Reaction kinetic behaviour with relation to crystallite/grain size dependency in the Mg-Si-H system

© 2015 Acta Materialia Inc. Published by Elsevier Ltd. All rights reserved. An empirical understanding of the relationship between crystallite size and reaction kinetics for the dehydrogenation of MgH<inf>2</inf> in the presence of Si was determined. MgH<inf&gt...

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Main Authors: Chaudhary, A., Sheppard, Drew, Paskevicius, M., Pistidda, C., Dornheim, M., Buckley, Craig
Format: Journal Article
Published: Elsevier Ltd 2015
Online Access:http://hdl.handle.net/20.500.11937/12557
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author Chaudhary, A.
Sheppard, Drew
Paskevicius, M.
Pistidda, C.
Dornheim, M.
Buckley, Craig
author_facet Chaudhary, A.
Sheppard, Drew
Paskevicius, M.
Pistidda, C.
Dornheim, M.
Buckley, Craig
author_sort Chaudhary, A.
building Curtin Institutional Repository
collection Online Access
description © 2015 Acta Materialia Inc. Published by Elsevier Ltd. All rights reserved. An empirical understanding of the relationship between crystallite size and reaction kinetics for the dehydrogenation of MgH<inf>2</inf> in the presence of Si was determined. MgH<inf>2</inf> was combined with Si under different conditions to obtain varying crystallite sizes of both reactants. Thermal analysis and isothermal desorption were undertaken to obtain reaction kinetic information and therefore determine activation energies as well as the rate limiting step for each of the different crystallite sizes. It was found that there is a strong correlation between crystallite size and activation energy for the growth of the Mg<inf>2</inf>Si phase, however, any correlation between the nucleation (of Mg<inf>2</inf>Si) activation energy was less evident. Direct measurements of kinetic behaviour from a manometric Sieverts apparatus showed that initial reaction kinetics were fastest when MgH<inf>2</inf> was mixed with Si nanoparticles, however, this sample was not able to fully desorb. Data from the Sieverts measurements were then used with well-known theoretical models to determine the rate limiting step of the reaction. The three dimensional Carter-Valensi (or contracting volume) diffusion model could be used to describe the rate limiting step for most of the reactions. These results have led to a proposed mechanism for the formation of Mg<inf>2</inf>Si during the decomposition reaction.
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spelling curtin-20.500.11937-125572017-09-13T14:59:52Z Reaction kinetic behaviour with relation to crystallite/grain size dependency in the Mg-Si-H system Chaudhary, A. Sheppard, Drew Paskevicius, M. Pistidda, C. Dornheim, M. Buckley, Craig © 2015 Acta Materialia Inc. Published by Elsevier Ltd. All rights reserved. An empirical understanding of the relationship between crystallite size and reaction kinetics for the dehydrogenation of MgH<inf>2</inf> in the presence of Si was determined. MgH<inf>2</inf> was combined with Si under different conditions to obtain varying crystallite sizes of both reactants. Thermal analysis and isothermal desorption were undertaken to obtain reaction kinetic information and therefore determine activation energies as well as the rate limiting step for each of the different crystallite sizes. It was found that there is a strong correlation between crystallite size and activation energy for the growth of the Mg<inf>2</inf>Si phase, however, any correlation between the nucleation (of Mg<inf>2</inf>Si) activation energy was less evident. Direct measurements of kinetic behaviour from a manometric Sieverts apparatus showed that initial reaction kinetics were fastest when MgH<inf>2</inf> was mixed with Si nanoparticles, however, this sample was not able to fully desorb. Data from the Sieverts measurements were then used with well-known theoretical models to determine the rate limiting step of the reaction. The three dimensional Carter-Valensi (or contracting volume) diffusion model could be used to describe the rate limiting step for most of the reactions. These results have led to a proposed mechanism for the formation of Mg<inf>2</inf>Si during the decomposition reaction. 2015 Journal Article http://hdl.handle.net/20.500.11937/12557 10.1016/j.actamat.2015.05.046 Elsevier Ltd restricted
spellingShingle Chaudhary, A.
Sheppard, Drew
Paskevicius, M.
Pistidda, C.
Dornheim, M.
Buckley, Craig
Reaction kinetic behaviour with relation to crystallite/grain size dependency in the Mg-Si-H system
title Reaction kinetic behaviour with relation to crystallite/grain size dependency in the Mg-Si-H system
title_full Reaction kinetic behaviour with relation to crystallite/grain size dependency in the Mg-Si-H system
title_fullStr Reaction kinetic behaviour with relation to crystallite/grain size dependency in the Mg-Si-H system
title_full_unstemmed Reaction kinetic behaviour with relation to crystallite/grain size dependency in the Mg-Si-H system
title_short Reaction kinetic behaviour with relation to crystallite/grain size dependency in the Mg-Si-H system
title_sort reaction kinetic behaviour with relation to crystallite/grain size dependency in the mg-si-h system
url http://hdl.handle.net/20.500.11937/12557