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，以及从天然气、天然气和煤炭中高效和可持续地使用不可再生的碳氢资源，对于实现全球气候目标至关重要，这也是最近一次由政治引发的公开讨论中的要求。在这方面，通过催化氧化和氧化反应对有机分子进行选择性官能化是从石油和天然气资源中制备碱性和精细化学品以及合成复杂活性成分(如医药产品)的关键技术。这明确了迫切需要建立新的可持续概念，以便在温和的条件下利用环境友好和丰富的氧化剂，如O2和H2O2来合成附加值产品。自然界经常使用活性部位含有铁离子的酶来选择性氧化有机底物。这类酶能够在氧气活化过程中实现各种具有挑战性的反应。这些酶的催化循环已经建立在跨学科的努力中，结合了包括生物无机化学在内的不同领域的专业知识和方法。它们通过提供大量的结构和光谱模型，为阐明酶中活性中心和中间体的分子结构和电子结构做出了巨大贡献。将这些从酶系统研究中获得的知识转移到新的均相催化剂(功能模型)的开发中，目前在世界范围内引起了极大的兴趣，也是本研究小组的重点。开发生物灵感均相催化剂用于碳氢化合物和更复杂的有机底物的氧化和氧化，具有更好的催化性能，具有很高的学术和工业应用潜力。因此，本研究单位的最终目标是提供改进的生物灵感均相催化剂，用于环境友好的氧化剂，如O2和H2O2的氧化反应，导致氧原子转移、氢原子提取和C-H键活化。这将通过收集申请者在生物无机模型化学、活性中间体的捕获和光谱分析、动力学分析、催化和理论建模方面的广泛专业知识来实现，以获得对现有的六个生物启发氧化催化体系的活性中间体和机理的详细了解。这种对生物启发的模型体系的机理洞察以及与相应金属酶的比较应该能够在第一步中识别模型体系的反应性的局限性，这将最终使ii)合理地改进其催化性能。