Model Nanocluster Catalysts: The Role of Size, Shape and Composition on the Catalytic Activity of Monometallic, Bimetallic and Metal Oxide Clusters on Oxide Surfaces

在这项由分析和表面化学项目支持的研究中，Buratto、Bowers和Metiu教授及其团队将制备、表征和测试三种新型纳米级催化剂，它们具有一个共同特征：非常小、分离、定义明确、催化活性位点。他们将制备和研究(a)在氧化物上支撑的非常小的石墨烯和Agn团簇，(b)在氧化物上支撑的非常小的石墨烯和Agn团簇，以及(c)在氧化物上支撑的非常小的石墨烯和Agn团簇。将采用多种技术，以协调一致的方式来研究这些重要的催化过程：模型催化系统将通过在氧化物表面沉积大量选择的团簇来制备，以确保对催化剂尺寸的原子逐个控制；所有样品将在催化化学之前、期间和之后通过表面科学技术（AES， XPS）以及STM/ AFM在超高真空中制备和研究；和密度泛函理论（DFT）将用于计算团簇的结构、XPS谱和化学活性。通过这里提出的工作，他们将对这些材料的催化化学有一个详细的了解，并找出这种化学是如何依赖于基材的大小、组成和性质的。虽然研究的重点是特定纳米级催化剂的催化活性，但研究结果很有可能适用于其他体系。此外，希望通过本研究开发的概念将有助于优化使用这些纳米级催化剂的重要工业过程，并为发现新的纳米级催化材料提供见解。这项资助的研究将是跨学科的。研究生将与三个不同的研究小组持续互动，每天与其他杰出的科学家接触，并将获得大量表面科学、气相化学、扫描探针显微镜和高级理论技术的实践经验。这项研究将为研究生教育提供一个宝贵的机会，这在世界上很少有地方能找到。该基金支持的研究人员（包括pi）也将积极地拓展到圣巴巴拉地区的K-12学校，提供关于多相催化的原子观的教程，并展示我们的模型催化剂系统的原子分辨图片。这将包括在UCSB化学系目前正在进行的外展项目中。一系列关于纳米结构催化的讲座将被开发，并作为目前材料化学课程中纳米科学课程的一部分。

In this research supported by the Analytical and Surface Chemistry Program, Professors Buratto, Bowers, and Metiu and their groups will prepare, characterize, and test three new types of nanoscale catalysts, having one feature in common: very small, isolated, well-defined, catalytically active sites. They will prepare and study (a) very small Aun and Agn mass-selected clusters supported on oxide, (b) very small mass-selected, binary clusters such as PdmAun supported on oxides, and (c) very small, mass-selected oxide clusters supported on oxides. A variety of techniques will be used, in a concerted manner, to study these important catalytic processes: model catalytic systems will be prepared by depositing mass-selected clusters on oxide surfaces to ensure atom-by-atom control of catalyst size; all samples will be prepared and studied in ultra-high vacuum by surface science techniques (AES, XPS) as well as by STM/ AFM before, during and after the catalytic chemistry; and density functional theory (DFT) will be used to calculate the structure of the clusters, their XPS spectrum and their chemical activity. Through the work proposed here they will develop a detailed understanding of the catalytic chemistry of these materials and find out how this chemistry depends on size, composition and the nature of the substrate. While the focus of the research is on the catalytic activity of specific nanoscale catalysts, there is a high probability that the results will be applicable to other systems. In addition, it is hoped that the concepts developed through this research will help optimize important industrial processes using these nanoscale catalysts and provide insight into the discovery of new nanoscale catalytic materials.The research funded by this grant will be interdisciplinary. Graduate students will interact continuously with three different research groups, will have daily contact with other outstanding scientists, and will acquire hands-on experience in a large number of techniques of surface science, gas-phase chemistry, scanned probe microscopy, and high level theory. The research will provide a valuable opportunity for graduate education, found in very few places in the world. Researchers supported by this grant (including PIs) will also be active in outreach to K-12 schools in the Santa Barbara area to present a tutorial on an atomistic view of heterogeneous catalysis and to show an atomically-resolved picture of our model catalyst systems. This will be included in the currently active outreach program in the chemistry department at UCSB. A series of lectures on catalysis by nanostructures will be developed and included as part of a course in nanoscience currently taught in the materials chemistry curriculum.