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

本研究首先确定了催化剂的制备方法，并对所制备的催化剂进行了工业应用试验。第一年，为了建立在载体颗粒上的选择性沉积技术，研究了金属纳米颗粒的选择性沉积，包括Ru、Rh、Pd、Ir和PtFor及其溶液。也就是说，首先在溶液相中精确控制条件(主要是pH)制备Ru、Rh、Pd、Ir、Pt等金属的目标络合物，以便在载体颗粒表面选择性地形成它们的氧化物或氢氧化物。其次，通过分散和老化载体粉末，如单分散的二氧化钛、赤铁矿和二氧化硅颗粒，在固体表面选择性地生成贵金属氢氧化物。最后通过氢气还原得到金属贵金属纳米颗粒。第二年，在第一年研究成果的基础上，重点考察了贵金属纳米粒子作为催化剂的应用。首先考察了1-辛烷加氢制辛烷的活性。将制备的纳米贵金属催化剂与传统催化剂进行了比较。从这个角度来看，我们的催化剂表现出了非常高的加氢活性。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，以苯加氢制环己烯为例进行了连续加氢反应。最后，在采用本方法制备的贵金属纳米颗粒催化剂上，考察了CO加氢生成有机化合物的反应。

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.