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

Research output: Contribution to journal › Article › peer-review

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.

Original language	English
Pages (from-to)	368-379
Number of pages	12
Journal	Catalysis Today
Volume	357
Early online date	9 Dec 2020
DOIs	https://doi.org/10.1016/j.cattod.2019.11.018
Publication status	Published - 2020

Keywords

Pd
Al2O3
CH4
Oxidation
Periodic DFT
Heterogeneous catalysis
СН4

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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",

}

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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

UR - http://www.scopus.com/inward/record.url?scp=85076833191&partnerID=8YFLogxK

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

Abstract

Keywords

Access to Document

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CÉCI – Consortium of high performance computing centers

Functional Supramolecular Systems (PAI P6/27)

High Performance Computing Technology Platform

Cite this

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

Keywords

Access to Document

Other files and links

Fingerprint

Projects

CÉCI – Consortium of high performance computing centers

Functional Supramolecular Systems (PAI P6/27)

Equipment

High Performance Computing Technology Platform

Cite this

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