Developing Foundations for Catalyst Design: From Cluster Science to Industrial Applications

在GOALI倡议下的实验物理化学计划的资助下，A。宾夕法尼亚州立大学的Welford Castleman将进行研究，旨在为过渡金属氧化物催化剂的设计提供科学依据，这些催化剂将有效地选择性活化碳-碳和碳-氢键，并确定促进与几类有机分子的氧转移反应所需的性质。引导离子束串联质谱技术将采用，以了解钒，铌和钽氧化物簇离子的催化活性。 目标是研究化学计量、尺寸、结构、电离势、电荷和氧化态对氧原子转移到各种有机分子以及C-C和C-H键活化的影响，并深入了解这些反应的机制。 此外，金属氧化物团簇的结构将进一步探测使用碰撞诱导解离技术。 这些结果与相关的凝聚相反应的比较将导致更好的理解反应物物种与催化表面的活性位点的相互作用。 PI组的学生将与杜邦中央研究与开发部的工业科学家合作进行相关研究，他们在固态化学和多相催化方面拥有丰富的经验。 气相研究的新发现将用于探索有希望作为新催化剂开发的材料。催化剂引起化学反应过程的变化，例如增加其速率或导致产生不同的最终产物，而催化剂本身在最后保持化学不变。 催化继续对经济产生巨大的影响，但设计催化剂的能力，将导致高选择性形成所需的产品，最小的环境影响仍然是基本的。过渡金属氧化物作为催化剂变得越来越重要，因为它们能够进行有用的反应，并且具有成本效益并且通常是环境友好的。这种学术/工业合作预计将提供见解，最终导致改进催化剂的开发。

In a grant supported by Experimental Physical Chemistry Program under the GOALI initiative, A. Welford Castleman of the Pennsylvania State University will perform studies that aim to provide a scientific basis for tailoring the design of transition metal oxide catalysts which will be effective in the selective activation of carbon-carbon and carbon-hydrogen bonds, and to determine the properties necessary to promote oxygen-transfer reactions with several classes of organic molecules. Guided ion beam tandem mass spectrometry techniques will be employed in order to understand the catalytic activity of vanadium, niobium, and tantalum oxide cluster ions. The objectives are to investigate the influence of stoichiometry, size, structure, ionization potentials, charge, and oxidation state on the transfer of oxygen atoms to various organic molecules as well as C-C and C-H bond activation, and to gain insights into the mechanisms of these reactions. Additionally, the structures of metal oxide clusters will be probed further using collision-induced dissociation techniques. Comparisons of these results with related condensed phase reactions will lead to improved understanding of the interaction of reactant species with active sites of catalytic surfaces. Students from the PI group will pursue related research in collaboration with industry scientists from DuPont Central Research and Development who have broad experience in solid state chemistry and heterogeneous catalysis. New findings from the gas phase studies will be implemented in exploring materials that have promise for development as new catalysts. A catalyst causes changes in a chemical reaction process, such as increasing its rate or causing different end products to be produced, while the catalyst itself remains chemically unaltered at the end. Catalysis continues to have an enormous impact on the economy, yet the ability to design catalysts that will lead to highly selective formation of desired products with minimal environmental effect is still rudimentary. Transition metal oxides are becoming increasingly important as catalysts because they enable useful reactions and are cost efficient and often environmentally benign. This academic/industrial collaboration is expected to provide insights that will ultimately lead to the development of improved catalysts.