高效加氢催化剂Ni2P/石墨烯的制备及催化性能研究

Transition metal phosphides are becoming a research hotspot in the field of new catalytic materials because of their excellent hydrogenation activities. However, the catalytic activities of phosphides are limited by the aggregation and the blocking of carrier pores during the preparation. This project proposes to use graphene as support to prepare a highly efficient Ni2P hydrogenation catalyst. We mainly study the interaction mechanism between graphene oxide and nickel ions, and the influences of hypophosphite decomposition on properties of graphene and dispersion state of Ni2P, to optimize preparation conditions.The good metal cation adsorption capacity of graphene oxide and the strong interaction between Ni2P and the defective sites located on the graphene surface will be employed to improve the dispersion of Ni2P and increase the amount of active sites. Meanwhile, the unique two-dimensional structure, perfect stability and thermal conduction, as well as high hydrogen storage and dissociation capacity of graphene are applied to achieve the high catalytic hydrogenation activity. Based on the strong adsorption of phenol on graphene, this project will study the catalytic performance of Ni2P/graphene in the phenol hydrogenation reaction and the relationship between catalytic behavior and physicochemical properties, expand the catalysis research areas of phosphides, and provide new ideas for the study of graphene in heterogeneous catalysis.

过渡金属磷化物因其优异的加氢处理活性成为新型催化材料领域的研究热点。然而，磷化物制备中的团聚和对载体孔道的堵塞限制了其催化活性的发挥。本项目提出以石墨烯为载体负载Ni2P制备高效加氢催化剂。重点研究氧化石墨烯与镍离子的作用机理以及次磷酸盐分解过程对石墨烯性质和Ni2P分散状态的影响，优化制备条件。利用氧化石墨烯强的阳离子吸附能力和石墨烯表面缺陷位对Ni2P的强作用力，提高Ni2P在石墨烯上的分散度，增加活性位数量。同时，借助石墨烯独特的二维结构、优异的稳定性和导热性、以及高储氢和氢解离能力，实现Ni2P/石墨烯的高效加氢性能。基于石墨烯对苯酚的强吸附作用，研究Ni2P/石墨烯在苯酚加氢反应中的催化行为及构效关系，拓展磷化物催化领域的研究，并为石墨烯在多相催化中的应用研究提供新思路。

过渡金属磷化物因其优异的加氢处理活性成为新型催化材料领域的研究热点。然而，磷化物制备中的团聚和对载体孔道的堵塞限制了其催化活性的发挥。本项目以石墨烯为载体负载磷化镍制备高效加氢催化剂。本项目主要研究了以下四方面：(1)氧化条件对氧化石墨烯组成及结构的影响;(2)氧化石墨烯与负载其上的金属纳米粒子的作用；（3）不同合成方法对过渡金属磷化物粒径、形貌及性能的影响；（4）合成的系列催化剂在不同加氢处理反应中的性能。通过上述研究我们通过一步水热法制备了高分散纳米磷化镍/石墨烯复合物。利用氧化石墨烯强的阳离子吸附能力和石墨烯表面缺陷位对磷化镍的强作用力，提高磷化镍在石墨烯上的分散度，增加活性位数量。同时，借助石墨烯独特的二维结构、优异的稳定性和导热性、以及高储氢和氢解离能力，实现了磷化镍/石墨烯的高效加氢性能。本研究拓展了磷化物催化领域的研究，并为石墨烯在多相催化中的应用研究提供新思路。