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

胺的功能被纳入广泛的天然产物，称为生物碱，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。从更容易获得的起始材料（包括烯烃和醇）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，催化方法正在成为提高能源效率和减少废物副产品形成的首选策略。催化剂为提高制造效率和商业盈利能力提供了最前沿的机会，因为它们帮助化学转化在更少的强迫条件下发生，并且它们控制化学反应的结果，而不消耗自己。因此，催化剂可以重复使用，只需要少量。***本提案的目标是制备新的催化剂，以廉价的胺、烯烃和醇为原料，高效合成增值选择性取代胺。几十年来，化学/制药/农用化学品制造部门一直以这种转变为目标，但众所周知，这种转变具有挑战性，因为胺试剂和产品可以与催化剂结合并使其失效。***我们的团队率先开发了生物启发的N， o螯合金属配合物，作为一种新的催化剂家族，能够通过催化C-N键形成或C-C键形成，从简单的胺，烯烃和醇构建块组装更复杂的胺。在这里，我们建议建立在我们以前的成功，以解决目前没有普遍有效的催化选择已知的具有挑战性的转变。此外，我们建议开发改进的催化剂来构建传统化学方法无法轻易组装的胺。我们的核心发现集中在实现和理解新的化学反应性和转化，这可以用来实现化学制造的创新和前沿方法。对加拿大的好处将包括发展世界领先的清洁技术，用于制备胺功能化小分子和与塑料、复合材料、农化和制药工业相关的材料。* * * * * * * *

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. ********