Synthesis, Reactivity, and Catalytic Studies of Mixed-Metal Gold Cluster Compounds

这个无机、生物无机和有机金属项目的奖项为明尼苏达大学化学系的Louis H. Pignolet博士对含金、铂和钯的混合金属簇化合物的研究提供了持续的支持。Pignolet将合成额外的更大的簇分子，包含更多种类的金属，并使用更小的磷化氢配体。最近，Pignolet观察到氢分子可以在这些团簇表面与氘分子平衡。他希望探索这种相互作用的机制，并描述所涉及的物种。他还将研究这些团簇在均相和非均相条件下加氢的催化活性。采用TEM、XPS、化学吸附和其他表面方法对催化剂体系进行表征。许多工业催化剂含有金属的混合物，据推测，这些催化剂的有效性取决于各种金属之间的协同相互作用。含有8到20个金属原子的混合金属团簇被认为是了解这种催化活性细节的有用模型化合物。在这个项目中，Pignolet将制作更大、更多样化的团簇，并减少金属上稳定磷化氢基团的大小，从而提高团簇的催化效能。团簇的催化行为将被研究，特别是对加氢催化，自由团簇和氧化铝支持团簇将被研究。研究结果有助于进一步了解影响催化剂反应性的因素。

This award in the Inorganic, Bioinorganic, and Organometallic Program provides continued support to Dr. Louis H. Pignolet of the Chemistry Department, University of Minnesota, for the investigation of mixed metal cluster compounds containing gold, platinum, and palladium. Pignolet will synthesize additional cluster molecules that are larger, contain a wider variety of metals, and use less bulky phosphine ligands. Recently, Pignolet has observed that hydrogen molecules can equilibrate with deuterium molecules on the surface of these clusters. He wishes to explore the mechanism of this interaction and characterize the species involved. He would also study the catalytic activity of these clusters upon hydrogenation under both homogeneous and heterogeneous conditions. The catalyst systems would be characterized using TEM, XPS, chemisorption and other surface methods. %%% Many industrial catalysts contain a mixture of metals, and it is speculated that the effectiveness of these catalysts depends on a synergistic interaction between the various metals. Mixed metal clusters, containing eight to twenty metal atoms, have been postulated as useful model compounds for understanding the details of such catalytic activity. In this project, Pignolet will make larger and more varied clusters and reduce the size of the stabilizing phosphine groups attached to the metals so as to enhance the cluster's catalytic effectiveness. The catalytic behavior of the clusters will be investigated, particularly for hydrogenation catalysis, and both free and alumina-supported clusters will be studied. The results could provide increased understanding of the factors affecting the reactivity of catalysts.