Development of new-to-nature reactions under the concept of synergistic catalysis through the design of novel cobalt-based artificial metalloenzymes.

Obiettivo

Artificial metalloenzymes (ARMs), that is, designed enzymes containing a synthetic metal co-factor within a protein framework, locates itself as a promising area of research for the discovery and development of new transformations. We set our attention in cobalt complexes as co-factors, a first-row, earth-abundant, and non-toxic metal that is currently underexplored in ARMs. Cobalt complexes present a highly versatile chemistry, including they ability to participate in allylic functionalization reactions, an important transformation for the pharmaceutical industry as can deliver structural frameworks that are widely spread in biological active compounds. Allylic functionalization reactions are underdeveloped in bio-catalysis, and the expansion of important homogeneous reactions, as the before mentioned, into the realm of enzymes is an absolute necessity for the development of sustainable chemistry. Co-ARMs (Cobalt-containing ARtificial Metalloenzymes) proposal aims to create new generations of ARMs relying on the unique reactivity of synthetic cobalt complexes in allylic substitution reactions, an unknown reaction in enzyme catalysis and an underexplored metal for the discovery of new-to-nature reactions. The proposal balance between host expertise (Dr. Gerard Roelfes) in bio-inorganic and chemical biology, and the researchers skills (Dr. Franco Della-Felice) in synthetic organic chemistry. The result is a cooperative field where two different branches converge with the aim to develop new concepts and environmentally compatible tools in chemistry to access organic frameworks of high significance to the pharmaceutical and agrochemical industries.