4.6 Article

Gas-phase synthesis of corannulene - a molecular building block of fullerenes

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PHYSICAL CHEMISTRY CHEMICAL PHYSICS
卷 23, 期 10, 页码 5740-5749

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ROYAL SOC CHEMISTRY
DOI: 10.1039/d0cp06537d

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资金

  1. US Department of Energy, Basic Energy Sciences [DE-FG02-03ER15411, DE-FG02-04ER15570]
  2. Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy through the Gas Phase Chemical Physics Program, Chemical Sciences Division [DE-AC02-05CH11231]
  3. Ministry of Higher Education and Science of the Russian Federation [14.Y26.31.0020]

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Studies have shown that corannulene can be synthesized in the gas phase under specific conditions, revealing critical reaction mechanisms for understanding the origin and evolution of the molecular universe.
Fullerenes (C-60, C-70) detected in planetary nebulae and carbonaceous chondrites have been implicated to play a key role in the astrochemical evolution of the interstellar medium. However, the formation mechanism of even their simplest molecular building block-the corannulene molecule (C20H10)-has remained elusive. Here we demonstrate via a combined molecular beams and ab initio investigation that corannulene can be synthesized in the gas phase through the reactions of 7-fluoranthenyl (C18H9 center dot) and benzo[ghi]fluoranthen-5-yl (C18H9 center dot) radicals with acetylene (C2H2) mimicking conditions in carbon-rich circumstellar envelopes. This reaction sequence reveals a reaction class in which a polycyclic aromatic hydrocarbon (PAH) radical undergoes ring expansion while simultaneously forming an out-of-plane carbon backbone central to 3D nanostructures such as buckybowls and buckyballs. These fundamental reaction mechanisms are critical in facilitating an intimate understanding of the origin and evolution of the molecular universe and, in particular, of carbon in our galaxy.

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