Development of N,O Chelated Complexes for the Catalytic Synthesis of Amines and Nitrogen Containing Materials

胺的功能被纳入一系列称为生物碱的天然产品中，是大多数合成和天然存在的生物活性化学品和材料的关键成分，如药品、农用化学品和抗微生物塑料。从包括烯烃和醇在内的更容易获得的原料中选择性和战略性地合成这种胺功能化小分子和材料的方法是一个深入研究的领域，催化方法已成为提高能源效率和减少废物形成的首选策略。催化剂为提高制造效率和商业盈利能力提供了前沿机会，因为它们有助于在较少的强制条件下发生化学转化，并且它们控制化学反应的结果，而不会本身被消耗。因此，催化剂可以重复使用，只需要少量的催化剂。*这项建议旨在制备新的催化剂，用于从廉价的胺、烯烃和醇的起始原料中高效地合成附加值高的选择性取代胺。几十年来，这种转变一直是化学/医药/农用化学品制造部门的目标，但众所周知是具有挑战性的，因为胺类试剂和产品可能与催化剂结合，使其无效。*我们的团队率先开发了受生物启发的N，O-螯合金属络合物作为一种新的催化剂家族，能够通过催化C-N键或C-C键的形成，从简单的胺、烯烃和醇的构建块组装更复杂的胺。在此，我们建议在以往成功的基础上，解决目前尚无普遍有效的催化选择的已知的具有挑战性的转型。此外，我们建议开发改进的催化剂，以构建使用传统化学方法无法容易组装的胺。我们的核心发现专注于实现和了解新的化学反应和转化，可用于实现化学制造中的创新和尖端方法。对加拿大的好处将包括开发世界领先的清洁技术，用于制备与塑料、复合材料、农用化学品和制药工业有关的胺功能化小分子和材料。********

Amine functionalities are incorporated into a broad range of natural products called alkaloids and are key components of a majority of synthetic and naturally occurring biologically active chemicals and materials, such as pharmaceuticals, agrochemicals and anti-microbial plastics. Methods for selectively and strategically synthesizing such amine functionalized small molecules and materials from more readily available starting materials, including alkenes and alcohols, is an area of intense investigation with catalytic approaches emerging as the preferred strategy for improving energy efficiency and reducing waste by-product formation. Catalysts offer cutting-edge opportunities for advancing manufacturing efficiency and commercial profitability as they help chemical transformations occur with less forcing conditions and they control the outcome of the chemical reaction while not being consumed themselves. Thus, catalysts can be reused repeatedly and are only required in small amounts. ***This proposal targets the preparation of new catalysts for the efficient synthesis of value-added selectively substituted amines from inexpensive amine, alkene and alcohol starting materials. Such transformations have been targeted by the chemical/pharmaceutical/agrochemical manufacturing sector for decades, but are known to be challenging as the amine reagents and products can bind to catalysts and render them ineffective. *** Our group has pioneered the development of bio-inspired, N,O-chelated metal complexes as a new family of catalysts that are capable of assembling more complex amines from simple amine, alkene and alcohol building blocks by either catalytic C-N bond formation or C-C bond formation. Here we propose to build upon our previous successes to tackle known challenging transformations that at present have no generally effective catalytic option. Additionally, we propose to develop improved catalysts to build amines that cannot be readily assembled using traditional chemical approaches. Our core discoveries focus on realizing and understanding new chemical reactivity and transformations, which could be used to achieve innovative and cutting-edge approaches in chemical manufacturing. Benefits to Canada will include the development of world-leading clean technologies for the preparation of amine functionalized small molecules and materials of relevance to the plastics, composite materials, agrochemical and pharmaceutical industries. ********