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Unravelling the Enigma of Nonoxidative Conversion of Methane on Iron Single‐Atom Catalysts
Author(s) -
Liu Yuan,
Liu JinCheng,
Li TengHao,
Duan ZengHui,
Zhang TianYu,
Yan Ming,
Li WanLu,
Xiao Hai,
Wang YangGang,
Chang ChunRan,
Li Jun
Publication year - 2020
Publication title -
angewandte chemie international edition
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 5.831
H-Index - 550
eISSN - 1521-3773
pISSN - 1433-7851
DOI - 10.1002/anie.202003908
Subject(s) - catalysis , methane , chemistry , reaction mechanism , desorption , hydrogen atom , photochemistry , atom (system on chip) , hydrogen , phase (matter) , inorganic chemistry , adsorption , organic chemistry , alkyl , computer science , embedded system
Abstract The direct, nonoxidative conversion of methane on a silica‐confined single‐atom iron catalyst is a landmark discovery in catalysis, but the proposed gas‐phase reaction mechanism is still open to discussion. Here, we report a surface reaction mechanism by computational modeling and simulations. The activation of methane occurs at the single iron site, whereas the dissociated methyl disfavors desorption into gas phase under the reactive conditions. In contrast, the dissociated methyl prefers transferring to adjacent carbon sites of the active center (Fe 1 ©SiC 2 ), followed by C−C coupling and hydrogen transfer to produce the main product (ethylene) via a key −CH−CH 2 intermediate. We find a quasi Mars–van Krevelen (quasi‐MvK) surface reaction mechanism involving extracting and refilling the surface carbon atoms for the nonoxidative conversion of methane on Fe 1 ©SiO 2 and this surface process is identified to be more plausible than the alternative gas‐phase reaction mechanism.