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资助下，宾夕法尼亚州立大学的A·韦尔福德·卡斯特尔曼将进行研究，旨在为过渡金属氧化物催化剂的设计提供科学基础，该催化剂将有效地选择性激活碳-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。导引离子束串联质谱技术将被用来了解钒、铌和氧化钽团簇离子的催化活性。研究的目的是研究化学计量比、尺寸、结构、电离势、电荷和氧化态对氧原子向各种有机分子的转移以及C-C和C-H键活化的影响，并深入了解这些反应的机理。此外，还将使用碰撞诱导解离技术进一步探索金属氧化物团簇的结构。将这些结果与相关的凝聚相反应进行比较，将有助于更好地理解反应物物种与催化剂表面活性中心之间的相互作用。PI小组的学生将与杜邦中央研究和开发公司的行业科学家合作进行相关研究，这些科学家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应用于探索有希望作为新催化剂开发的材料。催化剂会引起化学反应过程中的变化，例如增加反应速度或产生不同的最终产品，而催化剂本身在结束时保持化学上的不变。催化作用继续对经济产生巨大影响，然而，设计催化剂的能力仍处于初级阶段，能够以最小的环境影响产生高选择性地形成所需的产品。过渡金属氧化物作为催化剂正变得越来越重要，因为它们能够进行有用的反应，而且具有成本效益，而且往往对环境无害。这种学术/工业合作有望提供见解，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.