Enhanced catalytic performance of single-atom Cu on Mo2C toward CO2/CO hydrogenation to methanol : a first-principles study
Vidal-López, Anna (Universitat Autònoma de Barcelona. Departament de Química)
Díaz López, Estefanía (Universitat Autònoma de Barcelona. Departament de Química)
Comas-Vives, Aleix (Universitat Autònoma de Barcelona. Departament de Química)

Data:	2024
Resum:	CO emissions harm the environment due to their pivotal role in fostering climate change and ocean acidification. One way to take advantage of CO is to use it as a precursor to chemical materials to enable energy transition. The CO to methanol conversion from green H is a promising option. The silica-supported Cu/MoCT (MXene) catalyst displayed higher activity than the industrial reference system Cu/ZnO/AlO. To better understand CO hydrogenation in Cu/MoCT and related processes under reaction conditions (CO hydrogenation and reverse water gas shift reaction), we performed periodic DFT calculations to evaluate the methanol synthesis reaction mechanism using our previously calibrated theoretical model against experiment characterization. Our results show the crucial role played by the Cu/MoCT interface in providing low-energy pathways to facilitate the hydrogenation of CO to methanol, where both the Cu atom and the MoCT support participate in the reaction mechanism. The findings showcase the unique pathways provided by this supported single-atom catalyst, allowing the successive heterolytic cleavages of molecular hydrogen (H) to form HCOO*, HCOOH*, and HCOOH* species with co-adsorbed hydrogen in contrast with classical heterogeneous catalysts based on Cu NPs supported on oxides. Thus, CHOH is readily formed under reaction conditions. CO also forms via the reverse water-gas shift (RWGS) reaction, which can be hydrogenated to methanol. These findings open new avenues to understanding CO and CO hydrogenation by exploiting single-atom catalysts and metal-support interfaces.
Ajuts:	Agencia Estatal de Investigación PID2021-128416NB-I00 Ministerio de Ciencia e Innovación PRE2019-089647
Nota:	Altres ajuts: acords transformatius de la UAB
Drets:	Aquest document està subjecte a una llicència d'ús Creative Commons. Es permet la reproducció total o parcial, la distribució, la comunicació pública de l'obra i la creació d'obres derivades, sempre que no sigui amb finalitats comercials, i sempre que es reconegui l'autoria de l'obra original.
Llengua:	Anglès
Document:	Article ; recerca ; Versió publicada
Matèria:	Catalytic performance ; CO 2 emission ; CO hydrogenation ; First-principle study ; Ocean acidifications ; Reaction conditions ; Reaction mechanism ; Reverse water-gas shift reaction ; Single-atoms ; ]+ catalyst
Publicat a:	Catalysis science & technology, Vol. 14, Issue 23 (October 2024) , p. 6904-6916, ISSN 2044-4761

DOI: 10.1039/d4cy00703d

13 p, 2.0 MB

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