RNA polymerisation without catalyst from 2’,3’-cyclic nucleotides by drying at air-water interfaces

Authors

  • Avinash Vicholous Dass Systems Biophysics, Faculty of Physics, Ludwig-Maximili- ans-Universität München, Amalienstr. 54, 80799 München, Germany ,
  • Sreekar Wunnava Systems Biophysics, Faculty of Physics, Ludwig-Maximili- ans-Universität München, Amalienstr. 54, 80799 München, Germany ,
  • Juliette Langlais Systems Biophysics, Faculty of Physics, Ludwig-Maximili- ans-Universität München, Amalienstr. 54, 80799 München, Germany ,
  • Beatriz von der Esch Chair of Theoretical Chemistry, Department of Chemistry, Ludwig-Maximilians-Universität München Butentandtstraße 5-13, 81377, Munich, Germany ,
  • Maik Krusche Systems Biophysics, Faculty of Physics, Ludwig-Maximili- ans-Universität München, Amalienstr. 54, 80799 München, Germany ,
  • Lennard Ufer Systems Biophysics, Faculty of Physics, Ludwig-Maximili- ans-Universität München, Amalienstr. 54, 80799 München, Germany ,
  • Nico Chrisam Systems Biophysics, Faculty of Physics, Ludwig-Maximili- ans-Universität München, Amalienstr. 54, 80799 München, Germany ,
  • Romeo C. A. Dubini Faculty of Chemistry and Pharmacy, Ludwig-Maximilians- Universität München Butentandtstraße 5-13, 81377, Munich, Germany ,
  • Florian Gartner Faculty of Physics, Statistical and biological physics, Lud- wig-Maximilians-Universität München, Theresienstraße. 37, D-80333, Munich, Germany ,
  • Severin Angerpointner Faculty of Physics, Statistical and biological physics, Lud- wig-Maximilians-Universität München, Theresienstraße. 37, D-80333, Munich, Germany ,
  • Christina F. Dirscherl Systems Biophysics, Faculty of Physics, Ludwig-Maximili- ans-Universität München, Amalienstr. 54, 80799 München, Germany ,
  • Petra Rovó Institute of Science and Technology Austria c/o NMR Facility, Am Campus 1, A-3400 Klosterneuburg, Austria & Faculty of Chemistry and Pharmacy, Ludwig-Maximilians- Universität München Butentandtstraße 5-13, 81377, Munich, Germany ,
  • Christof B. Mast Systems Biophysics, Faculty of Physics, Ludwig-Maximili- ans-Universität München, Amalienstr. 54, 80799 München, Germany ,
  • Judit Šponer Institute of Biophysics Academy of Sciences of the Czech Republic Královopolská 135, 61265 Brno, Czech Republic ,
  • Christian Ochsenfeld Max Planck Institute for Solid State Research, Heisenbergstr. 1, D-70569 Stuttgart, Germany & Chair of Theoretical Chemistry, Department of Chemistry, Ludwig-Maximilians-Universität München Butentandtstraße 5-13, 81377, Munich, Germany ,
  • Erwin Frey Faculty of Physics, Statistical and biological physics, Lud- wig-Maximilians-Universität München, Theresienstraße. 37, D-80333, Munich, Germany ,
  • Dieter Braun Systems Biophysics, Faculty of Physics, Ludwig-Maximili- ans-Universität München, Amalienstr. 54, 80799 München, Germany

Abstract

For the emergence of life, the abiotic synthesis of RNA from its monomers is a central step. We found alkaline, uncatalysed drying conditions in bulk and at heated air-water interfaces where 2´,3´-cyclic nucleotides polymerised, forming up to 10-mers within a day. The polymerisation proceeded at a pH range of 7-12 at temperatures between 40-80 °C and was marginally enhanced by K+ ions. Among the canonical ribonucleotides, cGMP polymerised most efficiently. Quantification was performed using HPLC coupled to ESI-TOF by fitting the isotope distribution to the mass spectra. Our study suggests a polymerisation mechanism where cGMP aids the incorporation of the relatively unreactive nucleotides C, A and U. The 2´,3´-cyclic nucleotides are byproducts of prebiotic phosphorylation, nucleotide syntheses and RNA hydrolysis, indicating direct recycling pathways. The simple reaction condition offers a plausible entry point for RNA to the evolution of life on early Earth.

Version notes

The title was revised to be more specific about the importance of the results. Figures were improved to reflect more details of the results. The introduction, results and the discussion sections were further elaborated. Some recent and relevant references are added. New figures are added to the SI.

Content

Supplementary material

RNA polymerisation without catalyst from 2’,3’-cyclic nucleotides by drying at air water interfaces
Associated material of the main manuscript