Gas-phase Oxygenation and Sulfurization Processes of Fullerene Cations
Year: 2025
Type: article
Abstract: Atomic oxygen and sulfur are known to efficiently react with fullerenes and may thus form a long list of oxygenated and sulfurated fullerene species in the interstellar medium (ISM). In this work, the gas-phase collision reactions between fullerene (C60 and C54/56/58) cations and 18O or S atoms are investigated. Oxygenated and sulfurated fullerene cations ([C60 18O1−6]+, [C54/56/58 18O1−3]+ and [C60S1−4]+, [C54/56/58S1−4]+) are efficiently formed. Under laser irradiation, O-atom and CO-unit loss channels are identified in the photodeoxygenation processes; [C60O]+ only has an O-atom loss channel. Smaller fullerene cations can be produced through sequential steps, and species with repeatedly lost CO units, i.e., fullerenes containing odd carbon numbers (e.g., 55 or 57 C atoms), can be produced in the photodeoxygenation processes of oxygenated fullerene cations. A S-atom loss channel and no CS-unit loss channel are identified in the photodesulfurization processes. Through theoretical calculations, the structures of oxygenated and sulfurated fullerene cations (e.g., [C60 18O]+ and [C60S]+) and the bonding energies for the formation reaction pathways are investigated, together with their IR spectra. The exothermic energy for each reaction pathway is relatively high. Consequently, the oxygenation or sulfurization states and forms of fullerene compounds are intricate and complex. In addition, different types of oxygenation and sulfurization bonds are obtained with their evolution. Importantly, we infer that the photodeoxygenation of mono-oxygenated fullerene species or the photodesulfurization of sulfurated fullerene species is not involved in the top-down chemical evolution routes of buckminsterfullerene (C60) in the ISM.
Source: The Astrophysical Journal
Language: English
Subfield: Organic Chemistry
Field: Chemistry
Domain: Physical Sciences
Open Access status: gold
Estimated APC paid: $4,499
OpenAlex ID: W4408238331