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.

SUBMITTER: Tuli LB 

PROVIDER: S-EPMC10024697 | biostudies-literature | 2023 Mar

REPOSITORIES: biostudies-literature