Modeling of Catalytic Bond Functionalization by Base and Noble Metal Catalysts

在这个由化学系化学催化计划资助的项目中，北得克萨斯大学的托马斯·R·昆达里将使用最先进的计算化学模型来研究过渡金属催化。在碳氢化合物胺化反应中，铜催化剂的前景将被阐明。与实验合作者一起，将寻求对第一代催化剂进行改进，以提高活性、选择性和底物范围。这些利用锌的铜配合物的衍生物将被研究，以潜在地扩展这一催化剂家族，并描述重要的化学。将对钯催化剂进行研究，为理解贵金属催化剂的贱金属替代提供基础。NSF的资助还将支持分析均相(分子)和多相(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训研究生和本科生，为学生和教师以及学生和学生提供指导的机会，以及通过在会议和期刊上发表演讲来广泛传播研究成果。通过过渡金属元素的催化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减少为液体燃料、更高效的太阳能电池和更节能的分子电子学。拟议的研究将揭示与过渡金属催化剂相关的基本见解，这些催化剂反过来可以对许多应用产生积极影响，如碳氢化合物精炼、生物质用作化工原料和精细化工生产。

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.