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Direct evidence for a single-step cold radiation-induced synthesis of acetonitrile and isoacetonitrile from the 1:1 CH4∙∙∙HCN complex: is it a missing link between inorganic and prebiotic astrochemistry?статья
Статья опубликована в высокорейтинговом журнале
Статья опубликована в журнале из списка Web of Science и/или ScopusДата последнего поиска статьи во внешних источниках: 12 января 2022 г.
- Авторы: Volosatova Anastasia D., Lukianova Mariia A., Zasimov Pavel V., Feldman Vladimir I.
- Журнал: Physical Chemistry Chemical Physics
- Том: 23
- Номер: 34
- Год издания: 2021
- Издательство: Royal Society of Chemistry
- Местоположение издательства: United Kingdom
- Первая страница: 18449
- Последняя страница: 18460
- DOI: 10.1039/d1cp01598b
- Аннотация: Nitriles are important constituents of the extraterrestrial media. Nitriles are supposed to play a crucial role in the prebiotic chemistry occurring in the interstellar medium. In this work, we have investigated the low-temperature radiation-induced transformations of a 1:1 CH4∙∙∙HCN complex as a plausible precursor of the simplest nitriles using the matrix isolation approach with FTIR spectroscopic detection. The parent complexes isolated in a noble gas (Ng) matrix were obtained by deposition of the CH4/HCN/Ng gaseous mixture and characterized by comparison of experimental complexation-induced shifts of the HCN fundamentals with the results of the ab initio calculations. It was found that the X-ray irradiation of low-temperature matrices containing isolated 1:1 CH4∙∙∙HCN complex resulted in the formation of acetonitrile (CH3CN) and isoacetonitrile (CH3NC) and it appears to be the first experimental evidence for the formation of C2 nitriles (acetonitrile and isoacetonitrile) from such “building block”. Additionally, a 1:1 CH4∙∙∙HNC complex was tentatively assigned in the irradiated Ar and Kr matrices. It is demonstrated that the matrix has a strong effect on the CH3CN/CH3NC yields ratio, which dramatically increases in the row Ar < Kr < Xe. Also, the efficiency of the radiation-induced formation of the CH4∙∙∙HNC complex was shown to decrease from Ar to Kr. It is believed that the proposed pathway for acetonitrile formation may be a significant step in the radiation-induced evolution leading to complex organic molecules and biomolecules under astrochemical conditions. Furthermore, the obtained results provide a prominent example of the impact of very weak intermolecular interactions on the radiation-induced transformations in cold media.
- Добавил в систему: Засимов Павел Валерьевич