Exploration of New Reactivities for Sustainable Chemical Syntheses

探索可持续化学合成的新反应

• 批准号: RGPIN-2020-05659
• 负责人: Li, ChaoJun
• 金额: $ 5.76万
• 依托单位: McGill University
• 依托单位国家: 加拿大
• 项目类别: Discovery Grants Program - Individual
• 财政年份: 2022
• 资助国家: 加拿大
• 起止时间: 2022-01-01 至 2023-12-31
• 项目状态: 已结题
• 来源: https://www.nserc-crsng.gc.ca/ase-oro/Details-Detailles_eng.asp?id=747972
• 关键词: Exploration; New; Reactivities; Sustainable; Chemical

Background and Objectives: Chemical synthesis plays a vital role in producing pharmaceuticals, agrochemicals, plastics, coatings, textiles, and electronic materials by converting natural resources. However, state-of-the-art chemical synthesis often requires extensive auxiliary steps that lead to overall low resource efficiency and raise environmental/health concerns related to chemical waste. How to utilize limited natural resources efficiently constitutes a key aspect of future sustainability. The overall objective of this project is to discover new chemical reactivities for more sustainable future chemical syntheses and to establish a leading program of excellence in research output, impact, and training in Green/Sustainable Synthetic Chemistry. Research Plan: To explore new chemical reactivities that can work under ambient conditions, maximize atom-utilization, and directly transform natural resources such as renewable biomass from their native states into useful chemical products. Building on our previous successes and capitalizing our recent exciting breakthroughs, this Discovery Grant will direct our research in the following four major avenues: (1) To develop novel organometallic reactions without using stoichiometric metals and organic halides; (2) To explore new reaction pathways for aromatic compounds with photo energy; (3) To develop lignins as renewable aromatic building blocks; (4) Low-temperature activation and transformations of small abundant molecules (N2, CO2, and methane) into high valued products. Significance: The combined success of using hydrazones as organometallic reagent surrogates, transition-metal-free aromatic substitutions and cross couplings, direct conversion of phenols and lignins into aromatic amines, and efficient-conversion of small inert abundant (N2, CO2 and CH4) into high valued products will fundamentally change approaches to organic reactions as they are presented in chemistry textbooks and to the way chemists perform organic synthesis. These reactions will drastically increase the efficiency of chemical syntheses and minimize chemical waste by avoiding the presynthesis of organometallic reagents and functionalization-defunctionalization processes of common organics, as well as the manufacturing of aromatic products. Together, these will create new frontiers in sustainability challenges regarding metals, transition-metals, renewable aromatics and abundant inert molecules utilizations. Training of HQP: 7 out of 24 HQP in the PI's laboratory (1 postdoc, 5 PhDs, and 1 undergraduate student) will be directly involved at any given year in this proposal, who will be trained with comprehensive research skills in organic synthesis, gas-phase reactions, catalysis, photochemistry and nanotechnology, and instrumentation expertise in NMR, GCMS, TEM, SEM, TGA etc and approximately 80-90 HQPs (for the next 5 years) in the PI's laboratory will be benefited in related training from this Discovery Project.

背景和目标：化学合成在生产药物，农业化学，塑料，涂料，纺织品和电子材料中起着至关重要的作用，通过转换自然资源。但是，最先进的化学合成通常需要广泛的辅助步骤，从而导致总体资源效率低，并提高与化学废物有关的环境/健康问题。如何利用有限的自然资源有效构成了未来可持续性的关键方面。该项目的总体目的是发现新的化学反应性，以实现更可持续的未来化学合成，并在绿色/可持续合成化学方面建立领先的研究成果，影响和培训方面的领先计划。研究计划：探索可以在环境条件下起作用的新化学反应性，最大化原子利用，并直接将自然资源（例如可再生生物量）从其本地状态转化为有用的化学产品。这项Discovery Grant以我们以前的成功并利用了我们最近令人兴奋的突破，将在以下四个主要途径中指导我们的研究：（1）在不使用化学计量金属和有机卤化物的情况下发展新颖的有机金属反应； （2）探索带有光能的芳族化合物的新反应途径； （3）将木质素作为可再生芳香构建块； （4）小型丰富分子（N2，CO2和甲烷）向高价值产物的低温激活和转化。 Significance: The combined success of using hydrazones as organometallic reagent surrogates, transition-metal-free aromatic substitutions and cross couplings, direct conversion of phenols and lignins into aromatic amines, and efficient-conversion of small inert abundant (N2, CO2 and CH4) into high valued products will fundamentally change approaches to organic reactions as they are presented in chemistry textbooks and to the way chemists perform有机合成。这些反应将大大提高化学合成的效率，并通过避免有机金属试剂的前提和共同有机物的功能化清除过程以及芳香产物的生产来最大程度地减少化学废物。这些将在金属，过渡金属，可再生芳烃和丰富的惰性分子利用方面构成可持续性挑战的新领域。在PI实验室的24个HQP中，HQP的培训将在该提案中的任何一年中直接参与PI的24个HQP（1个博士后博士学位和1名本科生），他们将接受有机综合，气相反应，催化剂，光化学，光学化学和纳米技术等的全面研究技能培训。 PI实验室中的80-90 HQP（未来5年）将受益于该发现项目的相关培训。