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Solid State NMR studies on the mechanisms of immobilized organic-inorganic metal containing heterogeneous catalysts

固载有机-无机金属多相催化剂机理的固态核磁共振研究

基本信息

批准号：
57198502
负责人：
Professor Dr. Gerd Buntkowsky
金额：
--
依托单位：
Institut für Chemie und Biochemie
依托单位国家：
德国
项目类别：
Research Grants
财政年份：
2007
资助国家：
德国
起止时间：
2006-12-31 至 2014-12-31
项目状态：
已结题

来源：
https://gepris.dfg.de/gepris/projekt/57198502?language=en
关键词：
Solid State NMR studies mechanisms

项目摘要

Multi nuclear solid state NMR and other physico-chemical techniques are employed for the study of immobilized catalysts, metal-clusters, metal-nanoparticles and their interactions with substrates. The immobilized catalysts are made by covalently binding metal-containing catalysts to the surface of nano-structured silica materials with different morphologies(porous or nanoparticles) via organic linkers. The structure of the immobilized catalysts on the support material, its interactions with substrates and the influence of macroscopic parameters such as temperature on its properties are investigated. The catalytic activity of the catalysts is tested by model reactions, in particular hydrogenations. Initially simple reactions like the isotope scrambling of hydrogen or the hydrogenation of ethylene as model reactions for the catalysts are employed. To reveal effects of the size and morphology of the support, larger substrate molecules and enantio-selective immobilized catalysts are studied. In parallel to these studies we wish to continue our collaboration with the Chaudret and Poteau groups on the study of molecular hydrogen interacting with catalytically active transition metal compounds and nano-particles. Here we want to employ the 2H NMR data-base built in the first period for the study of hydrogen adsorbed on transition-metal nanoparticles (ruthenium, palladium, platinum). Finally we want to study the hydrogen dynamics of the H4Ru4(CO)12 cluster and reveal the nature of the dynamic process and its energetic parameters.

多核固体核磁共振和其他物理化学技术被用于研究固定化催化剂、金属簇、金属纳米颗粒及其与底物的相互作用。固定化催化剂是通过有机连接剂将含金属催化剂与不同形貌（多孔或纳米）的纳米结构二氧化硅材料表面共价结合而成的。研究了载体材料上固定化催化剂的结构、与底物的相互作用以及温度等宏观参数对其性能的影响。催化剂的催化活性是通过模型反应，特别是氢化反应来测试的。最初，简单的反应，如氢的同位素抢夺或乙烯的加氢反应作为催化剂的模型反应。为了揭示载体大小和形态的影响，研究了较大的底物分子和对映体选择性固定化催化剂。在这些研究的同时，我们希望继续与Chaudret和Poteau团队合作，研究分子氢与催化活性过渡金属化合物和纳米颗粒的相互作用。在这里，我们想利用第一期建立的2H核磁共振数据库来研究氢在过渡金属纳米粒子（钌、钯、铂）上的吸附。最后，我们希望研究H4Ru4(CO)12团簇的氢动力学，揭示动力学过程的性质及其能量参数。