具有加氢和重排活性双功能催化剂构筑及催化硝基环己烷一步制备己内酰胺研究

本项目拟采用分子模拟计算和实验研究相结合的方法，设计和制备具有加氢还原和重排活性中心的双功能催化剂，实现硝基环己烷加氢还原和重排反应耦合，完成由硝基环己烷一步高选择性制备己内酰胺。具体包括：在负载活性金属的酸性介孔分子筛上催化分解含碳气体生长碳纳米管，经硝酸等处理后负载金属钯纳米粒子，制备获得钯/碳纳米管-酸性介孔分子筛催化剂。在优选合适溶剂的基础上，考察催化剂还原活性中心不同结构的碳纳米管、钯粒径、形貌结构及催化剂重排活性中心不同酸强度和酸量等对催化性能的影响。结合催化剂分析表征结果，获得催化剂微观结构和催化性能的构效关系，借助在线反应红外技术，研究该过程反应机理和动力学，并对过程进行参数优化。本项目通过催化剂创新，实现加氢和重排反应耦合，可为类似共性问题提供借鉴作用。实现硝基环己烷一步高选择性制备己内酰胺，可望简化和改进现有生产工艺，可见本项目有着重要的学术价值和很好的应用前景。

Based on the combination of molecular simulation calculation and experimental study, bifunctional catalyst with both hydrogenation reduction and Beckmann rearrangement active center will be designed and prepared to fulfill the coupling nitrocyclohexane hydrogenation and Beckmann rearrangement so as to achieve the one-step synthesis of ε-caprolactam with high selectivity. The research contents include, growth of carbon nanotubes (CNTs) on the active metal supported acid mesoporous molecular sieve, treated with nitric acid and then the nano Palladium particles are supported on it to obtain the Pd/CNT- acid mesoporous molecular sieve catalyst. Based on determining the suitable solvent, the influences of the carbon nanotube structure, Palladium particle size and structure, acid strength and the numbers of acid sites on the performance of the catalyst will be investigated in detail. Combined with the characterization results of the catalyst, the relationship between the catalyst structure and the catalytic performance will be obtained. With the aid of on-line FTIR, the reaction mechanism and reaction kinetics will be studied, and then the process optimization will be carried out. The success in coupling hydrogenation and Beckmann rearrangement through the innovation of catalyst will provide experience in similar typical problem. And one-step synthesis of ε-caprolactam from nitrocyclohexane with high selectivity will simplify and improve the present production technology. Therefore, the project is of great scientific value and application prospects.