Well-defined Supported Metal Catalysts Synthesized From Organometallics

金属羰基前驱体用于合成结构独特的氧化负载的有机金属和金属催化剂，包括稳定分子金属簇阴离子的坚固类似物和通过去除羰基配体由它们形成的金属聚集体。这项工作主要集中在锇、铱和铂的镁支持上。表征了载体的结构和稳定性。这些聚合体中较稳定的聚合体进行了催化活性测试。这项工作旨在弥合金属配合物和配位簇行为（具有大量文献的化学分支）与支撑金属催化剂行为（工业应用中首选的类型）之间的差距。这将提高我们对催化剂对金属结构和金属-载体相互作用的敏感性的理解，并在设计实用催化剂方面取得重大进展。

Metal carbonyl precursors are used to synthesize structurally unique oxide-supported organometallic and metallic catalysts including robust analogues of stable molecular metal-cluster anions and metal aggregates formed from them by removal of the carbonyl ligands. The effort concentrates on osmium, iridium, and platinum on magnesia support. Structures and stabilities of the supported species are characterized. The more stable of these aggregates are tested for catalytic activity. This effort is designed to bridge the gap between metal complexes and coordination cluster behavior (a branch of chemistry with a voluminous literature) and the behavior of supported metal catalysts (the type preferred in industrial applications). This should improve our understanding of the sensitivity of catalysis to metal structure and metal-support interactions and be a major advance in the design of practical catalysts.