Theory and Design of Dinuclear Catalytic Reactions

在化学系化学催化项目的支持下，杨百翰大学的Daniel Ess专注于推进化学中双核催化反应的理论和设计。开发新的催化剂对于发现新的、有效的化学反应至关重要。从历史上看，均相催化剂只使用一个金属原子作为催化剂的核心。相比之下，双核催化剂在催化剂的核心有两个金属原子，在新的设计和操作模式方面有很大的希望。双核催化剂还有望加速目前单金属催化剂表现不佳的历史上缓慢/困难的化学反应。目前，研究科学家并不完全了解双核催化剂如何促进快速反应，或者哪些双核催化剂应该成为特定化学转化的合成目标。在这个项目中，Daniel Ess博士将使用计算方法和理论分析来理解这种双核金属系统催化反应的机制和选择性。这项工作与实验合作紧密结合，将导致新的双核催化剂和化学反应的预测和实验发现。这项工作还将为化学和计算机科学之间的界面的本科生和研究生以及博士后提供培训。杨百翰大学的Daniel Ess正在使用量子化学方法和理论分析来模拟和理解有机转化的过渡金属异双核和同双核催化剂。所研究的双核催化剂的核心是两个过渡金属之间的直接键合。研究了C-H键功能化、C-O键还原和脱氢的反应机理。碳氢化合物半氢化反应、环化反应和立体选择性加成反应的选择性将是这些研究的重点。这项工作将结合量子化学方法和机器学习技术来设计新的异核催化剂。本科生、研究生和博士后学者将接受先进计算技术方面的培训。学生和博士后将直接与几个实验组互动，并学习如何在实验环境中应用计算化学技术。该奖项反映了美国国家科学基金会的法定使命，并通过使用基金会的知识价值和更广泛的影响审查标准进行评估，被认为值得支持。

With support from the Chemical Catalysis program in the Division of Chemistry, Daniel Ess of Brigham Young University is focused upon advancing the theory and design of di-nuclear catalytic reactions in chemistry. Developing new catalysts is critical to discovering new, efficient chemical reactions. Historically, homogeneous catalysts use just one metal atom at the core of the catalyst. In contrast, dinuclear catalysts have two metal atoms at the core of the catalyst and have significant promise for new designs and modes of operation. Dinuclear catalysts also hold promise for speeding up historically slow/difficult chemical reactions where current single metal catalysts do not perform well. Currently, research scientists do not fully understand how dinuclear catalysts facilitate rapid reactions, or which dinuclear catalysts should be the target of synthesis for specific chemical transformations. In this project Dr. Daniel Ess will be using computational methods and theoretical analysis to understand mechanisms and selectivity of reactions catalyzed by such dinuclear metal systems. This work, interfaced tightly with experimental collaboration, will lead to the prediction and experimental discovery of new dinuclear catalysts and chemical reactions. This work will also provide training for undergraduate and graduate students as well as postdoctoral scholars at the interface between chemistry and computer science.Daniel Ess of Brigham Young University is using quantum-chemical methods and theoretical analyses to model and understand transition-metal heterodinuclear and homodinuclear catalysts for organic transformations. The dinuclear catalysts being investigated have direct bonding between two transition metals as the core of the catalyst. Reaction mechanisms will be investigated for C-H bond functionalization, C-O bond reduction, and dehydrogenation. Selectivity for hydrocarbon semi-hydrogenation, for cyclization reactions, and for stereoselective addition reactions will be the foci of these investigations. This work will be combining quantum-chemical methods and machine learning techniques to design new heterodinuclear catalysts. Undergraduate and graduate students and postdoctoral scholars will be trained in advanced computational techniques. Students and postdocs will interact directly with several experimental groups and learn how to apply computational chemistry techniques in an experimental environment.This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.