Unlocking mixed oxides with unprecedented stoichiometries from heterometallic metal-organic frameworks for the catalytic hydrogenation of CO2

Javier Castells-Gil, Samy Ould-Chikh, Adrian Ramírez, Rafia Ahmad, Gonzalo Prieto, Alberto Rodríguez Gómez, Luis Carlos Garzon Tovar, Selvedin Telalovic, Lingmei Liu, Alessandro Genovese, Natalia M. Padial, Antonio Aguilar-Tapia, Pierre Bordet, Luigi Cavallo, Carlos Martí-Gastaldo, Jorge Gascon

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Their complex surface chemistry and high oxygen lattice mobilities place mixed-metal oxides among the most important families of materials. Modulation of stoichiometry in mixed-metal oxides has been shown to be a very powerful tool for tuning optical and catalytic properties. However, accessing different stoichiometries is not always synthetically possible. Here, we show that the thermal decomposition of the recently reported metal-organic framework MUV-101(Fe, Ti) results in the formation of carbon-supported titanomaghemite nanoparticles with an unprecedented Fe/Ti ratio close to 2, not achievable by soft-chemistry routes. The resulting titanomaghemite phase displays outstanding catalytic activity for the production of CO from CO2 via the reverse water-gas shift (RWGS) reaction with CO selectivity values of ca. 100% and no signs of deactivation after several days on stream. Theoretical calculations suggest that the reaction proceeds through the formation of COOH* species, favoring in this way CO over other byproducts.
Original languageEnglish (US)
JournalChem Catalysis
StatePublished - Apr 26 2021

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