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

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

doi:10.1002/ange.202113625

Cited by 4 publications

(5 citation statements)

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“…The observations reported above, along with previous works, ,, create a scenario where DAP-mediated phosphorylation could potentially enable a continuous transition starting from nucleosides to oligonucleotides, helped by various small molecules, some of which also have the potential to give rise to efficient catalysts. Implicit in this scenario is the intriguing possibility of side-by-side formation and coevolution of peptides and oligonucleotides by DAP-mediated phosphorylation chemistry.…”

Section: Discussionmentioning

confidence: 56%

“…9,10 Thus, DAP-mediated phosphorylation with 2aminoimidazole could provide a model scenario for starting from the (a) phosphorylation of nucleosides to form mononucleotides, (b) activation of mononucleotides for use by ribozymes for ligation, and (c) conversion of mononucleotides to nucleoside-triphosphates (NTPs), which are the substrates used in extant biology. 54,55 The observations reported above, along with previous works, 5,55,56 create a scenario where DAP-mediated phosphorylation could potentially enable a continuous transition starting from nucleosides to oligonucleotides, helped by various small molecules, some of which also have the potential to give rise to efficient catalysts. Implicit in this scenario is the intriguing possibility of side-by-side formation and coevolution of peptides and oligonucleotides by DAP-mediated phosphorylation chemistry.…”

Section: Journal Of the Americanmentioning

confidence: 79%

“…Out of the imidazole family, 2-aminoimidazole is unique since it not only enables the phosphorylation of ribonucleosides but also is the sole additive among all of the ones investigated here that gives a high conversion of both ribo- and deoxyribonucleosides to their corresponding nucleotides. The advantage of 2-aminoimidazole has been demonstrated in terms of oligomer formation and nonenzymatic polymerization as well. , Thus, DAP-mediated phosphorylation with 2-aminoimidazole could provide a model scenario for starting from the (a) phosphorylation of nucleosides to form mononucleotides, (b) activation of mononucleotides for use by ribozymes for ligation, and (c) conversion of mononucleotides to nucleoside-triphosphates (NTPs), which are the substrates used in extant biology. , …”

Section: Discussionmentioning

confidence: 99%

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Enhancing Prebiotic Phosphorylation and Modulating the Regioselectivity of Nucleosides with Diamidophosphate

Cruz,

Jiménez,

Krishnamurthy

2023

J. Am. Chem. Soc.

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Among the many prebiotic phosphorylation chemistries investigated, diamidophosphate (DAP) has shown promising potential for nucleoside phosphorylation. Herein, we show that DAP's phosphorylation capability is enhanced significantly (up to 90%) in wet−dry cycles by a range of prebiotically plausible pHs (6−10) and temperatures (up to 80 °C) in the presence of additives such as formamide, cyanamide, urea, guanidine, 2-aminoimidazole, and hydantoin. For ribonucleosides, the main products are the 2′,3′-cyclic phosphates along with the corresponding 2′-and 3′phosphates, while deoxyribonucleosides form 5′-and 3′-phosphates, the ratios of which are affected by cycles and the presence and nature of the additives. A simple change of temperature to 80 °C with additives leads to higher conversion yields (≈80−90%) with an increased level of 5′-phosphorylation (≈40−49%). This demonstration of enhancing and controlling the regioselectivity of DAP-mediated phosphorylation by a range of additives and conditions potentiates transitioning to the search for more efficient catalysts, enabling regiospecific phosphorylations and oligonucleotide formation in the same milieu and setting.

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Section: Discussionmentioning

confidence: 56%

Section: Journal Of the Americanmentioning

confidence: 79%

Section: Discussionmentioning

confidence: 99%

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Enhancing Prebiotic Phosphorylation and Modulating the Regioselectivity of Nucleosides with Diamidophosphate

Cruz,

Jiménez,

Krishnamurthy

2023

J. Am. Chem. Soc.

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“…Assuming that RNA arose before ATP is nearly impossible, as ATP is a monomer of RNA (the activated form). RNA polymerases only work with NTPs and most prebiotic chemists agree that NTPs precede RNA chains [46,47] as NMPs cannot be polymerized without strong condensing agents. Assuming that once AMP (ADP or ATP) arose it only participated in RNA polymerization seems naïve.…”

Section: Resultsmentioning

confidence: 99%

Small-molecule autocatalytic networks are universal metabolic fossils

Xavier

Kauffman

2022

Phil. Trans. R. Soc. A.

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Life and the genetic code are self-referential and so are autocatalytic networks made of simpler, small molecules. Several origins of life theories postulate autocatalytic chemical networks preceding the primordial genetic code, yet demonstration with biochemical systems is lacking. Here, small-molecule reflexively autocatalytic food-generated networks (RAFs) ranging in size from 3 to 619 reactions were found in all of 6683 prokaryotic metabolic networks searched. The average maximum RAF size is 275 reactions for a rich organic medium and 93 for a medium with a single organic cofactor, NAD. In the rich medium, all universally essential metabolites are produced with the exception of glycerol-1-p (archaeal lipid precursor), phenylalanine, histidine and arginine. The 300 most common reactions, present in at least 2732 RAFs, are mostly involved in amino acid biosynthesis and the metabolism of carbon, 2-oxocarboxylic acid and purines. ATP and NAD are central in generating network complexity, and because ATP is also one of the monomers of RNA, autocatalytic networks producing redox and energy currencies are a strong candidate niche of the origin of a primordial information-processing system. The wide distribution of small-molecule autocatalytic networks indicates that molecular reproduction may be much more prevalent in the Universe than hitherto predicted. This article is part of the theme issue 'Emergent phenomena in complex physical and socio-technical systems: from cells to societies'.

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“…Similar mechanisms could in principle be implemented in RNA autocatalytic networks. In particular, recombinases have been shown to pre‐process RNA fragments for their own synthesis [68], and ribozymes could be evolved to catalyse the synthesis of one of their nucleotides [115]. Yet another possibility is recycling mechanisms, where access to building blocks is mediated by the processing of products instead of resources.…”

Section: Implementing Darwinian Properties In Rna Systemsmentioning

confidence: 99%

Abiogenesis through gradual evolution of autocatalysis into template‐based replication

et al. 2022

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How life emerged from inanimate matter is one of the most intriguing questions posed to modern science. Central to this research are experimental attempts to build systems capable of Darwinian evolution. RNA catalysts (ribozymes) are a promising avenue, in line with the RNA world hypothesis whereby RNA pre-dated DNA and proteins. Since evolution in living organisms relies on template-based replication, the identification of a ribozyme capable of replicating itself (an RNA self-replicase) has been a major objective. However, no self-replicase has been identified to date. Alternatively, autocatalytic systems involving multiple RNA species capable of ligation and recombination may enable self-reproduction. However, it remains unclear how evolution could emerge in autocatalytic systems. In this review, we examine how experimentally feasible RNA reactions catalysed by ribozymes could implement the evolutionary properties of variation, heredity and reproduction, and ultimately allow for Darwinian evolution. We propose a gradual path for the emergence of evolution, initially supported by autocatalytic systems leading to the later appearance of RNA replicases.

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

Cited by 4 publications

References 64 publications

Enhancing Prebiotic Phosphorylation and Modulating the Regioselectivity of Nucleosides with Diamidophosphate

Enhancing Prebiotic Phosphorylation and Modulating the Regioselectivity of Nucleosides with Diamidophosphate

Small-molecule autocatalytic networks are universal metabolic fossils

Abiogenesis through gradual evolution of autocatalysis into template‐based replication

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