Modeling of Catalytic Bond Functionalization by Base and Noble Metal Catalysts

在这个由化学部化学催化项目资助的项目中，北德克萨斯大学的Thomas R. Cundari将使用最先进的计算化学模型来研究过渡金属催化。本文将对铜催化剂在烃类胺化反应中的应用进行综述。与实验合作者一起，将对第一代催化剂进行改进，以提高活性、选择性和底物范围。这些铜配合物利用锌的衍生物将被研究，以潜在地扩展这一催化剂家族，并描绘重要的化学。钯催化剂的研究将为理解贱金属取代贵金属催化剂提供基础。NSF的资金也将支持分析均相（分子）和非均相（固态）催化之间的关键联系。更广泛的影响包括在跨学科的研究环境中培养研究生和本科生，为学生与教师和学生之间的指导提供机会，并通过在会议上发表报告和在期刊上发表文章广泛传播研究成果。过渡金属元素的催化作用对于开发急需的下一代技术至关重要，例如将温室气体二氧化碳催化还原为液体燃料、更高效的太阳能电池和更节能的分子电子产品。所提出的研究将揭示与过渡金属催化剂相关的基本见解，这反过来可以积极影响许多应用，如碳氢化合物精炼，生物质利用作为化学原料，以及精细化工生产。

In this project funded by the Chemical Catalysis Program of the Chemistry Division, Thomas R. Cundari of the University of North Texas will use state-of-the-art computational chemistry modeling to study transition metal catalysis. Promising copper catalysts for hydrocarbon amination will be elucidated. In conjunction with experimental collaborators, modifications to first-generation catalysts will be sought with enhanced activity, selectivity, and substrate scope. Derivatives of these copper complexes that utilize zinc will be studied to potentially extend this family of catalysts, and to delineate important chemistry. Palladium catalysts will be researched to provide a foundation to understand base metal replacements for precious metal catalysts. NSF funding also will support analysis of the critical linkage between homogeneous (molecular) and heterogeneous (solid-state) catalysis. The broader impacts involve training graduate and undergraduate students in an interdisciplinary research environment, providing opportunities for student-teacher and student-student mentorship, and disseminating research results broadly through presentations at conferences and publications in journals.Catalysis via transition metal elements is vital to development of much needed, next-generation technologies, such as the catalytic reduction of the greenhouse gas carbon dioxide to liquid fuels, more efficient solar cells, and more energy efficient molecular electronics. The proposed research will reveal fundamental insights relevant to transition metal catalysts, which can in turn positively impact many applications such as hydrocarbon refining, biomass utilization as chemical feedstocks, and fine chemical production.