新型改性海泡石负载型镍基多金属催化剂构筑及催化己二腈加氢性能研究

由于己内酰胺产能增速快于需求量增速，其市场竞争愈发激烈，因此需要加大技术研发。丁二烯/己二腈法采用来源丰富、价格低廉的丁二烯，物耗能耗低，工艺简单，但需突破关键步骤己二腈加氢过程。本项目采用分子模拟计算和实验结合的方法，设计制备改性海泡石负载型镍基多金属催化剂，研究修饰改性对载体孔结构、表面活性吸附中心及对活性组分形貌结构、分散度等的影响。通过研究活性组分与助剂金属的电子相互作用及对表面形貌、电子结构等的影响规律，进而研究载体、活性组分和助剂金属间协同催化效应，获得最优修饰改性方法和条件，构筑具有协同催化作用的新型催化剂用于己二腈加氢，实现在温和条件，不加氨水或碱溶液体系中，高转化和高选择性制备6-氨基己腈和己二胺。应用在线反应红外技术研究反应机理和动力学，为工业化应用提供指导，为腈基、含氮化合物加氢催化剂研制提供借鉴，项目成果有望简化和改进己内酰胺生产工艺，有重要学术价值和很好应用前景。

The production rate of ε-caprolactam is faster than its market demand, which leads to intense competition on the market and requirement for researchers to improve its production technology. Producing ε-caprolactam from Butadiene/Adiponitrile hydrogenation methods has the advantages of cheaper butadiene material, low energy consumption and simple process. But the key step of adiponitrile hydrogenation in the process is less than ideal and needs improvement..Based on the combination of the molecular simulation calculations and experiments, this project designs the modified sepiolite supported nickel based multi-metal catalysts, investigates the influence of modification on the pore structure of the support, active and adsorption centers, and morphology and dispersion of active component . With the investigation of electron interaction mechanism of active components and auxiliary metal, and of its influence on the surface morphology and electronic structure of catalysts and the further study of the synergistic catalytic effects between supports, active components and auxiliary metals, the optimal modification conditions are achieved, and the novel catalyst with synergistic catalysis will be prepared, which could catalyze adiponitrile hydrogenation to form 6-aminocapronitrile and hexamethylendiamine with high conversion and selectivity under mild conditions without addition of aqueous ammonia or alkali metal hydroxide solution. .Using the online FT-IR, the reaction mechanism and kinetics will be studied, and the results of this work could provide effective guidance for the industrial application and reactor design, and provide a reference for hydrogenation catalyst preparation of nitrile compounds and nitrogen compounds synthesis processes. The results of this work would also simplify and improve the present technology of ε-caprolactam production and is of great scientific value and application prospects.