Influence of Oxide Support on Pd Properties: A Gain for O Diffusion versus Minor Impact on CH4 Dissociation: A Gain for O Diffusion versus minor Impact for CH4 Dissociation

Andrey Rybakov; Ilya A. Bryukhanov; Alexander Larin; Silvia Zh. Todorova; Daniel Vercauteren; Georgii ZHIDOMIROV

doi:10.1016/j.cattod.2019.11.018

Influence of Oxide Support on Pd Properties: A Gain for O Diffusion versus Minor Impact on CH4 Dissociation: A Gain for O Diffusion versus minor Impact for CH₄ Dissociation

Andrey Rybakov, Ilya A. Bryukhanov, Alexander Larin, Silvia Zh. Todorova, Daniel Vercauteren, Georgii ZHIDOMIROV

Résultats de recherche: Contribution à un journal/une revue › Article › Revue par des pairs

Résumé

Multi-layer Pd(100)/γ-Al2O3(100) slab models were constructed over a non-defective γ-Al2O3 (100) surface in order to study the Pd oxidation steps including penetration of atomic oxygen from the surface to Pd bulk. The modeling using periodic DFT/PBE revealed that near the surface both chemisorbed O atoms or physisorbed O2 can play a promotive role regarding O diffusion starting from c(2 × 2) model of O adsorption. The calculated activation energies E# for O diffusion from Pd(100) surface approach experimental E# values between the deeper layers while underestimate the rearrangement barriers at the surface. We also calculated the activation energies of CH4 and O2 dissociation considering different Pd-Pd distances in the Pd and oxidized Pd(O*) layers on different types of oxide support shown earlier.

langue originale	Anglais
Pages (de - à)	368-379
Nombre de pages	12
journal	Catalysis Today
Volume	357
Date de mise en ligne précoce	9 déc. 2020
Les DOIs	https://doi.org/10.1016/j.cattod.2019.11.018
Etat de la publication	Publié - 2020

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10.1016/j.cattod.2019.11.018

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@article{a5e5cfdd266a4d98a48925cf1849bfe2,

title = "Influence of Oxide Support on Pd Properties: A Gain for O Diffusion versus Minor Impact on CH4 Dissociation: A Gain for O Diffusion versus minor Impact for CH4 Dissociation",

abstract = "Multi-layer Pd(100)/γ-Al2O3(100) slab models were constructed over a non-defective γ-Al2O3 (100) surface in order to study the Pd oxidation steps including penetration of atomic oxygen from the surface to Pd bulk. The modeling using periodic DFT/PBE revealed that near the surface both chemisorbed O atoms or physisorbed O2 can play a promotive role regarding O diffusion starting from c(2 × 2) model of O adsorption. The calculated activation energies E# for O diffusion from Pd(100) surface approach experimental E# values between the deeper layers while underestimate the rearrangement barriers at the surface. We also calculated the activation energies of CH4 and O2 dissociation considering different Pd-Pd distances in the Pd and oxidized Pd(O*) layers on different types of oxide support shown earlier.",

keywords = "Pd, Al2O3, CH4, Oxidation, Periodic DFT, Heterogeneous catalysis, СН4",

author = "Andrey Rybakov and Bryukhanov, {Ilya A.} and Alexander Larin and Todorova, {Silvia Zh.} and Daniel Vercauteren and Georgii ZHIDOMIROV",

note = "Funding Information: The authors thank the Bulgarian Science Fund for financial support through contracts DNTS/ Russia /01/1 and Russian Foundation for Basic Research within the grant 17-53-18026-Bolg_а. The research is carried out using the equipment of the shared research facilities of HPC computing resources at Lomonosov Moscow State University [ 75 ]. Funding Information: The authors acknowledge the Plateforme Technologique de Calcul Intensif (P.T.C.I.; http://www.ptci.unamur.be ), located at the University of Namur, which is part of the Consortium des Equipements de Calcul Intensif (C.E.C.I., supported by the F.R.S.-FNRS, Belgium ; http://www.ceci-hpc.be ). Funding Information: The authors thank the Bulgarian Science Fund for financial support through contracts DNTS/ Russia /01/1 and Russian Foundation for Basic Research within the grant 17-53-18026-Bolg_?. The research is carried out using the equipment of the shared research facilities of HPC computing resources at Lomonosov Moscow State University [75]. The authors acknowledge the Plateforme Technologique de Calcul Intensif (P.T.C.I.; http://www.ptci.unamur.be), located at the University of Namur, which is part of the Consortium des Equipements de Calcul Intensif (C.E.C.I. supported by the F.R.S.-FNRS, Belgium; http://www.ceci-hpc.be). Publisher Copyright: {\textcopyright} 2019 Elsevier B.V.",

year = "2020",

doi = "10.1016/j.cattod.2019.11.018",

language = "English",

volume = "357",

pages = "368--379",

journal = "Catalysis Today",

issn = "0920-5861",

publisher = "Elsevier",

}

Influence of Oxide Support on Pd Properties: A Gain for O Diffusion versus Minor Impact on CH4 Dissociation: A Gain for O Diffusion versus minor Impact for CH₄ Dissociation. / Rybakov, Andrey; Bryukhanov, Ilya A.; Larin, Alexander et al.
Dans: Catalysis Today, Vol 357, 2020, p. 368-379.

