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Non‐oxidative Methane Coupling over Silica versus Silica‐Supported Iron(II) Single Sites
Author(s) -
Šot Petr,
Newton Mark A.,
Baabe Dirk,
Walter Marc D.,
Bavel Alexander P.,
Horton Andrew D.,
Copéret Christophe,
Bokhoven Jeroen A.
Publication year - 2020
Publication title -
chemistry – a european journal
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 1.687
H-Index - 242
eISSN - 1521-3765
pISSN - 0947-6539
DOI - 10.1002/chem.202001139
Subject(s) - reactivity (psychology) , oxidative coupling of methane , methane , selectivity , chemistry , hydrocarbon , induction period , inorganic chemistry , photochemistry , catalysis , organic chemistry , medicine , alternative medicine , pathology
Abstract Non‐oxidative CH 4 coupling is promoted by silica with incorporated iron sites, but the role of these sites and their speciation under reaction conditions are poorly understood. Here, silica‐supported iron(II) single sites, prepared via surface organometallic chemistry and stable at 1020 °C in vacuum, are shown to rapidly initiate CH 4 coupling at 1000 °C, leading to 15–22 % hydrocarbons selectivity at 3–4 % conversion. During this process, iron reduces and forms carburized iron(0) nanoparticles. This reactivity contrasts with what is observed for (iron‐free) partially dehydroxylated silica, that readily converts methane, albeit with low hydrocarbon selectivity and after an induction period. This study supports that iron sites facilitate faster initiation of radical reactions and tame the surface reactivity.