Low-temperature gas-phase formation of cyclopentadiene and its role in the formation of aromatics in the interstellar medium.

Autor: Yang Z; Department of Chemistry, University of Hawai'i at Manoa, Honolulu, HI 96822., Medvedkov IA; Department of Chemistry, University of Hawai'i at Manoa, Honolulu, HI 96822., Goettl SJ; Department of Chemistry, University of Hawai'i at Manoa, Honolulu, HI 96822., Nikolayev AA; Laboratory of Combustion Physics and Chemistry, Samara National Research University, Samara 443086, Russia., Mebel AM; Department of Chemistry and Biochemistry, Florida International University, Miami, FL 33199., Li X; Xinjiang Astronomical Observatory, Chinese Academy of Sciences, Urumqi, Xinjiang 830011, People's Republic of China.; Key Laboratory of Radio Astronomy, Chinese Academy of Sciences, Urumqi, Xinjiang 830011, People's Republic of China.; Key Laboratory of Radio Astronomy and Technology, Chinese Academy of Sciences, Beijing 100101, People's Republic of China., Kaiser RI; Department of Chemistry, University of Hawai'i at Manoa, Honolulu, HI 96822.
Jazyk: angličtina
Zdroj: Proceedings of the National Academy of Sciences of the United States of America [Proc Natl Acad Sci U S A] 2024 Dec 17; Vol. 121 (51), pp. e2409933121. Date of Electronic Publication: 2024 Dec 11.
DOI: 10.1073/pnas.2409933121
Abstrakt: The cyclopentadiene (C 5 H 6 ) molecule has emerged as a molecular building block of nonplanar polycyclic aromatic hydrocarbons (PAHs) and carbonaceous nanostructures such as corannulene (C 20 H 10 ), nanobowls (C 40 H 10 ), and fullerenes (C 60 ) in deep space. However, the underlying elementary gas-phase processes synthesizing cyclopentadiene from acyclic hydrocarbon precursors have remained elusive. Here, by merging crossed molecular beam experiments with rate coefficient calculations and comprehensive astrochemical modeling, we afford persuasive testimony on an unconventional low-temperature cyclization pathway to cyclopentadiene from acyclic precursors through the reaction of the simplest diatomic organic radical-methylidyne (CH)-with 1,3-butadiene (C 4 H 6 ) representing main route to cyclopentadiene observed in TaurusMolecular Cloud. This facile route provides potential solution for the incorporation of the cyclopentadiene moiety in complex aromatic systems via bottom-up molecular mass growth processes and offers an entry point to the low-temperature chemistry in deep space leading eventually to nonplanar PAHs in our carbonaceous Universe.
Competing Interests: Competing interests statement:The authors declare no competing interest.
Databáze: MEDLINE
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