Mimicking Copper Sites of pMMO via endo- and exo-Functionalized Cage-Compounds

资源枯竭、能源供应问题和气候变化是当今的主要挑战。催化被认为是解决这些和其他紧迫问题的关键方面。在所期望的转化中，许多已知是由酶、天然催化剂介导的。从气候、科学和经济的角度来看，甲烷转化为甲醇非常重要。迄今为止，合成催化剂还没有充分掌握这种转化。自然界发展了两个基于铁和铜的酶家族，即甲烷单加氧酶。特别是，人们对更强大的铜基甲烷单加氧酶如何工作知之甚少。更好地理解酶的一种方法是开发模拟感兴趣的酶的结构和功能的合成模型复合物。该项目的目的是模拟铜基甲烷单加氧酶的可能活性位点，目的是了解更多这类非常重要的金属酶。实现这一点的方法使用功能化的笼状化合物，其类似于酶内部的配位氨基酸残基。该项目的一个目标是阐明铜基甲烷单加氧酶中不同铜位点的作用。特别是，这些项目旨在更好地了解氧气和底物活化如何在这些酶活性位点模拟物中发生。更好地理解铜基甲烷单加氧酶可以导致更强大的催化剂用于甲烷转化为甲醇。

The depletion of resources, energy supply problems and climate change are major challenges today. Catalysis is believed to be a key aspect in solving these and other urgent problems. Among the desirable transformation, many are known to be mediated by enzymes, natures catalysts. The conversion of methane to methanol is very important from a climatic, scientific and economic point of view. This transformation has so far not sufficiently been mastered by synthetic catalysts. Nature developed two enzyme families that are based on iron and copper, the methane monooxygenases. In particular, little is known about how the more powerful copper-based methane monooxygenases work. One way for a better understanding of enzymes is the development of synthetic model complexes that mimic the structure and functionality of the enzyme of interest. The project aim is to mimic the presumably active sites of the copper-based methane monooxygenase with the goal to understand more of this very important class of metalloenzymes. The approach to achieve this uses functionalized cage compounds that resemble the coordinating amino acid residues of the enzyme in their inner. One goal of the project is to shine light on the role of different copper sites within the copper-based methane monooxygenase. In particular, the projects aim to obtain a better understanding how oxygen and substrate activation occurs within these enzymes active site mimics. A better understanding of the copper-based methane monooxygenases can lead to more powerful catalysts for the conversion of methane to methanol.