Discovering Design Criteria in Early Transition Metal Catalysis

在化学系化学催化项目的支持下，密歇根州立大学的Aaron Odom教授正在研究催化剂优化新方法的发展。2008年，北美催化学会估计，催化通过改善燃料、能源、排放、聚合物、天然和生物改性酶、制药生产和食品，对全球GDP的贡献超过35%。这些类别每年占世界经济的10多万亿美元。虽然优化低氧化态过渡金属催化剂的方法已经研究了50多年，但优化高氧化态过渡金属体系的类似方法却几乎没有发展。因此，高氧化态催化剂通常通过筛选许多不同的化合物而进行低效和不系统的优化。奥多姆小组正在开发方法来解决这一差距，并设计改进的路线，以优化工业上常用的高氧化态富土催化剂体系。这些活动将为密歇根州立大学的研究生和本科生提供专业培训。作为该项目的一部分，奥多姆教授和他的研究生们还将为当地的K-12学生和在家上学的儿童组织外展活动。奥多姆研究小组已经开发了一种方法参数化辅助配体供体能力的高氧化态金属。使用电子参数，指定配体供体参数或LDP，结合配体大小的参数，可以确定催化剂结构变化时反应行为的数学模型。这个模型可以用来预测新的配合物的行为，并发现关于催化剂如何工作的新信息。奥多姆教授和他的研究小组目前正在通过研究更复杂的催化系统，如三组分偶联，以及研究在烯烃寡聚过程中结合中性和阴离子供体的配体，来推进这一系统。在第三个研究方向上，奥多姆团队也致力于将这种预测配体结构-功能策略扩展到f元素催化剂上。这些努力有望为催化剂优化提供新的假设驱动途径，并提高对高氧化态过渡金属催化剂中配体加速效应的理解。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 the support of the Chemical Catalysis Program in the Division of Chemistry, Professor Aaron Odom of Michigan State University is studying the development of new approaches to catalyst optimization. In 2008, the North American Catalysis Society estimated that catalysis contributes greater than 35% of the global GDP through improvements in fuels, energy, emissions, polymers, natural and biomodified enzymes, pharmaceutical production, and food. These categories account for over 10 trillion dollars of the annual world economy. While methods for optimization of low oxidation state transition metal catalysts have been studied for over 50 years, similar methods for optimizing high oxidation state transition metal systems have seen little development. As a result, high oxidation state catalysts are often optimized inefficiently and unsystematically by screening many different compounds. The Odom group is developing methods to address this gap and design improved routes to the optimization of high oxidation state earth abundant catalyst systems that are often used industrially. These activities will providing professional training for a diverse group of graduate and undergraduate students at Michigan State University. Also as part of this project, Professor Odom and his graduate students also will organize outreach activities to local K-12 students and home-schooled children.The Odom research group has developed a method for parameterizing ancillary ligand donor ability for high oxidation state metals. Using an electronic parameter, designated Ligand Donor Parameter or LDP, in conjunction with a parameter for the size of the ligand, a mathematical model for how the reaction behaves with changes in catalyst structure can be determined. This model can then be used to anticipate how new complexes will behave and discover new information about how catalysts work. Professor Odom and his research team are currently advancing this system through the investigation of more complicated catalytic systems such as a three-component coupling and studying ligands that incorporate neutral as well as anionic donors in olefin oligomerization. In a third research direction, the Odom group is also working towards expanding this predictive ligand structure-function strategy toward f-element catalysts. These efforts are expected to provide new hypothesis-driven routes to catalyst optimization and improved understanding of ligand acceleration effects in high oxidation state transition metal catalysts.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.