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Deep phylogenetic work provides fundamental insights into what biological processes were likely to have been present in early life. Certainly the universality of metabolic oxidation-reduction reactions suggests that these processes would be a hallmark of early life and thus represent a barrier on the path to the origin of life. Although fruitful in terms of insights into understanding aspects of the energy metabolism of early life, the features of extant biology tell us very little about the initial steps in the emergence of the protein based catalytic functionalities that facilitated these processes. Our main goal is to initiate a new collaboration to join forces across two NAI teams. We will combine the in vitro enzyme evolution technology pioneered by Seelig and coworkers of the NASA Ames team with the long standing expertise in biological oxidation reduction reactions of Peters’ group of the Montana State University Astrobiology Biogeocatalysis Research Center to evolve metal-based redox catalysts from random peptide libraries. The studies will provide fundamental insights into the first steps of the nesting and tuning of metal ions and metal clusters to achieve oxidation-reduction potentials that support reactions relevant to early life. We will use a simple nucleotide dependent oxidation of an alcohol as a selectable reaction and search for novel enzymes from random peptide libraries in the presence of different metal ions and counter ions. In addition, we will explore possible synergies between redox active mineral surfaces and polypeptide catalysis with the focus on early life scenarios.