Mesoporous Carbon Supported Metal Catalysts for Sustainable Hydrogenation Reactions

中孔炭（CMC，Carbon Made in China，专利号：J.Shen）是一种很有前途的多相催化载体材料。与传统的活性炭（AC）类似，CMC的特点是比表面积大，耐化学性高，负载金属易于回收。与AC的微孔性不同，介孔性有利于质量传递，这对于大分子或液相反应尤其重要。杂原子如N可并入CMC中以获得NMC。引入的N物种改善了载体的润湿性和碱性，促进了金属分散并增强了负载纳米颗粒的热稳定性以对抗烧结。在重要的加氢反应中，适当的碱性比酸性更有利于高选择性。N物质还改善了还原性，导致负载金属的较低氧化态，这被认为是对氢化反应的积极影响。在本项目中，我们实验室开发的CMC和NMC材料将用作活性金属组分，金属碳化物，氮化物和磷化物的载体，并应用于硝基化合物的加氢，苯胺及其衍生物中的苯环，加氢脱氧（HDO）和加氢脱硫（HDS）反应，以及生物质木质素的加氢解聚。将在不同条件下评价催化剂的催化性能。催化活性中心将被确定，金属载体相互作用，H溢出，表面扩散和催化机制将被研究支持国家的最先进的理论。

Mesoporous carbon (CMC, Carbon Made in China, Patent of Prof. J. Shen) is a promising support material in heterogeneous catalysis. Similar to the conventional activated carbon (AC), CMC is characterized by large surface area, high chemical resistance and easy recycling of supported metals. Different from the microporosity of AC, the mesoporous properties facilitate mass transport, which is especially important for large molecules or liquid phase reactions. Heteroatoms like N can be incorporated into CMC to obtain NMC. The incorporated N species improve the wettability and basicity of the support, promote metal dispersion and enhance thermal stability of supported nanoparticles against sintering. An appropriate basicity is more advantageous than acidity for high selectivity in important hydrogenation reactions. The N species also improve the reducibility leading to a lower oxidation state of supported metals, which is considered as a positive effect for hydrogenation reactions. In this project, the CMC and NMC materials developed in our lab will be used as support for active metallic components, metal carbides, nitrides and phosphides and applied in the hydrogenation of nitro-compounds, the benzene ring in aniline and its derivatives, hydrodeoxygenation (HDO) and hydrodesulfurization (HDS) reactions, and hydrodepolymerization of biomass-derived lignin. The catalytic performance of the catalysts will be evaluated under different conditions. The catalytically active centers will be identified, and the metal-support interactions, H spill-over, surface diffusion and catalytic mechanisms will be studied supported by state-of-the-art theory.