Artificial and Repurposed Metalloenzymes for in vivo New-to-Nature Catalysis - Challenges and Opportunities

Artificial metalloenzymes (ArMs) have attracted increasing attention in the past two decades as attractive alternatives to either homogeneous catalysts or enzymes. ArMs result from anchoring a catalytically-competent abiotic metal cofactor within a host protein, see Figure. The resulting ArMs combine attractive features of both homogeneous- and bio-catalysts.[1-3] Within the group, we have chemo-genetically optimized the performance of ArMs for twenty different reactions. Following a general introduction on the underlying principles of ArMs, this talk will highlight our recent progress towards engineering and evolving hybrid catalysts with an emphasis on new-to-nature transformations for whole-cell biocatalysis, including metal-catalyzed hydrogen atom transfer chemistry.