Geochemical Sources and Availability of Amidophosphates on the Early Earth

Gibard, Clémentine; Gorrell, Ian B.; Jiménez, Eddy I.; Kee, Terence P.; Pasek, Matthew A.; Krishnamurthy, Ramanarayanan

doi:10.1002/ange.201903808

Cited by 29 publications

(27 citation statements)

References 37 publications

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“…However, a recent report has described the synthesis of DAP by reacting the schreibersite surrogate Fe 3 P with concentrated (> 1 M) ammonia solutions. 25 The same study also showed that UV irradiation of HPO 3 2- in ammonia solution provides access to amidophosphate (H 2 N)PO 3 2- ). 25 …”

Section: Experimental Oxidation Of Reduced Phosphorus Speciesmentioning

confidence: 86%

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Supply of phosphate to early Earth by photogeochemistry after meteoritic weathering

2020

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During terrestrial differentiation, the relatively small amount of phosphorus that migrated to the lithosphere was incorporated into igneous rock, predominantly in the form of basic calcium orthophosphate (Ca 10 (PO 4 ) 6 (OH,F,Cl) 2 , apatite). Yet, the highly insoluble nature of calcium apatite presents a significant problem to those contemplating the origin of life given the foundational role of phosphate (PO 4 3- ) in extant biology and the apparent requirement for PO 4 3- as a catalyst, buffer and reagent in prebiotic chemistry. Reduced meteorites such as enstatite chondrites are highly enriched in phosphide minerals, and upon reaction with water these minerals can release phosphorus species of various oxidation states. Here, we demonstrate how reduced phosphorus species can be fully oxidized to PO 4 3- simply by the action of ultraviolet light on H 2 S/HS - . We used low pressure Hg lamps to simulate UV output from the young Sun and 31 P NMR spectroscopy to monitor the progress of reactions. Our experimental findings provide a cosmochemically and geochemically plausible means for supply of PO 4 3- that was widely available to prebiotic chemistry and nascent life on early Earth, and potentially on other planets.

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Section: Experimental Oxidation Of Reduced Phosphorus Speciesmentioning

confidence: 86%

“… 25 The same study also showed that UV irradiation of HPO 3 2- in ammonia solution provides access to amidophosphate (H 2 N)PO 3 2- ). 25 …”

Section: Experimental Oxidation Of Reduced Phosphorus Speciesmentioning

confidence: 86%

Supply of phosphate to early Earth by photogeochemistry after meteoritic weathering

2020

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“…However, CTMP is also formed via the oxidation of phosphite by hydroxyl radicals liberated via geochemical redox processes (Herschy et al, 2018) or from a reducing iron-rich impactor itself. It may also have emerged from phosphonamides which are becoming increasingly attractive as prebiotic phosphorylation agents (Gibard et al, 2019).…”

Section: Fig 2 (Continued)mentioning

confidence: 99%

Abiotic Synthesis of Nucleoside 5′-Triphosphates with Nickel Borate and Cyclic Trimetaphosphate (CTMP)

Kim

Benner

2021

Astrobiology

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While nucleoside 5¢-triphosphates are precursors for RNA in modern biology, the presumed difficulty of making these triphosphates on Hadean Earth has caused many prebiotic researchers to consider other activated species for the prebiotic synthesis of RNA. We report here that nickel(II), in the presence of borate, gives substantial amounts (2-3%) of nucleoside 5¢-triphosphates upon evaporative heating in the presence of urea, salts, and cyclic trimetaphosphate (CTMP). Also recovered are nucleoside 5¢-diphosphates and nucleoside 5¢-monophosphates, both likely arising from 5¢-triphosphate intermediates. The total level of 5¢-phosphorylation is typically 30%. Borate enhances the regiospecificity of phosphorylation, with increased amounts of other phosphorylated species seen in its absence. Experimentally supported paths are already available to make nucleosides in environments likely to have been present on Hadean Earth soon after a midsized 10 21 to 10 23 kg impactor, which would also have delivered nickel to the Hadean surface. Further, sources of prebiotic CTMP continue to be proposed. Thus, these results fill in one of the few remaining steps needed to demystify the prebiotic synthesis of RNA and support a continuous model from atmospheric components to oligomeric RNA that is lacking only a mechanism to obtain homochirality in the product RNA.

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“…In vivo, phosphate groups are added by a free-energy-rich molecule, ATP [24]. Prebiotic robust phosphorylating analogues, that are rich in energy, include trimetaphosphate ions, coming from volcanoes [25] [26], or phosphoramidates [27]. Their ammonolysis products can be substituted to ATP, as ATP is a far too complex assembly to have existed on the primordial Earth.…”

Section: Introductionmentioning

confidence: 99%

Carbamoyl phosphate and its substitutes for the uracil synthesis in origins of life scenarios

Ter-Ovanessian

Rigaud

Mezzetti

et al. 2021

Preprint

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The first step of pyrimidine synthesis along the orotate pathway is studied to test the hypothesis of geochemical continuity of protometabolic pathways at the origins of life. Carbamoyl phosphate (CP) is the first high-energy building block that intervenes in the in vivo synthesis of the uracil ring of UMP. Thus, the likelihood of its occurrence in prebiotic conditions is investigated herein. The evolution of carbamoyl phosphate in water and in ammonia aqueous solutions without enzymes was characterised using ATR-IR, 31P and 13C spectroscopies. Carbamoyl phosphate initially appears stable in water at ambient conditions before transforming to cyanate and carbamate/hydrogenocarbonate species within a matter of hours. Cyanate, less labile than CP, remains a potential carbamoylating agent. In the presence of ammonia, CP decomposition occurs more rapidly and generates urea. We conclude that CP is not a likely prebiotic reagent by itself. Alternatively, cyanate and urea may be more promising substitutes for CP, because they are both “energy-rich” (high free enthalpy molecules in aqueous solutions) and kinetically inert regarding hydrolysis. Energy-rich inorganic molecules such as trimetaphosphate or phosphoramidates were also explored for their suitability as sources of carbamoyl phosphate. Although these species did not generate CP or other carbamoylating agents, they exhibited energy transduction, specifically the formation of high-energy P-N bonds. Future efforts should aim to evaluate the role of carbamoylating agents in aspartate carbamoylation, which is the following reaction in the orotate pathway

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Geochemical Sources and Availability of Amidophosphates on the Early Earth

Cited by 29 publications

References 37 publications

Supply of phosphate to early Earth by photogeochemistry after meteoritic weathering

Supply of phosphate to early Earth by photogeochemistry after meteoritic weathering

Abiotic Synthesis of Nucleoside 5′-Triphosphates with Nickel Borate and Cyclic Trimetaphosphate (CTMP)

Carbamoyl phosphate and its substitutes for the uracil synthesis in origins of life scenarios

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