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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Abstract 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.
AbstractList 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.
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.
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 which are incompatible with the 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 of 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. Here, it is demonstrated that diamidophosphate phosphorylates nucleosides, amino acids and glycerol/fatty acids in aqueous medium, while simultaneously leading to higher-order structures (oligonucleotides, peptides and liposomes) in the same pot.
Author Gibard, Clémentine
Krishnamurthy, Ramanarayanan
Kim, Eun-Kyong
Bhowmik, Subhendu
Karki, Megha
AuthorAffiliation Department of Chemistry, The Scripps Research Institute, 10550 North Torrey Pines Road, La Jolla, California 92037, USA
AuthorAffiliation_xml – name: Department of Chemistry, The Scripps Research Institute, 10550 North Torrey Pines Road, La Jolla, California 92037, USA
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  surname: Gibard
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  surname: Bhowmik
  fullname: Bhowmik, Subhendu
  organization: Department of Chemistry, The Scripps Research Institute, 10550 North Torrey Pines Road
– sequence: 3
  givenname: Megha
  surname: Karki
  fullname: Karki, Megha
  organization: Department of Chemistry, The Scripps Research Institute, 10550 North Torrey Pines Road
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  givenname: Eun-Kyong
  surname: Kim
  fullname: Kim, Eun-Kyong
  organization: Department of Chemistry, The Scripps Research Institute, 10550 North Torrey Pines Road
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  givenname: Ramanarayanan
  orcidid: 0000-0001-5238-610X
  surname: Krishnamurthy
  fullname: Krishnamurthy, Ramanarayanan
  email: rkrishna@scripps.edu
  organization: Department of Chemistry, The Scripps Research Institute, 10550 North Torrey Pines Road
BackLink https://www.ncbi.nlm.nih.gov/pubmed/29359747$$D View this record in MEDLINE/PubMed
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Issue 2
Keywords PHOSPHATE
PHOSPHORUS
NUCLEOTIDES
EARLY EARTH
ALPHA-PHOSPHORYLATION
MONOCARBOXYLIC ACIDS
RIBONUCLEOSIDES
INTERSTELLAR PN
AQUEOUS-SOLUTION
LIFE
Language English
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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.
ORCID 0000-0001-5238-610X
0000-0002-0313-6654
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  day: 01
PublicationDecade 2010
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PublicationTitle Nature chemistry
PublicationTitleAbbrev Nature Chem
NAT CHEM
PublicationTitleAlternate Nat Chem
PublicationYear 2018
Publisher Nature Publishing Group UK
Springer Nature
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SSID ssj0065316
Score 2.6373527
Snippet Prebiotic phosphorylation of (pre)biological substrates under aqueous conditions is a critical step in the origins of life. Previous investigations have had...
Prebiotic phosphorylation of (pre) biological substrates under aqueous conditions is a critical step in the origins of life. Previous investigations have had...
Source Web of Science
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pubmed
webofscience
springer
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StartPage 212
SubjectTerms 639/638/403
639/638/904
639/638/92
Amino acids
Analytical Chemistry
Biochemistry
Chemistry
Chemistry, Multidisciplinary
Chemistry/Food Science
Inorganic Chemistry
Liposomes
Oligomerization
Oligomers
Oligonucleotides
Organic Chemistry
Peptides
Phosphorylation
Physical Chemistry
Physical Sciences
Prebiotics
Science & Technology
Self-assembly
Substrates
Title Phosphorylation, oligomerization and self-assembly in water under potential prebiotic conditions
URI https://link.springer.com/article/10.1038/nchem.2878
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https://www.ncbi.nlm.nih.gov/pubmed/29359747
https://www.proquest.com/docview/2022111416
https://search.proquest.com/docview/1990486765
https://pubmed.ncbi.nlm.nih.gov/PMC6295206
Volume 10
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