超临界CO2中催化剂合成及催化加氢反应共性问题研究

项目名称： 超临界CO2中催化剂合成及催化加氢反应共性问题研究

项目编号： No.21273222

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： 赵凤玉

作者单位： 中国科学院长春应用化学研究所

项目金额： 82万元

中文摘要： 近年，超临界CO2作为绿色溶剂在材料合成及催化反应等领域的应用研究得到了广泛关注。通过控制反应的温度和压力可以调变反应速率和选择性，这是超临界CO2作为绿色溶剂的突出特点之一。本课题研究超临界CO2中催化剂合成及催化加氢反应的共性基础科学问题:即,CO2压力对相态变化的影响，以及CO2分子与反应底物（金属前驱体或有机反应物）之间相互作用。以及超临界CO2的溶剂特性对催化剂活性和选择性的影响；CO2膨胀体系，CO2-H2O体系中加氢反应的规律性，特异性及反应机理，开发温和条件下催化加氢绿色反应体系。催化加氢反应由于受氢气在有机反应物中溶解度的限制，反应速率难以提高，工业上一般在高温高压的苛刻反应条件，反应过程使用大量有毒、挥发性有机溶剂，体系易燃易爆，生产过程存在安全风险。因此，开发绿色介质中清洁工艺对改造传统的工艺，节能减排，提高环境效益和社会效益具有重要意义。

中文关键词： 超临界二氧化碳；机理；催化加氢；催化剂；分子间作用

英文摘要： In these years, the application of supercritical carbon dioxide(scCO2) as a green solvent in the synthesis of nano-materials and catalysis reaction has been paid many attention.The function and morphology of the materials as well as the reaction rate and product selectivity could be adjusted by changing the CO2 pressure and conditions in the reaction system，this is one of the advantages of the scCO2。In this project,our main purpose was focused on the common fundamental scientific problems of the materials synthesis and catalytic hydrogenation in scCO2: naming the influence of CO2 properties on the pahse behaviour and the molecular interactions between CO2 with the metal precusors or the reactant. As well as the effect of specific properties of CO2 on the activity and selectivity of catalyst;The reaction mechanism of hydrogention in scCO2 ,CO2-expanding solution and CO2-H2O reaction systems. Exploring a green process for the catalytic hydrogeantion under the mild conditions. Catalytic hydrogenation was selected as the model reaction. The mutiphase hydrogenation is always hindered by the low solubility of hydrogen gas in the reaction phase,thus high pressure and temperature as well as large amount of organic solvent are always supplied in the industrial process, resulting in a process with flaming and explosing d

英文关键词： supercritical carbon dioxide；mechanism；catalytic hydrogenation；catalyst；molecualr interaction