Gas phase synthesis of the C40 nano bowl C40H10
Abstract
Nanobowls represent vital molecular building blocks of end-capped nanotubes and fullerenes detected in combustion systems and in deep space such as toward the planetary nebula TC-1, but their fundamental formation mechanisms have remained elusive. By merging molecular beam experiments with electronic structure calculations, we reveal a complex chain of reactions initiated through the gas-phase preparation of benzocorannulene (C24H12) via ring annulation of the corannulenyl radical (C20H9•) by vinylacetylene (C4H4) as identified isomer-selectively in situ via photoionization efficiency curves and photoion mass-selected threshold photoelectron spectra. In silico studies provided compelling evidence that the benzannulation mechanism can be expanded to pentabenzocorannulene (C40H20) followed by successive cyclodehydrogenation to the C40 nanobowl (C40H10) – a fundamental building block of buckminsterfullerene (C60). This high-temperature pathway opens up isomer-selective routes to nanobowls via resonantly stabilized free-radical intermediates and ring annulation in circumstellar envelopes of carbon stars and planetary nebulae as their descendants eventually altering our insights of the complex chemistry of carbon in our Galaxy.
- Authors:
-
[2];
[3];
[4];
[1];
[1];
[2]
- Florida International Univ. (FIU), Miami, FL (United States)
- Univ. of Hawaii at Manoa, Honolulu, HI (United States)
- Florida International Univ. (FIU), Miami, FL (United States); Johns Hopkins Univ., Baltimore, MD (United States)
- Paul Scherrer Inst. (PSI), Villigen (Switzerland)
- Tianjin Univ. (China)
- Publication Date:
- Research Org.:
- Univ. of Hawaii at Manoa, Honolulu, HI (United States); Florida International Univ. (FIU), Miami, FL (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1963547
- Grant/Contract Number:
- FG02-03ER15411; FG02-04ER15570
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Nature Communications
- Additional Journal Information:
- Journal Volume: 14; Journal Issue: 1; Related Information: https://www.nature.com/articles/s41467-023-37058-y#Sec10; Journal ID: ISSN 2041-1723
- Publisher:
- Nature Publishing Group
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Reaction kinetics and dynamics; Laboratory astrophysics; Reaction mechanisms
Citation Formats
Tuli, Lotefa B., Goettl, Shane J., Turner, Andrew M., Howlader, A. Hasan, Hemberger, Patrick, Wnuk, Stanislaw F., Guo, Tianjian, Mebel, Alexander M., and Kaiser, Ralf I. Gas phase synthesis of the C40 nano bowl C40H10. United States: N. p., 2023.
Web. doi:10.1038/s41467-023-37058-y.
Tuli, Lotefa B., Goettl, Shane J., Turner, Andrew M., Howlader, A. Hasan, Hemberger, Patrick, Wnuk, Stanislaw F., Guo, Tianjian, Mebel, Alexander M., & Kaiser, Ralf I. Gas phase synthesis of the C40 nano bowl C40H10. United States. https://doi.org/10.1038/s41467-023-37058-y
Tuli, Lotefa B., Goettl, Shane J., Turner, Andrew M., Howlader, A. Hasan, Hemberger, Patrick, Wnuk, Stanislaw F., Guo, Tianjian, Mebel, Alexander M., and Kaiser, Ralf I. Sat .
"Gas phase synthesis of the C40 nano bowl C40H10". United States. https://doi.org/10.1038/s41467-023-37058-y. https://www.osti.gov/servlets/purl/1963547.
@article{osti_1963547,
title = {Gas phase synthesis of the C40 nano bowl C40H10},
author = {Tuli, Lotefa B. and Goettl, Shane J. and Turner, Andrew M. and Howlader, A. Hasan and Hemberger, Patrick and Wnuk, Stanislaw F. and Guo, Tianjian and Mebel, Alexander M. and Kaiser, Ralf I.},
abstractNote = {Nanobowls represent vital molecular building blocks of end-capped nanotubes and fullerenes detected in combustion systems and in deep space such as toward the planetary nebula TC-1, but their fundamental formation mechanisms have remained elusive. By merging molecular beam experiments with electronic structure calculations, we reveal a complex chain of reactions initiated through the gas-phase preparation of benzocorannulene (C24H12) via ring annulation of the corannulenyl radical (C20H9•) by vinylacetylene (C4H4) as identified isomer-selectively in situ via photoionization efficiency curves and photoion mass-selected threshold photoelectron spectra. In silico studies provided compelling evidence that the benzannulation mechanism can be expanded to pentabenzocorannulene (C40H20) followed by successive cyclodehydrogenation to the C40 nanobowl (C40H10) – a fundamental building block of buckminsterfullerene (C60). This high-temperature pathway opens up isomer-selective routes to nanobowls via resonantly stabilized free-radical intermediates and ring annulation in circumstellar envelopes of carbon stars and planetary nebulae as their descendants eventually altering our insights of the complex chemistry of carbon in our Galaxy.},
doi = {10.1038/s41467-023-37058-y},
journal = {Nature Communications},
number = 1,
volume = 14,
place = {United States},
year = {Sat Mar 18 00:00:00 EDT 2023},
month = {Sat Mar 18 00:00:00 EDT 2023}
}
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