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Inverse temperature hysteresis and self-sustained oscillations in CO oxidation over Pd at elevated pressures of reaction mixture : Experiment and mathematical modeling. / Lashina, E. A.; Slavinskaya, E. M.; Chumakova, N. A. и др.

в: Chemical Engineering Science, Том 212, 115312, 02.02.2020.

Результаты исследований: Научные публикации в периодических изданияхстатьяРецензирование

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@article{9274529059a244849a76a2ba61799cc4,
title = "Inverse temperature hysteresis and self-sustained oscillations in CO oxidation over Pd at elevated pressures of reaction mixture: Experiment and mathematical modeling",
abstract = "Studying the kinetics of CO oxidation over Pd foil at elevated CO and O2 pressures, we observed an inverse hysteresis: CO conversion was much lower under sample cooling than under foil heating. It was established that under heating the oxidation of metallic palladium to bulk palladium oxide occurred through formation of the palladium surface oxide. Under cooling the bulk oxide reduced directly to metallic species, and in this case some self-sustained oscillations of reaction rate were observed. The catalytic scheme including main various oxygen states of the palladium surface and bulk with transitions between them under reaction conditions in heating/cooling catalytic cycle was proposed. On the base of this scheme the kinetic model of CO oxidation reaction was developed. Both most important mechanisms: Langmuir - Hinshelwood and Mars - van Krevelen, were involved for description of the observed kinetic nonlinear phenomena. The performed simulations demonstrated the capability of this model to describe well the inverse hysteresis of CO oxidation rate together with its oscillatory behavior at constant temperature within the hysteresis loop.",
keywords = "Inverse hysteresis, Isothermal lumped model, Phase transition, Self-sustained oscillations, Surface oxide, KINETIC OSCILLATIONS, SURFACE-STRUCTURE, METHANE OXIDATION, RANGE 1-150 TORR, SINGLE-CRYSTALS, CATALYTIC-PROPERTIES, SUBSURFACE OXYGEN, CARBON-MONOXIDE OXIDATION, PALLADIUM OXIDATION, PD/AL2O3 CATALYSTS",
author = "Lashina, {E. A.} and Slavinskaya, {E. M.} and Chumakova, {N. A.} and Stadnichenko, {A. I.} and Salanov, {A. N.} and Chumakov, {G. A.} and Boronin, {A. I.}",
year = "2020",
month = feb,
day = "2",
doi = "10.1016/j.ces.2019.115312",
language = "English",
volume = "212",
journal = "Chemical Engineering Science",
issn = "0009-2509",
publisher = "Elsevier",

}

RIS

TY - JOUR

T1 - Inverse temperature hysteresis and self-sustained oscillations in CO oxidation over Pd at elevated pressures of reaction mixture

T2 - Experiment and mathematical modeling

AU - Lashina, E. A.

AU - Slavinskaya, E. M.

AU - Chumakova, N. A.

AU - Stadnichenko, A. I.

AU - Salanov, A. N.

AU - Chumakov, G. A.

AU - Boronin, A. I.

PY - 2020/2/2

Y1 - 2020/2/2

N2 - Studying the kinetics of CO oxidation over Pd foil at elevated CO and O2 pressures, we observed an inverse hysteresis: CO conversion was much lower under sample cooling than under foil heating. It was established that under heating the oxidation of metallic palladium to bulk palladium oxide occurred through formation of the palladium surface oxide. Under cooling the bulk oxide reduced directly to metallic species, and in this case some self-sustained oscillations of reaction rate were observed. The catalytic scheme including main various oxygen states of the palladium surface and bulk with transitions between them under reaction conditions in heating/cooling catalytic cycle was proposed. On the base of this scheme the kinetic model of CO oxidation reaction was developed. Both most important mechanisms: Langmuir - Hinshelwood and Mars - van Krevelen, were involved for description of the observed kinetic nonlinear phenomena. The performed simulations demonstrated the capability of this model to describe well the inverse hysteresis of CO oxidation rate together with its oscillatory behavior at constant temperature within the hysteresis loop.

AB - Studying the kinetics of CO oxidation over Pd foil at elevated CO and O2 pressures, we observed an inverse hysteresis: CO conversion was much lower under sample cooling than under foil heating. It was established that under heating the oxidation of metallic palladium to bulk palladium oxide occurred through formation of the palladium surface oxide. Under cooling the bulk oxide reduced directly to metallic species, and in this case some self-sustained oscillations of reaction rate were observed. The catalytic scheme including main various oxygen states of the palladium surface and bulk with transitions between them under reaction conditions in heating/cooling catalytic cycle was proposed. On the base of this scheme the kinetic model of CO oxidation reaction was developed. Both most important mechanisms: Langmuir - Hinshelwood and Mars - van Krevelen, were involved for description of the observed kinetic nonlinear phenomena. The performed simulations demonstrated the capability of this model to describe well the inverse hysteresis of CO oxidation rate together with its oscillatory behavior at constant temperature within the hysteresis loop.

KW - Inverse hysteresis

KW - Isothermal lumped model

KW - Phase transition

KW - Self-sustained oscillations

KW - Surface oxide

KW - KINETIC OSCILLATIONS

KW - SURFACE-STRUCTURE

KW - METHANE OXIDATION

KW - RANGE 1-150 TORR

KW - SINGLE-CRYSTALS

KW - CATALYTIC-PROPERTIES

KW - SUBSURFACE OXYGEN

KW - CARBON-MONOXIDE OXIDATION

KW - PALLADIUM OXIDATION

KW - PD/AL2O3 CATALYSTS

UR - http://www.scopus.com/inward/record.url?scp=85074760620&partnerID=8YFLogxK

U2 - 10.1016/j.ces.2019.115312

DO - 10.1016/j.ces.2019.115312

M3 - Article

AN - SCOPUS:85074760620

VL - 212

JO - Chemical Engineering Science

JF - Chemical Engineering Science

SN - 0009-2509

M1 - 115312

ER -

ID: 22321423