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Prebiotic Phosphorylation of Uridine using Diamidophosphate in Aerosols

One of the most challenging fundamental problems in establishing prebiotically plausible routes for phosphorylation reactions using phosphate is that they are thermodynamically unfavorable in aqueous conditions. Diamidophosphate (DAP), a potentially prebiotically relevant compound, was shown to phos...

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Autores principales: Castañeda, A. D., Li, Z., Joo, T., Benham, K., Burcar, B. T., Krishnamurthy, R., Liotta, C. L., Ng, N. L., Orlando, T. M.
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Nature Publishing Group UK 2019
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC6753121/
https://www.ncbi.nlm.nih.gov/pubmed/31537885
http://dx.doi.org/10.1038/s41598-019-49947-8
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author Castañeda, A. D.
Li, Z.
Joo, T.
Benham, K.
Burcar, B. T.
Krishnamurthy, R.
Liotta, C. L.
Ng, N. L.
Orlando, T. M.
author_facet Castañeda, A. D.
Li, Z.
Joo, T.
Benham, K.
Burcar, B. T.
Krishnamurthy, R.
Liotta, C. L.
Ng, N. L.
Orlando, T. M.
author_sort Castañeda, A. D.
collection PubMed
description One of the most challenging fundamental problems in establishing prebiotically plausible routes for phosphorylation reactions using phosphate is that they are thermodynamically unfavorable in aqueous conditions. Diamidophosphate (DAP), a potentially prebiotically relevant compound, was shown to phosphorylate nucleosides in aqueous medium, albeit at a very slow rate (days/weeks). Here, we demonstrate that performing these reactions within an aerosol environment, a suitable model for the early Earth ocean-air interface, yields higher reaction rates when compared to bulk solution, thus overcoming these rate limitations. As a proof-of-concept, we demonstrate the effective conversion (~6.5–10%) of uridine to uridine-2′,3′-cyclophosphate in less than 1 h. These results suggest that aerosol environments are a possible scenario in which prebiotic phosphorylation could have occurred despite unfavorable rates in bulk solution.
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spelling pubmed-67531212019-10-01 Prebiotic Phosphorylation of Uridine using Diamidophosphate in Aerosols Castañeda, A. D. Li, Z. Joo, T. Benham, K. Burcar, B. T. Krishnamurthy, R. Liotta, C. L. Ng, N. L. Orlando, T. M. Sci Rep Article One of the most challenging fundamental problems in establishing prebiotically plausible routes for phosphorylation reactions using phosphate is that they are thermodynamically unfavorable in aqueous conditions. Diamidophosphate (DAP), a potentially prebiotically relevant compound, was shown to phosphorylate nucleosides in aqueous medium, albeit at a very slow rate (days/weeks). Here, we demonstrate that performing these reactions within an aerosol environment, a suitable model for the early Earth ocean-air interface, yields higher reaction rates when compared to bulk solution, thus overcoming these rate limitations. As a proof-of-concept, we demonstrate the effective conversion (~6.5–10%) of uridine to uridine-2′,3′-cyclophosphate in less than 1 h. These results suggest that aerosol environments are a possible scenario in which prebiotic phosphorylation could have occurred despite unfavorable rates in bulk solution. Nature Publishing Group UK 2019-09-19 /pmc/articles/PMC6753121/ /pubmed/31537885 http://dx.doi.org/10.1038/s41598-019-49947-8 Text en © The Author(s) 2019 Open Access This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/.
spellingShingle Article
Castañeda, A. D.
Li, Z.
Joo, T.
Benham, K.
Burcar, B. T.
Krishnamurthy, R.
Liotta, C. L.
Ng, N. L.
Orlando, T. M.
Prebiotic Phosphorylation of Uridine using Diamidophosphate in Aerosols
title Prebiotic Phosphorylation of Uridine using Diamidophosphate in Aerosols
title_full Prebiotic Phosphorylation of Uridine using Diamidophosphate in Aerosols
title_fullStr Prebiotic Phosphorylation of Uridine using Diamidophosphate in Aerosols
title_full_unstemmed Prebiotic Phosphorylation of Uridine using Diamidophosphate in Aerosols
title_short Prebiotic Phosphorylation of Uridine using Diamidophosphate in Aerosols
title_sort prebiotic phosphorylation of uridine using diamidophosphate in aerosols
topic Article
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC6753121/
https://www.ncbi.nlm.nih.gov/pubmed/31537885
http://dx.doi.org/10.1038/s41598-019-49947-8
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