Modeling the active sites of Co-promoted MoS2 particles by DFT
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Modeling the active sites of Co-promoted MoS2 particles by DFT. / Šarić, Manuel; Rossmeisl, Jan; Moses, Poul Georg.
I: Physical Chemistry Chemical Physics, Bind 19, Nr. 3, 2017, s. 2017-2024.Publikation: Bidrag til tidsskrift › Tidsskriftartikel › Forskning › fagfællebedømt
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TY - JOUR
T1 - Modeling the active sites of Co-promoted MoS2 particles by DFT
AU - Šarić, Manuel
AU - Rossmeisl, Jan
AU - Moses, Poul Georg
PY - 2017
Y1 - 2017
N2 - The atomic-scale structure of the Co-promoted MoS2 catalyst (CoMoS), used for hydrodesulfurization and as a potential replacement for platinum in the acidic hydrogen evolution reaction has been analyzed by modeling its sites using density functional theory and applying thermochemical corrections to account for different reaction conditions. The equilibrium structures of the edges, basal plane and corners have been found and used to obtain a picture of an ideal CoMoS nanoparticle under hydrodesulfurization and hydrogen evolution reaction conditions. Under hydrodesulfurization conditions small energy differences between structures having an additional or missing sulfur atom relative to the equilibrium structures have been observed for the edges and corners explaining their activity towards hydrodesulfurization at the atomic scale. The lack of these small energy differences at the basal plane explains why it is inert towards hydrodesulfurization. The adsorption free energy of hydrogen was calculated and used as a descriptor for qualifying each site in the context of hydrogen evolution, finding that the corner site should perform better than the edges.
AB - The atomic-scale structure of the Co-promoted MoS2 catalyst (CoMoS), used for hydrodesulfurization and as a potential replacement for platinum in the acidic hydrogen evolution reaction has been analyzed by modeling its sites using density functional theory and applying thermochemical corrections to account for different reaction conditions. The equilibrium structures of the edges, basal plane and corners have been found and used to obtain a picture of an ideal CoMoS nanoparticle under hydrodesulfurization and hydrogen evolution reaction conditions. Under hydrodesulfurization conditions small energy differences between structures having an additional or missing sulfur atom relative to the equilibrium structures have been observed for the edges and corners explaining their activity towards hydrodesulfurization at the atomic scale. The lack of these small energy differences at the basal plane explains why it is inert towards hydrodesulfurization. The adsorption free energy of hydrogen was calculated and used as a descriptor for qualifying each site in the context of hydrogen evolution, finding that the corner site should perform better than the edges.
U2 - 10.1039/c6cp06881b
DO - 10.1039/c6cp06881b
M3 - Journal article
C2 - 28009026
AN - SCOPUS:85009874483
VL - 19
SP - 2017
EP - 2024
JO - Physical Chemistry Chemical Physics
JF - Physical Chemistry Chemical Physics
SN - 1463-9076
IS - 3
ER -
ID: 176609785