The potential energy surface for the formation of protonated uracil (UH+) from urea and HC3O+ was explored by performing quantum chemical complete basis set-QB3 calculations. A barrierless pathway was found for the formation of UH+, which was estimated to occur in the interstellar medium (ISM) much faster than the timescale of chemical revolution of typical dense interstellar clouds. Investigation of further reactions of UH+ formed through the obtained pathway led to the conclusion that uracil could be produced on icy grain surfaces but not in the gas phase of the ISM.
Get full access to this article
View all access options for this article.
References
1.
BaerT and HaseWL (1996) Unimolecular Reaction Dynamics: Theory and Experiments. Oxford University Press, New York.
2.
BellocheA, GarrodRT, MüllerHSP, et al. (2019) Re-exploring molecular complexity with ALMA (ReMoCA): interstellar detection of urea. Astrono Astrophys, 628:A10.
3.
BeraPP, NuevoM, MatereseCK, et al. (2016) Mechanisms for the formation of thymine under astrophysical conditions and implications for the origin of life. J Chem Phys, 144:144308.
4.
BeraPP, NuevoM, MilamSN, et al. (2010) Mechanism for the abiotic synthesis of uracil via UV-induced oxidation of pyrimidine in pure H2O ices under astrophysical conditions. J Chem Phys, 133:104303.
5.
BeraPP, SteinT, Head-GordonM, et al. (2017) Mechanisms of the formation of adenine, guanine, and their analogues in UV-irradiated mixed NH3:H2O molecular ices containing purine. Astrobiology, 17:771–785.
6.
CernicharoJ, MarcelinoN, AgúndezM, et al. (2020) Discovery of HC3O+ in space: the chemistry of O-bearing species in TMC-1. Astron Astrophys, 642:L17.
7.
ChoeJC (2017) Water-assisted dimerization of hydrogen cyanide: a computational study. Bull Korean Chem Soc, 38:1531–1533.
8.
ChoeJC (2018) Guanine synthesis from 4-aminoimidazole-5-carbonitrile: a computational mechanistic study. Chem Phys Lett, 708:71–76.
9.
ChoeJC (2019) Dimerization of HCN in interstellar icy grain mantles: a DFT study. Bull Korean Chem Soc, 40:205–206.
10.
ChoeJC (2020a) Formation of cytosine and uracil from cyanoacetylaldehyde and guanidine: a computational study. Bull Korean Chem Soc, 41:382–384.
11.
ChoeJC (2020b) Prebiotic cytosine synthesis from urea in interstellar space: a computational mechanistic study. Astrophys J, 898:13.
12.
ChoeJC (2021) Can cytosine, uracil, and thymine be formed from HC3N and H2NCO+ in interstellar space?. Astrophys J, 914:136.
13.
ChoeJC and KimMH (2019) Dissociation of the ethyl formate radical cation: a computational mechanistic study. Chem Phys Lett, 730:538–543.
14.
da Silva JBP and de AraujoAPM (2017) A new mechanism of guanine-isomer formation from species previously observed in the interstellar medium. ACS Earth Space Chem, 1:376–383.
15.
DunbarRC, KlippensteinSJ, HrušákJ, et al. (1996) Binding energy of Al(C6H6)+ from analysis of radiative association kinetics. J Am Chem Soc, 118:5277–5283.
GerakinesPA, QasimD, FrailS, et al. (2022) Radiolytic destruction of uracil in interstellar and solar system ices. Astrobiology, 22:233–241.
18.
GuptaVP, TandonP, and MishraP (2013) Some new reaction pathways for the formation of cytosine in interstellar space—a quantum chemical study. Adv Space Res, 51:797–811.
19.
HammerPG, YiR, YodaI, et al. (2019) Radiolysis of solid-state nitrogen heterocycles provides clues to their abundance in the early solar system. Int J Astrobiol, 18:289–295.
20.
