Journal of the American Chemical Society · 2018 · 121 citations · 31 references
Life SciencesBiochemistryBiotechnologyBiocatalysisEnzymologyMicrobial MetabolismMetabolic ActivationOrigins Of LifePrebiotic ChemistryActivationNucleoside ModificationOligomerizationPhosphorylation ChemistryPrebiotic Phosphate ChemistryPrebiotic PhotochemistryPrebiotic SelectivityPrebiotic Synthesis Of Nucleotides
Investigations into the chemical origin of life have recently benefitted from a holistic approach in which possible atmospheric, organic, and inorganic systems chemistries are taken into consideration. In this way, we now report that a selective phosphate activating agent, namely methyl isocyanide, could plausibly have been produced from simple prebiotic feedstocks. We show that methyl isocyanide drives the conversion of nucleoside monophosphates to phosphorimidazolides under potentially prebiotic conditions and in excellent yields for the first time. Importantly, this chemistry allows for repeated reactivation cycles, a property long sought in nonenzymatic oligomerization studies. Further, as the isocyanide is released upon irradiation, the possibility of spatially and temporally controlled activation chemistry is thus raised.
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Synthesis of long prebiotic oligomers on mineral surfaces
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The eightfold path to non-enzymatic RNA replication
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