Computational Studies of Artificial Metalloenzymes: From Methods and Models to Design and Optimization

This chapter is aimed to present how molecular modeling is involved in the design and optimization of artificial metalloenzymes (ArMs) devised to catalyze organic reactions. Taking as starting point the wide knowledge available nowadays in the use of theoretical calculations to compute reaction mechanism of transition metal-catalyzed reactions, the differences between transition metal catalysts and ArM are discussed, highlighting from a computational perspective the complexity that entails its study. The requirement to explore a highly multidimensional chemogenetic space compels to use a vast ensemble of methods that are briefly introduced. Then, selected examples illustrate how the computational tools have been used for constructing ArMs with improved or novel activities and specificities