Coordination Funds

协调基金

• 批准号: 495584855
• 负责人: Professor Dr. Thorsten Glaser
• 金额: --
• 依托单位: Arbeitsgruppe Anorganische Chemie I
• 依托单位国家: 德国
• 项目类别: Research Units
• 资助国家: 德国
• 项目状态: 未结题
• 来源: https://gepris.dfg.de/gepris/projekt/495584855?language=en
• 关键词: Coordination; Funds

The decarbonization of the production of energy and an efficient and sustainable usage of non-renewable hydrocarbon resources from natural oil, gas, and coal is essential to achieve the global climate goals and has also been demanded in a politically-induced recent public dis¬cussion. In this respect, the selective functionalization of organic molecules by catalytic oxidation and oxygenation reactions is a key technology for the preparation of basic and fine chemicals from natural oil and gas resources, as well as for the synthesis of complex active ingredients, e. g. for pharmaceutical products. This defines an urgent need to establish new sustainable concepts for utilizing environmentally benign and abundant oxidants, such as O2 and H2O2 under mild con¬ditions for the synthesis of value-added products. Nature frequently uses enzymes with iron ions in the active sites for the selective oxidation of organic substrates. Such enzymes are capable of realizing a variety of challenging reactions during the course of O2 activation. The catalytic cycles of these enzymes have been established in interdisciplinary efforts combining expertise and methodologies from different fields including bioinorganic chemistry. They have strongly contributed to the elucidation of the molecular and electronic structures of the active sites and intermediates in the enzymes by providing a plethora of structural and spectroscopic modelsTransferring this knowledge gained from studies of the enzymatic systems to the development of new homogeneous catalysts (functional models) is presently of great interest worldwide and is the focus of this Research Unit. The development of bioinspired homogenous catalysts for the oxidation and oxygenation of hydrocarbons and more complex organic substrates with better catalytic performances has a high potential for academic and industrial applications.Thus, it is the ultimate goal of this Research Unit to provide improved bioinspired homogenous catalysts for oxidation reactions using environmentally benign oxidants such as O2 and H2O2 that results in oxygen-atom transfer, hydrogen atom abstraction, and C-H bond activation. This will be achieved by gathering the wide expertise of the applicants in bioinorganic model chemistry, trapping and spectroscopic analysis of reactive intermediates, kinetic analysis, catalysis, and theoretical modeling to obtain a detailed insight into the reactive intermediates and mechanisms of six already existing systems for bioinspired oxidation catalysis. This mechanistic insight in the bioinspired model systems and the comparison to the corresponding metalloenzymes should allow in the first step i) to identify the limitations in the reactivities of the model systems, which will finally allow ii) to rationally improve their catalytic performances.

能源生产的脱碳以及天然石油，天然气和煤炭对非可再生烃资源的有效和可持续使用对于实现全球气候目标至关重要，并且在可行的近期公共散发中也要求。在这方面，通过催化氧化和氧合反应对有机分子的选择性功能化是制备天然石油和天然气资源以及复杂活性成分的碱性化学物质的关键技术，例如。用于药品。这定义了迫切需要建立新的可持续概念，以利用环境良性和丰富的氧化物，例如在温和的结合下，以合成增值产品。自然经常在活性位点使用铁离子的酶来选择有机底物的选择性氧化。在O2激活过程中，这种酶能够意识到各种挑战反应。这些酶的催化循环已经在跨学科的工作中建立，该综合专家和来自不同领域的方法在内，包括生物无机化学。它们通过提供了多种结构和光谱模型，从酶系统中获得的知识转移到新同质催化剂的发展（功能性模型）中，这些知识是伟大的，它们促进了杰出的研究（功能性模型），这是伟大的convosity contence the the the the the the the thewlrove，它们通过提供了多种结构和光谱模型来阐明酶中活性位点和中间体的分子和电子结构的强烈贡献。生物启动的同质催化剂开发用于氧化物和碳氢化合物的氧合和具有更好催化性能的更复杂的有机底物的发展具有很高的学术和工业应用潜力。转移，氢原子抽象和C-H键激活。这将通过收集申请人在生物无机模型化学，反应性中间体，动力学分析，催化和理论模型中的诱捕和光谱分析中的广泛专业知识来详细介绍，以获取对生物启动氧化蛋白酶的六个已经现有系统的反应性中间体和机制的详细信息。在生物启发的模型系统中的这种机械洞察力以及与相应的金属酶的比较应允许在第一步i）中识别模型系统反应性的局限性，最终将允许ii）理性地改善其催化性能。