Engineering the Cu/Mo2CTx (MXene) interface to drive CO2 hydrogenation to methanol
Abstract
Development of efficient catalysts for the direct hydrogenation of CO2 to methanol is essential for the valorization of this abundant feedstock. Here we show that a silica-supported Cu/Mo2CTx (MXene) catalyst achieves a higher intrinsic methanol formation rate per mass Cu than the reference Cu/SiO2 catalyst with a similar Cu loading. The Cu/Mo2CTx interface can be engineered due to the higher affinity of Cu for the partially reduced MXene surface (in preference to the SiO2 surface) and the mobility of Cu under H2 at 500 °C. With increasing reduction time, the Cu/Mo2CTx interface becomes more Lewis acidic due to the higher amount of Cu+ sites dispersed onto the reduced Mo2CTx and this correlates with an increased rate of CO2 hydrogenation to methanol. The critical role of the interface between Cu and Mo2CTx is further highlighted by density functional theory calculations that identify formate and methoxy species as stable reaction intermediates. [Figure not available: see fulltext.] Mehr anzeigen
Persistenter Link
https://doi.org/10.3929/ethz-b-000512844Publikationsstatus
publishedExterne Links
Zeitschrift / Serie
Nature CatalysisBand
Seiten / Artikelnummer
Verlag
Macmillan PublishersOrganisationseinheit
03865 - Müller, Christoph R. / Müller, Christoph R.
03872 - Copéret, Christophe / Copéret, Christophe
Förderung
800419 - Sorbent-enhanced Steam Biomass Reforming for Integrated Bio-energy with Carbon Capture and (EC)
819573 - Advancing CO2 Capture Materials by Atomic Scale Design: the Quest for Understanding (EC)
ETH-40 17-2 - Advanced materials by atomic layer deposition (ALD): from controlling porosity of ALD-grown overcoats to the molecular understanding of silica-aluminas (ETHZ)
ETH-44 16-2 - The direct integration of CO2 conversion into CO2 capture: Development of model bi-functional Cu-MgO-MOx materials through the elucidation of the carbonation mechanism and active sites for CO2 hydrogenation (ETHZ)