Phosphorylation, oligomerization and self-assembly in water under potential prebiotic conditions

Prebiotic phosphorylation of (pre)biological substrates under aqueous conditions is a critical step in the origins of life. Previous investigations have had limited success and/or require unique environments that are incompatible with subsequent generation of the corresponding oligomers or higher-or...

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Published inNature chemistry Vol. 10; no. 2; pp. 212 - 217
Main Authors Gibard, Clémentine, Bhowmik, Subhendu, Karki, Megha, Kim, Eun-Kyong, Krishnamurthy, Ramanarayanan
Format Journal Article
LanguageEnglish
Published London Nature Publishing Group UK 01.02.2018
Springer Nature
Nature Publishing Group
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Summary:Prebiotic phosphorylation of (pre)biological substrates under aqueous conditions is a critical step in the origins of life. Previous investigations have had limited success and/or require unique environments that are incompatible with subsequent generation of the corresponding oligomers or higher-order structures. Here, we demonstrate that diamidophosphate (DAP)—a plausible prebiotic agent produced from trimetaphosphate—efficiently (amido)phosphorylates a wide variety of (pre)biological building blocks (nucleosides/tides, amino acids and lipid precursors) under aqueous (solution/paste) conditions, without the need for a condensing agent. Significantly, higher-order structures (oligonucleotides, peptides and liposomes) are formed under the same phosphorylation reaction conditions. This plausible prebiotic phosphorylation process under similar reaction conditions could enable the systems chemistry of the three classes of (pre)biologically relevant molecules and their oligomers, in a single-pot aqueous environment. Phosphorylation of (pre)biological molecules in water has been a long-sought goal in prebiotic chemistry. Now, it has been demonstrated that diamidophosphate phosphorylates nucleosides, amino acids and glycerol/fatty acids in aqueous medium, while simultaneously leading to higher-order structures such as oligonucleotides, peptides and liposomes in the same reaction mixture.
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Author Contributions
R.K. conceived the project. R.K., C.G., S.B., M.K. and E-K.K. designed the experiments. C.G., S.B. performed the nucleoside/nucleotide/oligonucleotide phosphorylation experiments. M.K., S.B. and C.G. performed the amino acid phosphorylation experiments. M.K. performed the liposome studies. E-K.K. and S.B. made the initial observations of DAP-mediated phosphorylation. R.K. wrote the paper with inputs from C.G., S.B., M.K and E-K. K. All authors discussed the results and commented on the manuscript.
ISSN:1755-4330
1755-4349
DOI:10.1038/nchem.2878