HerbstE (1985) An update of and suggested increase in calculated radiative association rate coefficients. Astrophys J, 291:226–229.
21.
HerbstE (2001) The chemistry of interstellar space. Chem Soc Rev, 30:168–176.
22.
IoppoloS, CuppenH, RomanzinC, et al. (2008) Laboratory evidence for efficient water formation in interstellar ices. Astrophys J, 686:1474.
23.
IoppoloS, CuppenHM, RomanzinC, et al. (2010) Water formation at low temperatures by surface O2 hydrogenation I: characterization of ice penetration. Phys Chem Chem Phys, 12:12065–12076.
24.
JeilaniYA, NguyenHT, NewalloD, et al. (2013) Free radical routes for prebiotic formation of DNA nucleobases from formamide. Phys Chem Chem Phys, 15:21084–21093.
25.
JeilaniYA, FearceC, and NguyenMT (2015) Acetylene as an essential building block for prebiotic formation of pyrimidine bases on Titan. Phys Chem Chem Phys, 17:24294–24303.
26.
JeilaniYA, WilliamsPN, WaltonS, et al. (2016) Unified reaction pathways for the prebiotic formation of RNA and DNA nucleobases. Phys Chem Chem Phys, 18:20177–20188.
27.
Jiménez-SerraI, Martín-PintadoJ, RivillaVM, et al. (2020) Toward the RNA-world in the interstellar medium—detection of urea and search of 2-amino-oxazole and simple sugars. Astrobiology, 20:1048–1066.
28.
JungSH and ChoeJC (2013) Mechanisms of prebiotic adenine synthesis from HCN by oligomerization in the gas phase. Astrobiology, 13:465–475.
29.
KaurS and SharmaP (2019) Cyanoacetaldehyde as a building block for prebiotic formation of pyrimidines. Int J Quantum Chem, 119:e25886.
30.
KitadaiN and MaruyamaS (2018) Origins of building blocks of life: a review. Geosci Front, 9:1117–1153.
31.
KobayashiK (2019) Prebiotic synthesis of bioorganic compounds by simulation experiments. In: Astrobiology, edited by YamagishiA., KakegawaT. and UsuiT.. Springer, Singapore, pp 43–61.
32.
LuS, MengZ, XieP, et al. (2021) Gas-phase formation of interstellar nucleobases from dehydrogenated formamide and vinyl cyanide. Astron Astrophys, 656:A84.
33.
MarcusRA and RiceOK (1951) The kinetics of the recombination of methyl radicals and iodine atoms. J Phys Colloid Chem, 55:894–908.
34.
MatereseCK, NuevoM, BeraPP, et al. (2013) Thymine and other prebiotic molecules produced from the ultraviolet photo-irradiation of pyrimidine in simple astrophysical ice analogs. Astrobiology, 13:948–962.
35.
MatereseCK, NuevoM, and SandfordSA (2017) The formation of nucleobases from the ultraviolet photoirradiation of purine in simple astrophysical ice analogues. Astrobiology, 17:761–770.
36.
MatereseCK, NuevoM, McDowellBL, et al. (2018) The photochemistry of purine in ice analogs relevant to dense interstellar clouds. Astrophys J, 864:44.
37.
Menor-SalvánC and Marín-YaseliMR (2013) A new route for the prebiotic synthesis of nucleobases and hydantoins in water/ice solutions involving the photochemistry of acetylene. Chem Eur J, 19:6488–6497.
38.
MillerSL (1953) A production of amino acids under possible primitive earth conditions. Science, 117:528–529.
39.
MiyauchiN, HidakaH, ChigaiT, et al. (2008) Formation of hydrogen peroxide and water from the reaction of cold hydrogen atoms with solid oxygen at 10 K. Chem Phys Lett, 456:27–30.
40.
MolinaER, SalpinJ-Y, SpeziaR, et al. (2016) On the gas phase fragmentation of protonated uracil: a statistical perspective. Phys Chem Chem Phys, 18:14980–14990.