Résultats de recherche: Contribution à un journal/une revue › Article › Revue par des pairs

TY - JOUR

T1 - Influence of Oxide Support on Pd Properties: A Gain for O Diffusion versus Minor Impact on CH4 Dissociation

T2 - A Gain for O Diffusion versus minor Impact for CH4 Dissociation

AU - Rybakov, Andrey

AU - Bryukhanov, Ilya A.

AU - Larin, Alexander

AU - Todorova, Silvia Zh.

AU - Vercauteren, Daniel

AU - ZHIDOMIROV, Georgii

N1 - Funding Information: The authors thank the Bulgarian Science Fund for financial support through contracts DNTS/ Russia /01/1 and Russian Foundation for Basic Research within the grant 17-53-18026-Bolg_а. The research is carried out using the equipment of the shared research facilities of HPC computing resources at Lomonosov Moscow State University [ 75 ]. Funding Information: The authors acknowledge the Plateforme Technologique de Calcul Intensif (P.T.C.I.; http://www.ptci.unamur.be ), located at the University of Namur, which is part of the Consortium des Equipements de Calcul Intensif (C.E.C.I., supported by the F.R.S.-FNRS, Belgium ; http://www.ceci-hpc.be ). Funding Information: The authors thank the Bulgarian Science Fund for financial support through contracts DNTS/ Russia /01/1 and Russian Foundation for Basic Research within the grant 17-53-18026-Bolg_?. The research is carried out using the equipment of the shared research facilities of HPC computing resources at Lomonosov Moscow State University [75]. The authors acknowledge the Plateforme Technologique de Calcul Intensif (P.T.C.I.; http://www.ptci.unamur.be), located at the University of Namur, which is part of the Consortium des Equipements de Calcul Intensif (C.E.C.I. supported by the F.R.S.-FNRS, Belgium; http://www.ceci-hpc.be). Publisher Copyright: © 2019 Elsevier B.V.

PY - 2020

Y1 - 2020

N2 - Multi-layer Pd(100)/γ-Al2O3(100) slab models were constructed over a non-defective γ-Al2O3 (100) surface in order to study the Pd oxidation steps including penetration of atomic oxygen from the surface to Pd bulk. The modeling using periodic DFT/PBE revealed that near the surface both chemisorbed O atoms or physisorbed O2 can play a promotive role regarding O diffusion starting from c(2 × 2) model of O adsorption. The calculated activation energies E# for O diffusion from Pd(100) surface approach experimental E# values between the deeper layers while underestimate the rearrangement barriers at the surface. We also calculated the activation energies of CH4 and O2 dissociation considering different Pd-Pd distances in the Pd and oxidized Pd(O*) layers on different types of oxide support shown earlier.

AB - Multi-layer Pd(100)/γ-Al2O3(100) slab models were constructed over a non-defective γ-Al2O3 (100) surface in order to study the Pd oxidation steps including penetration of atomic oxygen from the surface to Pd bulk. The modeling using periodic DFT/PBE revealed that near the surface both chemisorbed O atoms or physisorbed O2 can play a promotive role regarding O diffusion starting from c(2 × 2) model of O adsorption. The calculated activation energies E# for O diffusion from Pd(100) surface approach experimental E# values between the deeper layers while underestimate the rearrangement barriers at the surface. We also calculated the activation energies of CH4 and O2 dissociation considering different Pd-Pd distances in the Pd and oxidized Pd(O*) layers on different types of oxide support shown earlier.

KW - Pd

KW - Al2O3

KW - CH4

KW - Oxidation

KW - Periodic DFT

KW - Heterogeneous catalysis

KW - СН4

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U2 - 10.1016/j.cattod.2019.11.018

DO - 10.1016/j.cattod.2019.11.018

M3 - Article

SN - 0920-5861

VL - 357

SP - 368

EP - 379

JO - Catalysis Today

JF - Catalysis Today

ER -

Influence of Oxide Support on Pd Properties: A Gain for O Diffusion versus Minor Impact on CH4 Dissociation: A Gain for O Diffusion versus minor Impact for CH4 Dissociation

Résumé

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Projets

CÉCI – Consortium des Équipements de Calcul Intensif

Systèmes supramoléculaires fonctionnels (PAI P6/27)

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Plateforme Technologique Calcul Intensif

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Influence of Oxide Support on Pd Properties: A Gain for O Diffusion versus Minor Impact on CH4 Dissociation: A Gain for O Diffusion versus minor Impact for CH₄ Dissociation