RUI: Anionic Multitopic N-Heterocyclic Carbenes: Building Blocks for Molecular and Supramolecular Architectures

化学系的化学合成计划支持肯纳索州立大学的Daniela Tapu教授研究一系列刚性配体的合成和表征，这些配体旨在支持多金属配合物和超分子笼子。这个项目挑战了传统的化学键和结构模型。了解这些新化合物的分子结构、电子结构和化学反应活性之间的关系，可能会开发出更有效的均相和多相催化剂，并可能导致促进它们回收的策略。这项研究有可能对催化工业和学术研究产生积极的影响。更广泛的影响包括对本科生和硕士研究生的培训和指导，包括来自低收入家庭和传统上在STEM学科中代表性较低的群体的学生。该项目的目标是一种可应用于配位化学和催化的新型刚性阴离子多主题非螯合N-杂环卡宾(NHCS)。这些卡宾作为一系列两性离子双金属和三金属配合物以及金属超分子系统的构建块，这些新的结构是目前的NHC配体无法访问的。这些任务的核心是开发新的合成方法和战略，以促进目标分子的合成和对其催化性能的评价。拟议的工作将提供广泛的学生培训，从开发获得目标卡宾及其络合物的合成方法到表征它们的物理和电子结构，再到研究它们的反应性。

The Chemical Synthesis program of the Chemistry Division supports Professor Daniela Tapu from Kennesaw State University to investigate the synthesis and characterization of a series of rigid ligands that are designed to support multimetallic complexes and supramolecular cages. This project challenges conventional models of chemical bonding and structure. Understanding the relationship between molecular architecture, electronic structure and chemical reactivity of these new compounds may allow the development of more efficient homogeneous and heterogeneous catalysts, and may lead to strategies to facilitate their recovery. This research has the potential to positively impact both the catalysis industry and academic research. Broader impacts include the training and mentoring of undergraduate and M.S. students including students from lower income families and groups traditionally underrepresented in the STEM disciplines.This project targets a pallet of novel rigid anionic multitopic non-chelating N-heterocyclic carbenes (NHCs) that can be applied in coordination chemistry and catalysis. These carbenes function as building blocks for a series of zwitterionic bi- and tri-metallic complexes, as well as metallosupramolecular systems, novel architectures that are not accessible with the current NHC ligands. Central to these tasks are the development of new synthetic methodologies and strategies to facilitate the synthesis of the target molecules and the evaluation of their catalytic properties. The proposed work will provide broad-based student training from developing synthetic methods to access the targeted carbenes and their complexes to characterizing their physical and electronic structures, to studying their reactivities.