Details

Autor(en) / Beteiligte

• Lin, Huacan
• Jiménez, Eddy I.
• Arriola, Joshua T.
• Müller, Ulrich F.
• Krishnamurthy, Ramanarayanan

Titel

Concurrent Prebiotic Formation of Nucleoside‐Amidophosphates and Nucleoside‐Triphosphates Potentiates Transition from Abiotic to Biotic Polymerization

Ist Teil von

• Angewandte Chemie International Edition, 2022-01, Vol.61 (1), p.e202113625-n/a

Auflage

International ed. in English

Ort / Verlag

Germany: Wiley Subscription Services, Inc

Erscheinungsjahr

2022

Quelle

MEDLINE

Beschreibungen/Notizen

• Polymerization of nucleic acids in biology utilizes 5′‐nucleoside triphosphates (NTPs) as substrates. The prebiotic availability of NTPs has been unresolved and other derivatives of nucleoside‐monophosphates (NMPs) have been studied. However, this latter approach necessitates a change in chemistries when transitioning to biology. Herein we show that diamidophosphate (DAP), in a one‐pot amidophosphorylation‐hydrolysis setting converts NMPs into the corresponding NTPs via 5′‐nucleoside amidophosphates (NaPs). The resulting crude mixture of NTPs are accepted by proteinaceous‐ and ribozyme‐polymerases as substrates for nucleic acid polymerization. This phosphorylation also operates at the level of oligonucleotides enabling ribozyme‐mediated ligation. This one‐pot protocol for simultaneous generation of NaPs and NTPs suggests that the transition from prebiotic‐phosphorylation and oligomerization to an enzymatic processive‐polymerization can be more continuous than previously anticipated. The DAP mediated prebiotic phosphorylation of nucleosides/nucleotides/oligonucleotides produces a spectrum of the corresponding mono‐, di‐, and tri(amido)phosphorylated derivatives which are substrates for both prebiotic‐oligomerization and biotic‐polymerization/ligation. The compatibility of the phosphorylation and activation chemistry across a broad spectrum of (oligo)nucleos(t)ide structures suggests a smoother transition from chemistry to biology.