41.
Montgomery JrJA, FrischMJ, OchterskiJW, et al. (1999) A complete basis set model chemistry. VI. Use of density functional geometries and frequencies. J Chem Phys, 110:2822–2827.
42.
NguyenHT, JeilaniYA, HungHM, et al. (2015) Radical pathways for the prebiotic formation of pyrimidine bases from formamide. J Phys Chem A, 119:8871–8883.
43.
NuevoM, MilamSN, SandfordSA, et al. (2009) Formation of uracil from the ultraviolet photo-irradiation of pyrimidine in pure H2O ices. Astrobiology, 9:683–695.
44.
NuevoM, MilamSN, and SandfordSA (2012) Nucleobases and prebiotic molecules in organic residues produced from the ultraviolet photo-irradiation of pyrimidine in NH3 and H2O + NH3 ices. Astrobiology, 12:295–314.
45.
NuevoM, MatereseCK, and SandfordSA (2014) The photochemistry of pyrimidine in realistic astrophysical ices and the production of nucleobases. Astrophys J, 793:125.
46.
ObaY, TakanoY, NaraokaH, et al. (2019) Nucleobase synthesis in interstellar ices. Nat Comm, 10:1–8.
47.
OróJ (1960) Synthesis of adenine from ammonium cyanide. Biochem Biophys Res Commun, 2:407–412.
48.
OróJ (1961) Mechanism of synthesis of adenine from hydrogen cyanide under possible primitive earth conditions. Nature, 191:1193–1194.
49.
PearceBK and PudritzRE (2015) Seeding the pregenetic Earth: meteoritic abundances of nucleobases and potential reaction pathways. Astrophys J, 807:85.
50.
PeetersZ, BottaO, CharnleyS, et al. (2003) The astrobiology of nucleobases. Astrophys J, 593:L129.
51.
PillingS, AndradeD, do NascimentoE, et al. (2011) Photostability of gas-and solid-phase biomolecules within dense molecular clouds due to soft X-rays. Mon Not R Astron Soc, 411:2214–2222.
52.
RoyD, NajafianK, and von Ragué SchleyerP (2007) Chemical evolution: the mechanism of the formation of adenine under prebiotic conditions. Proc Natl Acad Sci U S A, 104:17272–17277.
53.
RufA, LangeJ, EddhifB, et al. (2019) The challenging detection of nucleobases from pre-accretional astrophysical ice analogs. Astrophys J Lett, 887:L31.
54.
Sadr-AraniL, MignonP, ChermetteH, et al. (2014) Theoretical and experimental study of the fragmentation of protonated uracil. Chem Phys Lett, 605:108–114.
55.
SmithIWM, TalbiD, and HerbstE (2001) The production of HCN dimer and more complex oligomers in dense interstellar clouds. Astron Astrophys, 369:611–615.
56.
TielensAG (2021) Molecular Astrophysics. Cambridge University Press, New York.
57.
WakelamV, SmithIWM, HerbstE, et al. (2010) Reaction networks for interstellar chemical modelling: improvements and challenges. Space Sci Rev, 156:13–72.
58.
WangT and BowieJH (2012) Can cytosine, thymine and uracil be formed in interstellar regions? A theoretical study. Org Biomol Chem, 10:652–662.
59.
YimMK and ChoeJC (2011) Formation of C4H4•+ from the pyridine radical cation: a theoretical mechanistic and kinetic study. J Phys Chem A, 115:3087–3094.
60.
YimMK and ChoeJC (2012) Dimerization of HCN in the gas phase: a theoretical mechanistic study. Chem Phys Lett, 538:24–28.
61.
ZamirriL, UgliengoP, CeccarelliC, et al. (2019) Quantum mechanical investigations on the formation of complex organic molecules on interstellar ice mantles. Review and perspectives. ACS Earth Space Chem, 3:1499–1523.
