NO2气相硝化氧化低碳环烷烃一步制备硝基烷烃和二元羧酸反应及其多相催化调控研究

项目名称： NO2气相硝化氧化低碳环烷烃一步制备硝基烷烃和二元羧酸反应及其多相催化调控研究

项目编号： No.21276216

项目类型： 面上项目

立项/批准年度： 2013

项目学科： 化学工业

项目作者： 游奎一

作者单位： 湘潭大学

项目金额： 80万元

中文摘要： 围绕着硝基烷烃和二元羧酸化合物生产方法的创新，开展低碳环烷烃与NO2气相硝化氧化一步制备硝基烷烃和二元羧酸及其多相催化调控研究，构筑气相硝化氧化催化剂的方法学，研究反应体系中环烷烃C-H键硝化与氧化反应多样性的催化调控规律；设计和研究催化剂的性能调变方法，探索其催化调控硝化与氧化反应产物选择性的规律。应用密度泛函理论（DFT）对反应物分子和催化剂结构进行优化，计算反应物分子的电子云密度和反应活性，研究催化剂结构参数与催化性能的对应关系；利用原位漫反射红外光谱（DRIFTS）、在线反应红外光谱深入研究催化剂活性中心的状态和反应机理，建立反应动力学模型，求解动力学参数，认识低碳环烷烃气相催化硝化氧化反应的调变规律，为开辟硝基烷烃和二元羧酸化合物的合成新方法提供理论基础和技术依据，丰富含氮化合物和二元羧酸化合物的合成方法学，促进我国在精细化工和功能材料等领域中的应用和创新。

中文关键词： 环己烷；二氧化氮；硝基环己烷；己二酸；多相催化调控

英文摘要： According to the synthesis method innovation of nitroalkanes and dicarboxylic acids, the heterogeneous catalytic regulation on one-step synthesis of nitroalkanes and dicarboxylic acids from vapor phase nitration-oxidation of low carbon cycloalkanes with NO2 is developed. The methodology for preparation of nitration-oxidation catalysts is builded. And the catalytic regulation law on the diversity of nitration and oxidation reaction for C-H bond of cycloalkanes is researched., Its catalytic regulation law on products selectivity of nitration and oxidation reaction is studied by designing and researching for modulation method of catalyst performance. The structure of reactants and catalysts is optimizated by DFT and the electron cloud density and reaction activity are calculated in order to research the relationship between structure parameters of catalyst and catalytic performance. The activity state of catalyst and reaction mechanism is studied thoroughly by the use of diffuse reflectance infrared spectroscopy ( DRIFTS ) and online reaction infrared spectroscopy, and the reaction kinetics model is established to obtain the dynamics parameter. The modulation rules for catalytic nitration-oxidation reaction of low carbon cycloalkanes with NO2 in vapor phase are understanded. The theoretical and technical basis are

英文关键词： Cyclohexane；Nitrogen dioxide；Nitrocyclohexane；Adipic acid；Heterogeneous catalytic regulation