中文摘要
均相催化由于具有反应条件温和、活性和选择性高等优点，在化学工业中被广泛地应用于催化合成有机化合物。本项目的研究目标是建立和发展定向合成含氧有机化合物的新型环境友好均相催化反应体系。1. 羰基化反应是催化合成有机化学品中最基本的含氧化合物的重要催化过程。重点开展具有催化功能的离子液体设计、合成与物理化学性质测定；以一氧化碳、二氧化碳、甲醛等为羰基化试剂，构建新型高效催化剂体系；新型手性配体及其金属配合物的设计、合成与结构表征，研究催化不对称羰基化反应的构效关系。2. 仿生催化氧化可在温和条件下实现分子氧选择性氧化烃类物质转变成含氧化合物。重点开展以过氧化氢和分子氧为氧源的烃类清洁催化氧化反应体系研究，探讨催化循环过程的作用机制和分子氧及底物的活化机理；建立高效的手性类卟啉金属催化剂催化不对称氧化反应体系。3. 生物催化是一类比较符合"绿色化学"的反应过程。重点开展具有高转化效能的甲烷利用菌菌株的选育，建立高效合成脂肪酸聚酯的甲烷生物催化转化体系；研究微水相或有机相中酶催化聚合、不对称拆分等反应，建立化学-生物顺序反应新方法。
英文摘要
Homogeneous catalysis has been widely applied in catalyzed synthesis of organic compounds in chemical industries due to its advantages of mild reaction conditions, high catalytic activity and selectivity. The research goal of this project is the establishment and development of several environment friendly homogeneous catalysis systems for selective synthesis of oxygenated organic compounds. 1. Carbonylation is a significant catalytic process for catalyzed synthesis of the most basic oxygenated compounds in organic chemicals. Lay emphasis of development on design, synthesis and determination of physicochemical properties of ionic liquids bearing catalytic activity. Build up new-type and high efficiency carbonylation systems using carbon monoxide, carbon dioxide, formaldehyde etc. Design, synthesis and characterization of new-type chiral ligands and chiral metallic complexes, studies on structure-activity relationship in asymmetric carbonylation. 2.Selective oxidation of hydrocarbons to oxygenated compounds by molecular oxygen can be realized under mild conditions by biomimetic catalytic oxidation. Develop the cleaner catalytic oxidation system using hydrogen peroxide or molecular oxygen as oxidants, investigate the catalytic cyclic process and the activation mechanism of molecular oxygen and substrates. Build a high efficiency asymmetric oxidation system catalyzed by chiral porphyrin-resembling metal complexes. 3. Biocatalysis is a reaction process which is compatible with the green chemistry. Screening and breeding of strains of methane-utilizing bacteria with high conversion efficiency, establishing biocatalytic conversion system of methane for high efficiency synthesis polyhydroxyalkanoates. Researching the enzyme catalyzed ploymerization and asymmetric resolution reactions in low aqueous media or organic phase, establishing the new methods of chemical-biological consecutive reaction.
结题摘要
均相催化由于具有反应条件温和、活性和选择性高等优点，在化学工业中被广泛地应用于催化合成有机化合物。本项目的研究目标是建立和发展定向合成含氧有机化合物的新型环境友好均相催化反应体系。1. 羰基化反应是催化合成有机化学品中最基本的含氧化合物的重要催化过程。重点开展具有催化功能的离子液体设计、合成与物理化学性质测定；以一氧化碳、二氧化碳、甲醛等为羰基化试剂，构建新型高效催化剂体系；新型手性配体及其金属配合物的设计、合成与结构表征，研究催化不对称羰基化反应的构效关系。2. 仿生催化氧化可在温和条件下实现分子氧选择性氧化烃类物质转变成含氧化合物。重点开展以过氧化氢和分子氧为氧源的烃类清洁催化氧化反应体系研究，探讨催化循环过程的作用机制和分子氧及底物的活化机理；建立高效的手性类卟啉金属催化剂催化不对称氧化反应体系。3. 生物催化是一类比较符合"绿色化学"的反应过程。重点开展具有高转化效能的甲烷利用菌菌株的选育，建立高效合成脂肪酸聚酯的甲烷生物催化转化体系；研究微水相或有机相中酶催化聚合、不对称拆分等反应，建立化学-生物顺序反应新方法。