RUI: Novel Fe Catalysts for Alcohol Amine Coupling Reaction to Imine

化学系化学催化项目将资助田纳西中部州立大学的丁凯英教授开发一种新型的富含稀土的催化剂，用于有用的偶联反应。目标化学结构亚胺代表了一类非常重要的化合物，在化学、制药和生物领域有着广泛的应用。目前，这种偶联反应使用的贵金属催化剂价格昂贵，有时甚至有毒，而且供应有限。因此，当今最常见的方法会带来经济挑战，而且往往还会带来环境挑战。利用富含地球的金属系统开发此类反应的催化过程符合可持续的化学目标。在这方面的成功也可能会吸引制药工艺集团和工业化学家的注意。这项研究的更广泛的影响包括为本科生、硕士水平的研究人员和高中生提供培训机会和实践研究经验，包括那些来自代表不足的群体和低收入背景的人。在这个项目中，丁克英教授正在设计、合成和表征新型配体及其各自定义的铁配合物，这些配合物具有“金属-配体协作性”。丁教授正在研究它们在温和条件下对醇-胺偶联的催化反应性。在目前研究的体系中，配体不仅作为金属结合部位，还直接参与化学键的活化。该项目正在探索醇和胺的最佳反应条件和底物范围。通过实验和理论相结合的研究，正在研究重要的反应中间体和催化机理，这将丰富对此类转化的非贵金属催化的基本认识，并将为高选择性催化剂的设计提供新的见解。

With this award, the Chemical Catalysis Program of the Chemistry Division is funding Professor Keying Ding from Middle Tennessee State University to develop a novel types of earth-abundant catalysts for a useful coupling reaction. The target chemical structures, imines, represent a very important class of compounds with applications in the chemical, pharmaceutical and biological sectors. Currently, such coupling reactions employ precious metal catalysts that are expensive,sometimes toxic, and limited in supply. Thus, the most common approaches today pose economic and often environmental challenges. Developing catalytic processes for such reactions with earth-abundant metal systems is compatible with sustainable chemistry goals. Success here would also likely capture the attention of pharmaceutical process groups and industrial chemists. The broader impacts of the research include training opportunities and hands-on research experiences for undergraduate students, master-level researchers and high school students, including those from underrepresented groups and low-income backgrounds.In this project, Professor Keying Ding is designing, synthesizing and characterizing new types of ligands and their respective defined iron complexes featuring "metal-ligand cooperativities." Professor Ding is studying their catalytic reactivity toward alcohol-amine couplings under mild conditions. In the currently studied system, the ligands not only serve as metal binding sites, but also directly participate in chemical bond activations. The project is exploring the optimal reaction conditions and the substrate scope for alcohols and amines. Important reaction intermediates and catalytic mechanisms are being investigated by combined experimental and theoretical studies, which will enrich fundamental understanding of non-precious metal catalysis for such transformations and will provide new insights into the design of highly selective catalysts.