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氧化物和沸石负载的分子金属配合物与簇合物:物理表征以及结构、键合和金属氧化态的测定

Oxide- and zeolite-supported molecular metal complexes and clusters: physical characterization and determination of structure, bonding, and metal oxidation state.

作者信息

Fierro-Gonzalez Juan C, Kuba Stefan, Hao Yalin, Gates Bruce C

机构信息

Department of Chemical Engineering and Materials Science, University of California, Davis, California 95616, USA.

出版信息

J Phys Chem B. 2006 Jul 13;110(27):13326-51. doi: 10.1021/jp0571123.

DOI:10.1021/jp0571123
PMID:16821852
Abstract

This article is a review of the physical characterization of well-defined site-isolated molecular metal complexes and metal clusters supported on metal oxides and zeolites. These surface species are of interest primarily as catalysts; as a consequence of their relatively uniform structures, they can be characterized much more precisely than traditional supported catalysts. The properties discussed in this review include metal nuclearity, oxidation state, and ligand environment, as well as metal-support interactions. These properties are determined by complementary techniques, including transmission electron microscopy; X-ray absorption, infrared, Raman, and NMR spectroscopies; and density functional theory. The strengths and limitations of these techniques are assessed in the context of results characterizing samples that have been investigated thoroughly and with multiple techniques. The depth of understanding of well-defined metal complexes and metal clusters on supports is approaching that attainable for molecular analogues in solution. The results provide a foundation for understanding the more complex materials that are typical of industrial catalysts.

摘要

本文是对负载于金属氧化物和沸石上的结构明确的位点隔离分子金属配合物和金属簇的物理特性的综述。这些表面物种主要作为催化剂受到关注;由于其结构相对均匀,与传统负载型催化剂相比,它们能够得到更精确的表征。本综述中讨论的性质包括金属核数、氧化态、配体环境以及金属-载体相互作用。这些性质通过多种互补技术来确定,包括透射电子显微镜、X射线吸收光谱、红外光谱、拉曼光谱和核磁共振光谱以及密度泛函理论。在利用多种技术对样品进行深入研究的结果背景下,评估了这些技术的优势和局限性。对负载型结构明确的金属配合物和金属簇的理解深度正在接近对溶液中分子类似物所能达到的理解深度。这些结果为理解工业催化剂中典型的更复杂材料奠定了基础。

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