While metalloenzymes have benefited from the process of evolution to generate precise arrays of proximal non-covalent interactions that enhance metal-centered catalysis, this process is underexplored in abiotic catalysts due to challenging syntheses of elaborate, multifunctional ligands, which impedes iterative design. To overcome this synthetic bottleneck, we developed a highly modular and rapid synthetic strategy that leverages the efficiency of solid-phase peptide synthesis and conformational control afforded by non-canonical residues to construct ligand platforms displaying multiple residues of varying electronics and sterics in the secondary coordination sphere. We apply this scaffold to evolve improved activity in abiotic Fe catalysts. Solution-state NMR structures of several catalyst variants provides structure-functional insights and guides the design of future generations.

Rapid and multivariate evolution of abiotic peptide-conjugated metallocatalysts

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ACS Fall 2022

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