Hydrogenography of MgyNi1-yHx gradient thin films: Interplay between the thermodynamics and kinetics of hydrogenation

R.F.A. Gremaud, C.P. Broedersz, A. Borgschulte, M.J. van Setten, H. Schreuders, M.J. Slaman, B. Dam, R.P. Griessen

Research output: Contribution to JournalArticleAcademicpeer-review

Abstract

We monitor the hydrogenation of PTFE/Pd-capped MgyNi1-yHx gradient thin films using the change in optical transmission as a function of time, temperature and hydrogen pressure, to study the relation between kinetics and thermodynamics of hydrogenation of this multiphase hydride system. The interplay between kinetics and thermodynamics is used to extrapolate the hydrogenation equilibrium pressures via the H-absorption rate. Pressure-optical-transmission-isotherms determined independently at different temperatures provide a cross-check for the equilibrium pressure and the enthalpy of H-absorption. We find that the hydrogenation reaction is destabilized with respect to the Mg2Ni -> Mg2NiH4 reaction for Mg fractions close to the Mg2Ni-Mg eutectic point. From a comparison with calculated enthalpies obtained from density functional theory, we conclude that the experimentally observed destabilization originates from the well-mixed microstructure around the eutectic point. (C) 2009 Acta Materialia Inc. Published by Elsevier Ltd. All rights reserved.
Original languageEnglish
Pages (from-to)658-668
Number of pages11
JournalActa Materialia
Volume58
Issue number2
DOIs
Publication statusPublished - Jan 2010

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