CAREER: Catalytic C-C Bond Formation and Cleavage at Cobalt: Mechanism, Origins and Application

在这项由化学系化学催化计划资助的职业奖项中，来自布朗大学的Wesley Bernskoetter教授正在研究地球上丰富的金属中选择性双电子、碳-碳键转化的机制路径和起源。特别是，催化应用所需的介导碳-碳键还原消除和氧化加成反应的强场钴络合物是目标。这些基础研究考察了配体场强、自旋态相互转化和配位几何结构等因素，这些因素可能会影响这些转换的速度和选择性。这项研究将进一步利用贱金属作为铂族金属催化的替代品，反应范围从交叉偶联到碳氰化。与研究工作相一致，该项目正在通过同伴指导和教程以及通过为大学预科学生提供基于发现的物理科学介绍来加强对本科生的培训。各种制造业依靠金属催化，以高能效和低成本的方式生产化学品和材料。在过去的几十年里，由金属催化剂促进的重要新催化反应的数量有了显著的增长；然而，这些发现中使用的金属主要来自一组昂贵的、稀有的和有毒的金属。这项研究项目寻求开发使用更丰富、更便宜、潜在毒性更低的金属来完成一些同样重要的催化反应的方法。这项工作的未来影响可能包括开发更经济和可持续的制造技术。该项目还将包括对下一代研究科学家的专业培训，以及为大学预科学生提供发现科学在社会中重要地位的机会。

In this CAREER award funded by the Chemical Catalysis Program of the Chemistry Division, Professor Wesley Bernskoetter from Brown University is investigating the mechanistic pathways and origins of selective two-electron, carbon-carbon bond transformations at earth abundant metals. In particular, strong field cobalt complexes that mediate carbon-carbon bond reductive elimination and oxidative addition reactions necessary for catalytic applications are being targeted. These fundamental studies examine factors such as ligand field strength, spin state interconversion, and coordination geometry, which may influence the rate and selectivity of these transformations. This research will further the utilization of base-metals as surrogates for platinum group metal catalysis in reactions ranging from cross-coupling to carbocyanation. In concert with the research endeavors, this project is enhancing the training of undergraduate students through peer mentoring and tutorials as well as through a discovery-based introduction to physical sciences for pre-college students. A variety of manufacturing industries rely on metal-based catalysis to produce chemicals and materials in an energy efficient and cost-effective manner. The past decades have witnessed a significant growth in the number of important new catalytic reactions promoted by metal catalysts; however, the metals employed in these discoveries have largely come from a group of expensive, rare, and toxic metals. This research project seeks to develop routes to accomplish some of the same important catalytic reactions using metals that are much more abundant, less expensive, and potentially less toxic. Future impacts of the work could include the development of more economical and sustainable manufacturing technologies. This project will also include professional training for the next generation of research scientists and opportunities for pre-college students to discover the important place of science in society.