Artificial Metalloenzymes

In nature, a large scope of chemical transformations are performed by complex molecules, known as enzymes. Enzymes are catalysts that are able to produce building blocks of just one mirror image. The production of these building blocks possessing just one mirror image is important for the construction of medicine, for example. However, enzymes have a very limited scope of transformation they can achieve. On the other hand, homogenous catalysis, can perform a much wider scope of transformations. However, it does not always produce one mirror image of the building block. Artificial metalloenzymes utilizes the benefits of the catalysts mentioned previously. An artificial metalloenzymes consists of a metal complex and a biomolecule. Artificial metalloenzymes proved to be very successful, however the number of available biomolecules for the construction of artificial metalloenzymes is limited.
This thesis describes a new approach for the development and construction of artificial metalloenzymes.
An active site, in which the chemical transformation takes place, was constructed on the interface of a protein that consisted of two equal parts. The protein that was used was LmrR. Different approaches to anchor the metal complex covalent or non-covalent are described in this thesis. The resulting artificial metalloenzymes were able to catalyze a variety of chemical transformations with very good results, i.e. a high percentage of one of the two mirror images of the products were formed. A study of these artificial metalloenzyme gave more insight in how these transformations were performed.