Selective hydrogenation by highly-dispersed and highly-loaded noble metallic nanoparticulate catalysts

在本研究中，首先建立了制备方法，然后对所制备的催化剂进行了工业应用测试。第一年，为了在载体颗粒上建立选择性沉积技术，开展了从其溶液中选择性沉积Ru、Rh、Pd、Ir、Pt等金属纳米粒子的研究项目。即首先在以pH为主的精确控制条件下，在溶液中制备Ru、Rh、Pd、Ir、Pt等金属靶配合物，选择性地在载体颗粒表面形成氧化物或氢氧化物。其次，通过分散和时效支撑粉末，如单分散的二氧化钛、赤铁矿和二氧化硅颗粒，选择性地在固体表面生成贵金属氢氧化物。最后，通过氢还原法制备金属贵金属纳米颗粒。第二年，在第一年研究成果的基础上，重点研究了贵金属纳米颗粒作为催化剂的应用。首先，考察了1-辛烷加氢生成辛烷的活性。在这方面，将制备的贵金属纳米颗粒催化剂与常规催化剂进行了比较。从这个角度来看，我们的催化剂表现出非常高的加氢活性。随后，对催化剂的选择性进行了测试。考虑到本研究使用的是无孔载体粉末，以连续加氢反应为例，对苯加氢制环己烯进行了测试。最后，在本方法制备的贵金属纳米颗粒催化剂上，研究了CO加氢生成有机化合物。

In the present study, first of all, the preparation method was established and then as-prepared catalysts were tested for industrial use. In the first year, in order to establish the selective deposition technique onto the support particles, the research project on the selective deposition of metallic nanoparticles, such as Ru, Rh, Pd, Ir, and Pt from, its solution was investigated. Namely, first of all, target complexes of metal, such as Ru, Rh, Pd, Ir, and Pt, was prepared in the solution phase under the precise control of conditions, mainly pH, in order to form their oxide or hydroxide selectively on surfaces of the support particles. In the next, noble metal hydroxide was selectively generated on the solid surfaces by dispersing and aging support powders, such as monodispersed particles of titania, hematite, and silica. Finally, metallic noble nanoparticles were formed by the hydrogen reduction. In the second year, based on the results obtained in the first year, application of noble nanoparticles as a catalyst was mainly investigated. First of all, the activity of hydrogenation of 1-octent to octane was investigated. As-prepared noble nanoparticulate catalysts were compared with a conventional catalyst in this regard. From this point of view, our catalyst exhibited remarkably high activity for the hydrogenation. Hereafter, the selectivity of the catalysts was tested. Taking it into the consideration that nonporous support powders were used in the present study, the hydrogenation of benzene to cyclohexene was tested as an example of successive hydrogenation reaction. Finally, CO hydrogenation to form organic compounds was investigated over the noble nanoparticulate catalysts prepared by the present method.