Naslov
Intrazeolite CO Methanation by Small Ruthenium Carbonyl Complexes: Translation from Free Clusters into the Cage

Autori
Mravak, Antonija ; Krstić, Marjan ; Lang, Sandra M. ; Bernhardt, Thorsten M. ; Bonačić‐Koutecký, Vlasta

Izvornik
ChemCatChem (1867-3880) 12 (2020), 15; 3857-3862

Vrsta, podvrsta i kategorija rada
Radovi u časopisima, članak, znanstveni

Ključne riječi
CO methanation ; density functional calculations ; fuel cell feed gas purification ; ruthenium carbonyl cluster ; zeolites

Sažetak
Catalytic CO methanation represents an important reaction to improve the feed gas quality for hydrogen fuel cells. Previously, the large potential of small bare and ligated ruthenium clusters as highly selective and active catalysts has been shown by employing gas phase clusters as model systems. Now, density functional theory (DFT) calculations are employed to demonstrate the possibility to translate the gas phase CO methanation reaction mediated by a ligated Ru-4(CO)(13)H-2(+) complex into the framework of a ZSM-5 zeolite. Such a translation, manifested by a reaction pathway which is mechanistically and energetically similar to the gas phase analogue, is possible since the zeolite framework does not influence the reactive center. Furthermore, we reveal the important role of the CO ligand environment in protecting the Ru-4(+) metal core from formation of bonds with the zeolite and in the creation of the reactive center by promoting the cooperatively enhanced adsorption and dissociation of H-2.

Izvorni jezik
Engleski

Znanstvena područja
Fizika, Kemija

POVEZANOST RADA