Development of Catalytic Cyclization/Coupling Reactions for New Chemical Space

在化学系化学催化计划的支持下，宾夕法尼亚州立大学的Ramesh Giri博士正在开发催化剂，将烯烃转化为环状分子，然后将它们连接到另一个烃片段。在这项工作中，密切关注地球丰富的过渡金属催化剂，特别是那些基于镍和铜的使用。 这项工作正在解决更有效的方法来制造复杂分子的需求，这些分子对于支持新药物和材料的发现至关重要。Giri博士和他的研究团队正在研究的催化剂用于在一个步骤中构建两个碳-碳键，以快速获得增值产品，并减少效率较低的迭代过程中积累的浪费。选择性元素也被纳入到催化剂设计中，以控制使用这种技术可以产生的复杂分子的精细结构。该项目的理念、概念和产品通过外展活动与当地高中分享，通过可持续发展的透镜培养化学科学的批判性思维。Ramesh Giri博士和他的研究团队正在开发催化剂，以推进烯烃双官能化反应的环化/偶联策略。该计划的三个目标旨在解决反应设计这一领域长期存在的挑战和新方向的组合。β-氢化物消除是环化/偶联反应中的竞争过程，其显著限制了这些转化的范围。Giri集团正在设计新的催化剂和催化剂-配体组合，以避免这一经典的基本挑战。为了进一步扩大环化/偶联策略的范围，以获得更广泛的复杂分子，该研究计划还测试了新的烯胺和甲硅烷基烯醇醚底物，以及探索具有可裂解系链的线性化底物。这些活动为不同的研究生和本科生提供了催化、反应设计和机理研究方面的培训机会。该奖项反映了NSF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, Dr. Ramesh Giri of The Pennsylvania State University is developing catalysts that convert alkenes to cyclic molecules and then link them to another hydrocarbon fragment. In this work, close attention is paid to the use of earth-abundant transition metal catalysts, particularly those based upon Ni and Cu. This work is addressing the need for more efficient ways to make complex molecules that are critical to support the discovery of new pharmaceuticals and materials. The catalysts that Dr. Giri and his research team are studying are used to construct two carbon-carbon bonds in a single step to rapidly access value-added products and decrease the waste that accumulates from less efficient iterative processes. Selectivity elements are also being incorporated into catalyst design to control the fine structure of the complex molecules that can be generated using this technology. The ideas, concepts, and products of this work are being shared with local high schools through outreach activities to foster critical thinking in chemical science through the lens of sustainability.Dr. Ramesh Giri and his research team are developing catalysts to advance cyclization/coupling strategies for alkene difunctionalization reactions. The three objectives of the program seek to tackle a combination of long-standing challenges and new directions in this area of reaction design. Beta-hydride elimination is a competing process in cyclization/coupling reactions that has significantly limited the scope of these transformations. The Giri group is designing new catalysts and catalyst-ligand combinations to avoid this classic fundamental challenge. To further broaden the scope of cyclization/coupling strategies towards accessing a broader range of complex molecules, this research program is also testing new enamine and silyl enol ether substrates, as well as exploring linearizable substrates with cleavable tethers. These activities are providing training opportunities for a diverse group of graduate and undergraduate students in catalysis, reaction design, and mechanistic study.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.