Reduction and oxidation kinetics of Co-Ni/Al2O3 oxygen carrier involved in a chemical-looping combustion cycles

Mohammad M. Hossain; Hugo I. de Lasa

doi:10.1016/j.ces.2009.01.059

Reduction and oxidation kinetics of Co-Ni/Al₂O₃ oxygen carrier involved in a chemical-looping combustion cycles

Mohammad M. Hossain, Hugo I. de Lasa^*

^*Corresponding author for this work

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

118 Scopus citations

Abstract

The solid-state kinetics of Co-Ni/Al₂O₃ oxygen carrier is studied using non-isothermal reaction data and a non-linear regression analysis. XRD analysis of the fresh samples shows that NiO is the dominant reducible phase of the oxygen carrier. Pulse chemisorption suggests a negligible nuclei growth over the repeated reduction/oxidation cycles. Mercury porosimetry confirms that the pore size of the carrier particle is slightly increased following reduction. A nucleation and nuclei growth model and an unreacted shrinking-core model are developed based on the oxygen carrier texture change during reduction/oxidation, as observed by pulse chemisorption and mercury porosimetry. Model parameters are calculated using H₂-TPR and O₂-TPO data. It is found that the random nucleation model describes solid phase changes adequately. The determined apparent activation energies are 45 and 44 kJ/mol for the reduction and oxidation, respectively. The established kinetic model is successfully evaluated for the reduction cycle using a CREC mini-fluidized Riser Simulator reactor operating under expected conditions of large industrial scale fluidized CLC units.

Original language	English
Pages (from-to)	98-106
Number of pages	9
Journal	Chemical Engineering Science
Volume	65
Issue number	1
DOIs	https://doi.org/10.1016/j.ces.2009.01.059
State	Published - 2010
Externally published	Yes

Bibliographical note

Funding Information:
M.M.H. wishes to acknowledge the Natural Sciences and Engineering Research Council of Canada (NSERC) for Canada Graduate Scholarship for Doctoral study (CGS-D) and The University of Western Ontario for President's Scholarship for Graduate Study (PSGS). The authors also like to thank NSERC for their financial support to this project.

Keywords

CLC
CO capture
Gas-solid reaction kinetics
Nucleation and nuclei growth model
Shrinking-core model

ASJC Scopus subject areas

General Chemistry
General Chemical Engineering
Industrial and Manufacturing Engineering

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

Access to Document

10.1016/j.ces.2009.01.059

Cite this

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title = "Reduction and oxidation kinetics of Co-Ni/Al2O3 oxygen carrier involved in a chemical-looping combustion cycles",

abstract = "The solid-state kinetics of Co-Ni/Al2O3 oxygen carrier is studied using non-isothermal reaction data and a non-linear regression analysis. XRD analysis of the fresh samples shows that NiO is the dominant reducible phase of the oxygen carrier. Pulse chemisorption suggests a negligible nuclei growth over the repeated reduction/oxidation cycles. Mercury porosimetry confirms that the pore size of the carrier particle is slightly increased following reduction. A nucleation and nuclei growth model and an unreacted shrinking-core model are developed based on the oxygen carrier texture change during reduction/oxidation, as observed by pulse chemisorption and mercury porosimetry. Model parameters are calculated using H2-TPR and O2-TPO data. It is found that the random nucleation model describes solid phase changes adequately. The determined apparent activation energies are 45 and 44 kJ/mol for the reduction and oxidation, respectively. The established kinetic model is successfully evaluated for the reduction cycle using a CREC mini-fluidized Riser Simulator reactor operating under expected conditions of large industrial scale fluidized CLC units.",

keywords = "CLC, CO capture, Gas-solid reaction kinetics, Nucleation and nuclei growth model, Shrinking-core model",

author = "Hossain, \{Mohammad M.\} and \{de Lasa\}, \{Hugo I.\}",

note = "Funding Information: M.M.H. wishes to acknowledge the Natural Sciences and Engineering Research Council of Canada (NSERC) for Canada Graduate Scholarship for Doctoral study (CGS-D) and The University of Western Ontario for President's Scholarship for Graduate Study (PSGS). The authors also like to thank NSERC for their financial support to this project. ",

year = "2010",

doi = "10.1016/j.ces.2009.01.059",

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pages = "98--106",

journal = "Chemical Engineering Science",

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AU - Hossain, Mohammad M.

AU - de Lasa, Hugo I.

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PY - 2010

Y1 - 2010

N2 - The solid-state kinetics of Co-Ni/Al2O3 oxygen carrier is studied using non-isothermal reaction data and a non-linear regression analysis. XRD analysis of the fresh samples shows that NiO is the dominant reducible phase of the oxygen carrier. Pulse chemisorption suggests a negligible nuclei growth over the repeated reduction/oxidation cycles. Mercury porosimetry confirms that the pore size of the carrier particle is slightly increased following reduction. A nucleation and nuclei growth model and an unreacted shrinking-core model are developed based on the oxygen carrier texture change during reduction/oxidation, as observed by pulse chemisorption and mercury porosimetry. Model parameters are calculated using H2-TPR and O2-TPO data. It is found that the random nucleation model describes solid phase changes adequately. The determined apparent activation energies are 45 and 44 kJ/mol for the reduction and oxidation, respectively. The established kinetic model is successfully evaluated for the reduction cycle using a CREC mini-fluidized Riser Simulator reactor operating under expected conditions of large industrial scale fluidized CLC units.

AB - The solid-state kinetics of Co-Ni/Al2O3 oxygen carrier is studied using non-isothermal reaction data and a non-linear regression analysis. XRD analysis of the fresh samples shows that NiO is the dominant reducible phase of the oxygen carrier. Pulse chemisorption suggests a negligible nuclei growth over the repeated reduction/oxidation cycles. Mercury porosimetry confirms that the pore size of the carrier particle is slightly increased following reduction. A nucleation and nuclei growth model and an unreacted shrinking-core model are developed based on the oxygen carrier texture change during reduction/oxidation, as observed by pulse chemisorption and mercury porosimetry. Model parameters are calculated using H2-TPR and O2-TPO data. It is found that the random nucleation model describes solid phase changes adequately. The determined apparent activation energies are 45 and 44 kJ/mol for the reduction and oxidation, respectively. The established kinetic model is successfully evaluated for the reduction cycle using a CREC mini-fluidized Riser Simulator reactor operating under expected conditions of large industrial scale fluidized CLC units.

KW - CLC

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KW - Nucleation and nuclei growth model

KW - Shrinking-core model

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