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Emergence of a Promiscuous Peroxidase Under Non-Equilibrium Conditions

preprint
submitted on 12.01.2021, 04:33 and posted on 13.01.2021, 05:53 by Sumit Pal, Antara Reja, Subhajit Bal, Baishakhi Tikader, Sandip Kar, Dibyendu Das

In the far from equilibrium state of living matter, energy is consumed to fuel the metabolic networks of enzymatic reactions. The emergence of protometabolic pathways in primeval earth is intricately related to the evolutionary journey of modern enzymes. Fundamental understanding of such energy driven generation of early catalytic systems would help us recognize the conditions required for the minimal metabolism that predated the chemical emergence of life. Herein, we report substrate driven generation of a non-equilibrium catalytic machinery from a single amino acid functionalized fatty acid in presence of a cofactor hemin. The non-equilibrium assembled state showed acceleration of catalytic potential resulting in degradation of the substrate and subsequently led to disassembly. Controls that promoted equilibration could not access the three-dimensional microphases and showed substantially lower catalytic activity. Significantly, the assembled state showed latent catalytic function by hydrolysing a precursor to yield the same substrate. Consequently, the assembly was benefitted with augmented lifetime of the catalytic state exploiting a promiscuous cascade and thus foreshadowing protometabolism. The results contribute towards our understanding of energy driven generation of primitive catalytic machineries that assisted the minimal metabolism of early life.

Funding

SERB India

History

Email Address of Submitting Author

dasd@iiserkol.ac.in

Institution

Indian Institute of Science Education and Research (IISER) Kolkata

Country

India

ORCID For Submitting Author

ORCID Dibyendu Das:0000-0001-6597-8454

Declaration of Conflict of Interest

Authors declare no conflict of interest

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