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Title: Boosting the activity of transition metal carbides towards methane activation by nanostructuring
Author: Figueras Valls, Marc
Gutiérrez, Ramon A.
Prats Garcia, Hèctor
Viñes Solana, Francesc
Ramírez, Pedro J.
Illas i Riera, Francesc
Rodriguez, J.A.
Keywords: Carburs
Teoria del funcional de densitat
Density functionals
Issue Date: 13-Mar-2020
Publisher: Royal Society of Chemistry
Abstract: The interaction of methane with pristine surfaces of bulk MoC and Mo2C is known to be weak. In contrast, a series of X-ray photoelectron spectroscopy (XPS) experiments, combined with thermal desorption mass spectroscopy (TDS), for MoCy (y = 0.5-1.3) nanoparticles supported on Au(111)¿which is completely inert towards CH4¿show that these systems adsorb and dissociate CH4 at room temperature and low CH4 partial pressure. This industrially-relevant finding has been further investigated with accurate density functional theory (DFT) based calculations on a variety of MoCy supported model systems. The DFT calculations reveal that the MoCy/Au(111) systems can feature low C-H bond scission energy barriers, smaller than the CH4 adsorption energy. Our theoretical results for bulk surfaces of Mo2C and MoC show that a simple Brønsted-Evans-Polanyi (BEP) relationship holds for C-H bond scission on these systems. However, this is not the case for methane activation on the MoCy nanoparticles as a consequence of their unique electronic and chemical properties. The discovery that supported molybdenum carbide nanoparticles are able to activate methane at room temperature paves the road towards the design of a new family of active carbide catalysts for methane activation and valorisation, with important implications in climate change mitigation and carbon cycle closure.
Note: Versió postprint del document publicat a:
It is part of: Physical Chemistry Chemical Physics, 2020, vol. 22, num. 13, p. 7110-7118
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ISSN: 1463-9076
Appears in Collections:Articles publicats en revistes (Ciència dels Materials i Química Física)

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