Microkinetic evaluation of normal and inverse kinetic isotope effects during methane steam reforming to synthesis gas over a Ni/NiAl2O4 model catalyst

C. Sprung; P.N. Kechagiopoulos; J.W. Thybaut; B. Arstad; U. Olsbye; G.B. Marin

doi:10.1016/j.apcata.2014.10.062

Microkinetic evaluation of normal and inverse kinetic isotope effects during methane steam reforming to synthesis gas over a Ni/NiAl2O4 model catalyst

C. Sprung, P.N. Kechagiopoulos, J.W. Thybaut, B. Arstad, U. Olsbye, G.B. Marin

Engineering

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24 Citations (Scopus)

Abstract

Abstract
A microkinetic model was developed and applied to simulate an extensive experimental dataset on methane steam reforming. The data set consisted of 537 data points, and was collected over a Ni/NiAl2O4 catalyst at 843, 858, and 873 K in a wide steam-to-carbon ratio range between 0.2 and 7.1. A microkinetic engine modeling tool was applied for the construction and parameter estimation of an elementary step network consisting of 12 reversible reactions. Specific reaction pathways were implemented for the formation of CO and CO2, respectively. The model qualitatively if not quantitatively explains inverse and normal isotope effects experimentally observed at low and high S/C ratios, respectively, and is thermodynamically consistent. A combination of the approach to partial equilibrium (i.e. whether the elementary step proceeds forward or backward) and net rate (i.e. the difference between forward and backward reaction rate) provides novel insight into the oxidation mechanism of CHx and CHxO surface species.

Original language	English
Pages (from-to)	231-242
Number of pages	12
Journal	Applied Catalysis A: General
Volume	492
Early online date	23 Dec 2014
DOIs	https://doi.org/10.1016/j.apcata.2014.10.062
Publication status	Published - 25 Feb 2015

Bibliographical note

Acknowledgements
The Norwegian Research Council, through the RENERGI project “Hydrogen production by Sorbent Enhanced Reforming”, P 178129/S30, is acknowledged for financial support. This paper reports work undertaken in the context ofthe project
OCMOL, Oxidative Coupling of Methane followed by Oligomerization to Liquids. OCMOL is a Large Scale Collaborative Project supported by the European Commission in the 7th Framework Programme (GA no. 228953). For further information about OCMOL see: http://www.ocmol.eu or http://www.ocmol.com.

Keywords

microkinetic modelling
methane steam reforming
kinetic isotope effect
reaction pathway
partial equilibrium

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Panagiotis Kechagiopoulos
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title = "Microkinetic evaluation of normal and inverse kinetic isotope effects during methane steam reforming to synthesis gas over a Ni/NiAl2O4 model catalyst",

abstract = "Abstract A microkinetic model was developed and applied to simulate an extensive experimental dataset on methane steam reforming. The data set consisted of 537 data points, and was collected over a Ni/NiAl2O4 catalyst at 843, 858, and 873 K in a wide steam-to-carbon ratio range between 0.2 and 7.1. A microkinetic engine modeling tool was applied for the construction and parameter estimation of an elementary step network consisting of 12 reversible reactions. Specific reaction pathways were implemented for the formation of CO and CO2, respectively. The model qualitatively if not quantitatively explains inverse and normal isotope effects experimentally observed at low and high S/C ratios, respectively, and is thermodynamically consistent. A combination of the approach to partial equilibrium (i.e. whether the elementary step proceeds forward or backward) and net rate (i.e. the difference between forward and backward reaction rate) provides novel insight into the oxidation mechanism of CHx and CHxO surface species.",

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note = "Acknowledgements The Norwegian Research Council, through the RENERGI project “Hydrogen production by Sorbent Enhanced Reforming”, P 178129/S30, is acknowledged for financial support. This paper reports work undertaken in the context ofthe project OCMOL, Oxidative Coupling of Methane followed by Oligomerization to Liquids. OCMOL is a Large Scale Collaborative Project supported by the European Commission in the 7th Framework Programme (GA no. 228953). For further information about OCMOL see: http://www.ocmol.eu or http://www.ocmol.com. ",

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AU - Arstad, B.

AU - Olsbye, U.

AU - Marin, G.B.

N1 - Acknowledgements The Norwegian Research Council, through the RENERGI project “Hydrogen production by Sorbent Enhanced Reforming”, P 178129/S30, is acknowledged for financial support. This paper reports work undertaken in the context ofthe project OCMOL, Oxidative Coupling of Methane followed by Oligomerization to Liquids. OCMOL is a Large Scale Collaborative Project supported by the European Commission in the 7th Framework Programme (GA no. 228953). For further information about OCMOL see: http://www.ocmol.eu or http://www.ocmol.com.

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N2 - Abstract A microkinetic model was developed and applied to simulate an extensive experimental dataset on methane steam reforming. The data set consisted of 537 data points, and was collected over a Ni/NiAl2O4 catalyst at 843, 858, and 873 K in a wide steam-to-carbon ratio range between 0.2 and 7.1. A microkinetic engine modeling tool was applied for the construction and parameter estimation of an elementary step network consisting of 12 reversible reactions. Specific reaction pathways were implemented for the formation of CO and CO2, respectively. The model qualitatively if not quantitatively explains inverse and normal isotope effects experimentally observed at low and high S/C ratios, respectively, and is thermodynamically consistent. A combination of the approach to partial equilibrium (i.e. whether the elementary step proceeds forward or backward) and net rate (i.e. the difference between forward and backward reaction rate) provides novel insight into the oxidation mechanism of CHx and CHxO surface species.

AB - Abstract A microkinetic model was developed and applied to simulate an extensive experimental dataset on methane steam reforming. The data set consisted of 537 data points, and was collected over a Ni/NiAl2O4 catalyst at 843, 858, and 873 K in a wide steam-to-carbon ratio range between 0.2 and 7.1. A microkinetic engine modeling tool was applied for the construction and parameter estimation of an elementary step network consisting of 12 reversible reactions. Specific reaction pathways were implemented for the formation of CO and CO2, respectively. The model qualitatively if not quantitatively explains inverse and normal isotope effects experimentally observed at low and high S/C ratios, respectively, and is thermodynamically consistent. A combination of the approach to partial equilibrium (i.e. whether the elementary step proceeds forward or backward) and net rate (i.e. the difference between forward and backward reaction rate) provides novel insight into the oxidation mechanism of CHx and CHxO surface species.

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KW - methane steam reforming

KW - kinetic isotope effect

KW - reaction pathway

KW - partial equilibrium

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DO - 10.1016/j.apcata.2014.10.062

M3 - Article

SN - 0926-860X

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JO - Applied Catalysis A: General

JF - Applied Catalysis A: General

ER -

Microkinetic evaluation of normal and inverse kinetic isotope effects during methane steam reforming to synthesis gas over a Ni/NiAl2O4 model catalyst

Abstract

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Keywords

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