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

RUI：用于醇胺偶联反应生成亚胺的新型铁催化剂

• 批准号: 1465051
• 负责人: Keying Ding
• 金额: $ 14.32万
• 依托单位: Middle Tennessee State University
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2015
• 资助国家: 美国
• 起止时间: 2015-08-01 至 2021-07-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1465051&HistoricalAwards=false
• 关键词: RUI; Novel; Fe; Catalysts; Alcohol

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.

有了这个奖项，化学系的化学催化计划正在资助来自中田纳西州立大学的Keying Ding教授开发一种用于有用偶联反应的新型地球丰富催化剂。目标化学结构，亚胺，代表了一类非常重要的化合物，在化学，制药和生物领域的应用。目前，这种偶联反应使用贵金属催化剂，其昂贵，有时有毒，并且供应有限。 因此，当今最常见的方法带来了经济挑战，而且往往是环境挑战。开发利用地球上丰富的金属系统进行此类反应的催化工艺符合可持续化学目标。 这方面的成功也可能引起制药工艺组和工业化学家的注意。该研究的更广泛影响包括为本科生、硕士研究生和高中生提供培训机会和实践研究经验，包括来自代表性不足的群体和低收入背景的学生。在该项目中，丁科颖教授设计、合成和表征了新型配体及其各自定义的具有“金属-配体协同作用”的铁配合物。“丁教授正在研究它们在温和条件下对醇胺偶联反应的催化活性。在目前研究的体系中，配体不仅作为金属结合位点，而且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。重要的反应中间体和催化机理正在通过实验和理论相结合的研究，这将丰富对此类转化的非贵金属催化的基本理解，并将为高选择性催化剂的设计提供新的见解。

项目成果

Switching between borrowing hydrogen and acceptorless dehydrogenative coupling by base transition-metal catalysts

• DOI: 10.1016/j.tet.2021.132451
• 发表时间: 2021-09
• 期刊: Tetrahedron
• 影响因子: 2.1
• 作者: Keying Ding

Switchable Cobalt-Catalyzed α-Olefination and α-Alkylation of Nitriles with Primary Alcohols

钴催化的伯醇对腈的α-烯烃化和α-烷基化

• DOI: 10.1021/acs.orglett.1c01553
• 发表时间: 2021
• 期刊: Organic Letters
• 影响因子: 5.2
• 作者: Paudel, Keshav;Xu, Shi;Ding, Keying
• 通讯作者: Ding, Keying

Switchable Imine and Amine Synthesis Catalyzed by a Well-Defined Cobalt Complex

• DOI: 10.1021/acs.organomet.0c00727
• 发表时间: 2021-01
• 期刊: Organometallics
• 影响因子: 2.8
• 作者: K. Paudel;Shi Xu;O. Hietsoi;Bedraj Pandey;Chuka Onuh;Keying Ding