Multifunctional reactive intermediates: preparation, characterization, reactivity and catalysis

多功能反应中间体：制备、表征、反应性和催化

• 批准号: 209205738
• 负责人: Professor Dr. Ilan Marek
• 金额: --
• 依托单位: Institut für Organische Chemie
• 依托单位国家: 德国
• 项目类别: DIP Programme
• 财政年份: 2012
• 资助国家: 德国
• 起止时间: 2011-12-31 至 2018-12-31
• 项目状态: 已结题
• 来源: https://gepris.dfg.de/gepris/projekt/209205738?language=en
• 关键词: Multifunctional; reactive; intermediates; preparation; characterization

One of the prime elements for advancing chemical synthesis is the preparation, characterization, and control of multi-functional reactive intermediates. Currently, standard chemical technology typically employs mono- functional reactive species (organometallics, radicals, carbenes, cations, anions, etc.) and this seriously hampers the rapid construction of complex structures. Hence, most total syntheses involve a large number of steps and consequently are neither atom / mass nor energy economic. Despite the tremendous progress in this area, a much larger panel of reactions and especially reagents achieving a significant increase in structural complexity per chemical step is necessary. In this proposal five groups with diverse expertise have teamed together to prepare and study a variety of multi- functional reagents and reactive species that are possible intermediates in important synthetic transformations. Emphasis is on main group element reagents and reactive intermediates spanning from di- and tri- metallo hydrocarbons and silanes, to functionalized radicals and carbenes, to the analogous silicon-based intermediates, to oxenoids and nitrenoids and to transition metal functionalized reagents. The proposed research combines synthesis, mechanistic studies and the isolation of reactive intermediates in inert matrix and their spectroscopic characterization. It combines experiment and theoretical calculations which will provide additional insights into the nature of the many new reactive species which we plan to study. Overall, we believe that this research will enrich chemistry with many new multifunctional reagents and reactive species providing new possibilities for efficient synthesis of complex molecules.

推进化学合成的主要因素之一是多功能反应中间体的制备、表征和控制。目前，标准化学技术通常采用单官能反应性物质（有机金属化合物、自由基、卡宾、阳离子、阴离子等）。这严重阻碍了复杂结构的快速建造。因此，大多数全合成涉及大量的步骤，因此既不原子/质量也不节能。尽管在这一领域取得了巨大的进展，但需要更大的反应组，特别是每个化学步骤实现结构复杂性显著增加的试剂。在这项提案中，五个具有不同专业知识的小组合作制备和研究了各种多功能试剂和反应物种，这些试剂和反应物种可能是重要合成转化中的中间体。重点是主族元素试剂和反应中间体，从二-和三-金属烃和硅烷，到官能化的自由基和卡宾，到类似的硅基中间体，到氧杂环丁烷和类氮杂环戊烯，以及过渡金属官能化试剂。该研究结合了合成，机理研究和惰性基质中反应中间体的分离及其光谱表征。它结合了实验和理论计算，这将为我们计划研究的许多新的活性物种的性质提供更多的见解。总的来说，我们相信这项研究将丰富化学与许多新的多功能试剂和活性物种提供新的可能性，有效地合成复杂的分子。