An experimentally validated numerical model of interface advance of the lithium sulfate monohydrate dehydration reaction

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Abstract

Interface advance plays an essential role in understanding the kinetics and mechanisms of thermal decomposition reactions such as the dehydration reaction of lithium sulfate monocrystals. However, many fundamental processes including mass transfer during interface advance are still not clear. In this work, the dynamics of interface advance, involving interaction between interfacial reaction and mass diffusion, is investigated numerically together with microscopy observations. A mathematical model is developed for interface advance with a moving boundary and then solved by using a conservative scheme. To examine the significance between the intrinsic chemical reaction and mass diffusion, a Damköhler number is defined as Da=krL/(Dec0)Da=krL/(Dec0) . Numerical results at various Da values are discussed to distinguish the limiting step of the dehydration reaction of lithium sulfate monocrystals. Moreover, experiments are carried out with a hot-stage microscopy system where the propagation of the reaction interface into the crystal bulk is followed in situ. By fitting the experimental results with the numerical results, the effective diffusivity of water through the dehydrated crystal is estimated to be in the order of 10−8m2s−110−8m2s−1 . According to the corresponding Da values, it is found that, within the reaction temperature ranging from 110 to 130 °C and a partial water vapor pressure of 13 mbar, the rate of dehydration interface advance in the bulk of large crystals (typically in the order of millimeters) is not constant, but shows a small decrease over time due to the influence of mass diffusion.
Original languageEnglish
Pages (from-to)1109-1118
JournalJournal of Thermal Analysis and Calorimetry
Volume124
Issue number2
DOIs
Publication statusPublished - Jan 2016

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lithium sulfates
Dehydration
dehydration
Numerical models
Crystals
Microscopic examination
Steam
Surface chemistry
Vapor pressure
microscopy
crystals
Chemical reactions
Pyrolysis
water pressure
Mass transfer
single crystals
Mathematical models
vapor pressure
Kinetics
mass transfer

Cite this

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title = "An experimentally validated numerical model of interface advance of the lithium sulfate monohydrate dehydration reaction",
abstract = "Interface advance plays an essential role in understanding the kinetics and mechanisms of thermal decomposition reactions such as the dehydration reaction of lithium sulfate monocrystals. However, many fundamental processes including mass transfer during interface advance are still not clear. In this work, the dynamics of interface advance, involving interaction between interfacial reaction and mass diffusion, is investigated numerically together with microscopy observations. A mathematical model is developed for interface advance with a moving boundary and then solved by using a conservative scheme. To examine the significance between the intrinsic chemical reaction and mass diffusion, a Damk{\"o}hler number is defined as Da=krL/(Dec0)Da=krL/(Dec0) . Numerical results at various Da values are discussed to distinguish the limiting step of the dehydration reaction of lithium sulfate monocrystals. Moreover, experiments are carried out with a hot-stage microscopy system where the propagation of the reaction interface into the crystal bulk is followed in situ. By fitting the experimental results with the numerical results, the effective diffusivity of water through the dehydrated crystal is estimated to be in the order of 10−8m2s−110−8m2s−1 . According to the corresponding Da values, it is found that, within the reaction temperature ranging from 110 to 130 °C and a partial water vapor pressure of 13 mbar, the rate of dehydration interface advance in the bulk of large crystals (typically in the order of millimeters) is not constant, but shows a small decrease over time due to the influence of mass diffusion.",
author = "S. Lan and H.A. Zondag and {van Steenhoven}, A.A. and C.C.M. Rindt",
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T1 - An experimentally validated numerical model of interface advance of the lithium sulfate monohydrate dehydration reaction

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AU - Zondag, H.A.

AU - van Steenhoven, A.A.

AU - Rindt, C.C.M.

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N2 - Interface advance plays an essential role in understanding the kinetics and mechanisms of thermal decomposition reactions such as the dehydration reaction of lithium sulfate monocrystals. However, many fundamental processes including mass transfer during interface advance are still not clear. In this work, the dynamics of interface advance, involving interaction between interfacial reaction and mass diffusion, is investigated numerically together with microscopy observations. A mathematical model is developed for interface advance with a moving boundary and then solved by using a conservative scheme. To examine the significance between the intrinsic chemical reaction and mass diffusion, a Damköhler number is defined as Da=krL/(Dec0)Da=krL/(Dec0) . Numerical results at various Da values are discussed to distinguish the limiting step of the dehydration reaction of lithium sulfate monocrystals. Moreover, experiments are carried out with a hot-stage microscopy system where the propagation of the reaction interface into the crystal bulk is followed in situ. By fitting the experimental results with the numerical results, the effective diffusivity of water through the dehydrated crystal is estimated to be in the order of 10−8m2s−110−8m2s−1 . According to the corresponding Da values, it is found that, within the reaction temperature ranging from 110 to 130 °C and a partial water vapor pressure of 13 mbar, the rate of dehydration interface advance in the bulk of large crystals (typically in the order of millimeters) is not constant, but shows a small decrease over time due to the influence of mass diffusion.

AB - Interface advance plays an essential role in understanding the kinetics and mechanisms of thermal decomposition reactions such as the dehydration reaction of lithium sulfate monocrystals. However, many fundamental processes including mass transfer during interface advance are still not clear. In this work, the dynamics of interface advance, involving interaction between interfacial reaction and mass diffusion, is investigated numerically together with microscopy observations. A mathematical model is developed for interface advance with a moving boundary and then solved by using a conservative scheme. To examine the significance between the intrinsic chemical reaction and mass diffusion, a Damköhler number is defined as Da=krL/(Dec0)Da=krL/(Dec0) . Numerical results at various Da values are discussed to distinguish the limiting step of the dehydration reaction of lithium sulfate monocrystals. Moreover, experiments are carried out with a hot-stage microscopy system where the propagation of the reaction interface into the crystal bulk is followed in situ. By fitting the experimental results with the numerical results, the effective diffusivity of water through the dehydrated crystal is estimated to be in the order of 10−8m2s−110−8m2s−1 . According to the corresponding Da values, it is found that, within the reaction temperature ranging from 110 to 130 °C and a partial water vapor pressure of 13 mbar, the rate of dehydration interface advance in the bulk of large crystals (typically in the order of millimeters) is not constant, but shows a small decrease over time due to the influence of mass diffusion.

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