Please use this identifier to cite or link to this item: http://hdl.handle.net/2445/113064
Title: Effective and highly selective CO generation from CO2 using a polycrystalline α‑Mo2C catalyst
Author: Liu, Xinayun
Kunkel, Christian
Ramírez de la Piscina, Pilar
Homs Martí, Narcís
Viñes Solana, Francesc
Illas i Riera, Francesc
Keywords: Teoria del funcional de densitat
Catàlisi
Monòxid de carboni
Density functionals
Catalysis
Carbon monoxide
Issue Date: 16-May-2017
Publisher: American Chemical Society
Abstract: Present experiments show that synthesized polycrystalline hexagonal α-Mo2C is a highly efficient and selective catalyst for CO2 uptake and conversion to CO through the reverse water gas shift reaction. The CO2 conversion is ~16% at 673 K, with selectivity towards CO > 99%. CO2 and CO adsorption is monitored by DRIFTS, TPD, and microcalorimetry, and a series of DFT based calculations including the contribution of dispersion terms. The DFT calculations on most stable model surfaces allow for identifying numerous binding sites present on the catalyst surface, leading to a high complexity in measured and interpreted IR- and TPD-spectra. The computational results also explain ambient temperature CO2 dissociation towards CO as resulting from the presence of surface facets such as Mo2C(201)-Mo/C ¿displaying Mo and C surface atoms¿ and Mo-terminated Mo2C(001)-Mo. An ab initio thermodynamics consideration of reaction conditions however demonstrates that these facets bind CO2 and CO + O intermediates too strong for a subsequent removal, whereas the Mo2C(101)-Mo/C exhibits balanced binding properties, serving a possible explanation of the observed reactivity. In summary, results show that polycrystalline α-Mo2C is an economically viable, highly efficient, and selective catalyst for CO generation using CO2 as a feedstock.
Note: Versió postprint del document publicat a: https://doi.org/10.1021/acscatal.7b00735
It is part of: ACS Catalysis, 2017, vol. 7, p. 4323-4335
Related resource: https://doi.org/10.1021/acscatal.7b00735
URI: http://hdl.handle.net/2445/113064
ISSN: 2155-5435
Appears in Collections:Publicacions de projectes de recerca finançats per la UE
Articles publicats en revistes (Ciència dels Materials i Química Física)

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