现行碳水化合物氢解制备二元醇过程中存在的反应温度高、产物选择性差等问题，本研究力图开发一种在温和条件下即有较高催化活性和选择性的碳水化合物选择氢解催化反应体系。通过对碱促进和金属盐促进下，氢解过程中涉及的关键基元反应进行反应路径分析与反应动力学研究，明晰不同反应条件下，催化反应的过程与机理，形成碳水化合物催化氢解中C-C键断裂的初步理论。采用原位水热合成的方法，合成分子筛限域的Ru基择形加氢催化剂，实现对C-C键裂解所得的小分子中间产物的选择性加氢；与此同时，含有活泼羰基基团的单糖反应物分子不会被加氢。在此基础上，设计并构建温和条件下高选择性转化碳水化合物制备二元醇的新型催化体系。

中文关键词： 碳水化合物；生物质；催化；多元醇；断键

英文摘要： Diols are important industrial mass chemicals, which could be obtained from fossil feedstocks or biomass. However, elevated reaction conditions, such as high temperature and high hydrogen pressure, are usually inevitable for diols production through catalytic hydrogenolysis of bio-derived carbohydrates, which often results in the low selectivity to the desired products. Aiming to the catalytic conversion of carbohydrates into diols under mild conditions, we are trying to develop a selective catalytic hydrogenolysis reaction system which could achieve high catalytic reactivity and high selectivity under mild conditions. Reaction path analysis and reaction dynamics study would be perform to the related key reaction steps in the catalytic hydrogenolysis accelerated by alkali or metal salts. The primary theory for the selective C-C bond cleavage of carbohydrates under different conditions will be clarified. Zeolite-confined Ru-based shape selective hydrogenation catalysts will be fabricated through in-situ hydrothermal synthesis, which could be potentially used to catalyze the hydrogenation of small molecular intermediates generated through catalytic carbon-carbon cleavage. Meanwhile, the sugars bearing reactive carbonyl groups will not be hydrogenated. Based on the above mentioned, a novel catalytic system for eff

英文关键词： carbohydrate；biomass；catalysis；polyols；bond-cleavage