US-Federal Republic of Germany Cooperative Research: Supported Metal Catalysts with Unique Structures Derived from Molecular Metal Clusters

该奖项支持特拉华大学催化科学与技术中心的Bruce C. Gates博士与德国慕尼黑大学物理化学研究所的Helmut Knoezinger博士合作进行研究。他们对催化和表面化学有共同的兴趣，并正在合作研究由有机金属前体在碱性金属氧化物载体上制备的新型金属催化剂。他们使用的前体包括铼、铑、锇、铱和铂。支撑材料包括氧化镁、氧化镧和氧化钙。催化剂包括单核配合物的集合，强健的阴离子金属团簇，以及通过从分子金属团簇中去除配体而形成的具有独特核的金属聚集体。在制备了各种负载催化剂后，他们将确定其结构并表征表面结合簇的反应性。他们还将通过实验确定它们的催化活性、选择性和工业上重要测试反应的稳定性。这项工作将基于两个研究小组的互补性专业知识和设施进行共享。Knoezinger博士在表面物理化学和光谱学方面拥有专业知识，Gates博士更多地从事表面有机金属合成和使用流动反应器技术详细表征催化剂性能的工作。因此，催化剂将在特拉华州制备，分析和实验测试将在两个实验室进行，具体取决于合适的设备和可用人力的位置。本研究将促进对具有分子结构的金属氧化物负载型金属催化剂的结构和催化活性的基本认识。它还可以阐明分子金属簇在迄今为止被认为是传统负载金属催化剂中的作用。通过建立分子金属络合催化剂、簇催化剂和传统负载型金属催化剂之间的联系，为开发分子前驱体制备新型催化材料指明了可能的途径。

This award supports Dr. Bruce C. Gates of the Center for Catalytic Science and Technology, University of Delaware, to collaborate in research with Dr. Helmut Knoezinger of the Institute for Physical Chemistry, University of Munich, FRG. They share an interest in catalysis and surface chemistry, and are collaborating in a study of new classes of metal catalysts prepared from organometallic precursors on basic metal oxide supports. The precursors they are using include rhenium, rhodium, osmium, iridium and platinum. The supports include magnesium oxide, lanthanum oxide and calcium oxide. The catalysts include ensembles of mononuclear complexes, robust anionic metal clusters, and metal aggregates with unique nuclearities formed by removal of ligands from molecular metal clusters. After preparing a variety of supported catalysts, they will determine their structures and characterize the reactivities of surface bound clusters. They will also experimentally determine their catalytic activities, selectivities and stabilities for industrially important test reactions. The work will be shared based on the complementary expertise and facilities of the two research groups. Dr. Knoezinger has expertise in surface physical chemistry and spectroscopy and Dr. Gates has worked more with surface organometallic synthesis and detailed characterization of catalyst performance using flow-reactor techniques. Therefore, the catalysts will be prepared in Delaware and the analyses and experimental testing will be done in both laboratories, depending on where the appropriate equipment and available manpower is located. This research will advance fundamental understanding of the structures and catalytic activities of metal oxide-supported metal catalysts having molecular structures. It may also elucidate the role of molecular metal clusters in what have heretofore been considered conventional supported metal catalysts. By making the connection between molecular metal complex catalysts and cluster catalysts and conventional supported metal catalysts, it will point the way to possible exploitation of the molecular precursors in the preparation of novel catalytic materials.