Development and application of an artificial allylic aminase for in vivo catalysis purposes.

Natural enzymes have evolved to catalyze numerous reactions displaying unmatched selectivity and activity. Furthermore, nature has evolved many enzymes to work in a cascade, affording complex molecules from the simple starting material. However, the evolutionary process endowing these enzymes with such abilities took millions of years. This timescale does not match the demand for efficient catalytic systems to resolve societal problems in ecology, medicine, and pharmacology. Artificial metalloenzymes (ArMs) are an exciting solution since they combine the chemical versatility brought by a synthetic catalyst within a natural protein optimizable via a quick mutagenesis campaign. These two pivot points give artificial metalloenzyme great flexibility in terms of optimization since chemical fine-tuning and bio-engineering can be done to reach the maximal potential of ArMs. This inspired the research presented in this thesis which aims to present the development of a new class of ArMs.