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Combining Bimetallic Scaffolds and Metal-Coordinated Phenoxyl Radicals for Multi Electron Transformations: A Step Beyond Nature

结合双金属支架和金属配位苯氧基自由基进行多电子转化：超越自然的一步

基本信息

批准号：
165831467
负责人：
Professor Dr. Franc Meyer
金额：
--
依托单位：
Department of Chemistry
依托单位国家：
德国
项目类别：
Research Grants
财政年份：
2010
资助国家：
德国
起止时间：
2009-12-31 至 2013-12-31
项目状态：
已结题

来源：
https://gepris.dfg.de/gepris/projekt/165831467?language=en
关键词：
Combining Bimetallic Scaffolds Metal Coordinated

项目摘要

The main objective of this joint project is to combine two of nature s strategies for mediating multi-electron redox transformations: using the redox reservoir of (i) bimetallic sites and (it) metal-coordinated phenoxyl radicals. To this end new binucleating ligand scaffolds that bear two metal-binding phenolate groups will be synthesized, and redox properties of their bimetallic complexes (mainly dinickel, dicopper and dizinc complexes) will be studied in detail. The project will focus on elucidating the electronic structures of the binuclear species in various oxidation levels and on modulating the sequence of metal- and ligand-based redox processes by fine-tuning of the ligand scaffolds. Our primary goal is to prepare highly preorganized binuclear metal complexes with variable endogenous and exogeneous bridging groups and variable terminal coordination to supply a total of four electrons (two from the metal centers and two from each terminal phenolate units) and to study their potential towards oxidation/oxygenation reactions of relevance to biology and of importance to industrial processes, ultimately, our goal is to apply newly discovered chemical knowledge to achieve a better understanding of the properties of a selected class of metalloenzymes (a typical example is galactose oxidase) and to pave new ways to bioinspired catalysts by combining two of nature s functional principles in a single artificial molecular system.

这个联合项目的主要目标是联合收割机两个自然界的策略调解多电子氧化还原转换：使用（i）氧化还原水库和（it）金属配位的苯氧基自由基。为此，新的双核配体支架，承载两个金属结合的酚基团将被合成，并将详细研究它们的双金属络合物（主要是二镍，二铜和二锌配合物）的氧化还原性能。该项目将侧重于阐明不同氧化水平下双核物种的电子结构，并通过微调配体支架来调节基于金属和配体的氧化还原过程的顺序。我们的主要目标是制备高度预组装的双核金属配合物，其具有可变的内源性和外源性桥联基团以及可变的末端配位，以提供总共四个电子（两个来自金属中心，两个来自每个末端酚盐单元），并研究它们对与生物学相关且对工业过程重要的氧化/氧化反应的潜力，最终，我们的目标是应用新发现的化学知识，更好地理解一类金属酶（典型的例子是半乳糖氧化酶）的性质，并通过将两种自然功能原理结合在一个人工分子系统中，为生物启发催化剂铺平新的道路。