Combined computational and experimental investigation of high temperature thermodynamics and structure of cubic ZrO2 and HfO2

Abstract Structure and thermodynamics of pure cubic ZrO2 and HfO2 were studied computationally and experimentally from their tetragonal to cubic transition temperatures (2311 and 2530 °C) to their melting points (2710 and 2800 °C). Computations were performed using automated ab initio molecular dyna...

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Autores principales:	Qi-Jun Hong, Sergey V. Ushakov, Denys Kapush, Chris J. Benmore, Richard J. K. Weber, Axel van de Walle, Alexandra Navrotsky
Formato:	article
Lenguaje:	EN
Publicado:	Nature Portfolio 2018
Materias:	Hafnium Fusion Enthalpy Volumetric Thermal Expansion Aerodynamic Levitation Pure ZrO2 Medicine R Science Q
Acceso en línea:	https://doaj.org/article/994cd5f41e9b43cbb2500fb8d7e945e6
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id	oai:doaj.org-article:994cd5f41e9b43cbb2500fb8d7e945e6
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spelling	oai:doaj.org-article:994cd5f41e9b43cbb2500fb8d7e945e62021-12-02T15:09:07ZCombined computational and experimental investigation of high temperature thermodynamics and structure of cubic ZrO2 and HfO210.1038/s41598-018-32848-72045-2322https://doaj.org/article/994cd5f41e9b43cbb2500fb8d7e945e62018-10-01T00:00:00Zhttps://doi.org/10.1038/s41598-018-32848-7https://doaj.org/toc/2045-2322Abstract Structure and thermodynamics of pure cubic ZrO2 and HfO2 were studied computationally and experimentally from their tetragonal to cubic transition temperatures (2311 and 2530 °C) to their melting points (2710 and 2800 °C). Computations were performed using automated ab initio molecular dynamics techniques. High temperature synchrotron X-ray diffraction on laser heated aerodynamically levitated samples provided experimental data on volume change during tetragonal-to-cubic phase transformation (0.55 ± 0.09% for ZrO2 and 0.87 ± 0.08% for HfO2), density and thermal expansion. Fusion enthalpies were measured using drop and catch calorimetry on laser heated levitated samples as 55 ± 7 kJ/mol for ZrO2 and 61 ± 10 kJ/mol for HfO2, compared with 54 ± 2 and 52 ± 2 kJ/mol from computation. Volumetric thermal expansion for cubic ZrO2 and HfO2 are similar and reach (4 ± 1)·10−5/K from experiment and (5 ± 1)·10−5/K from computation. An agreement with experiment renders confidence in values obtained exclusively from computation: namely heat capacity of cubic HfO2 and ZrO2, volume change on melting, and thermal expansion of the liquid to 3127 °C. Computed oxygen diffusion coefficients indicate that above 2400 °C pure ZrO2 is an excellent oxygen conductor, perhaps even better than YSZ.Qi-Jun HongSergey V. UshakovDenys KapushChris J. BenmoreRichard J. K. WeberAxel van de WalleAlexandra NavrotskyNature PortfolioarticleHafniumFusion EnthalpyVolumetric Thermal ExpansionAerodynamic LevitationPure ZrO2MedicineRScienceQENScientific Reports, Vol 8, Iss 1, Pp 1-11 (2018)
institution	DOAJ
collection	DOAJ
language	EN
topic	Hafnium Fusion Enthalpy Volumetric Thermal Expansion Aerodynamic Levitation Pure ZrO2 Medicine R Science Q
spellingShingle	Hafnium Fusion Enthalpy Volumetric Thermal Expansion Aerodynamic Levitation Pure ZrO2 Medicine R Science Q Qi-Jun Hong Sergey V. Ushakov Denys Kapush Chris J. Benmore Richard J. K. Weber Axel van de Walle Alexandra Navrotsky Combined computational and experimental investigation of high temperature thermodynamics and structure of cubic ZrO2 and HfO2
description	Abstract Structure and thermodynamics of pure cubic ZrO2 and HfO2 were studied computationally and experimentally from their tetragonal to cubic transition temperatures (2311 and 2530 °C) to their melting points (2710 and 2800 °C). Computations were performed using automated ab initio molecular dynamics techniques. High temperature synchrotron X-ray diffraction on laser heated aerodynamically levitated samples provided experimental data on volume change during tetragonal-to-cubic phase transformation (0.55 ± 0.09% for ZrO2 and 0.87 ± 0.08% for HfO2), density and thermal expansion. Fusion enthalpies were measured using drop and catch calorimetry on laser heated levitated samples as 55 ± 7 kJ/mol for ZrO2 and 61 ± 10 kJ/mol for HfO2, compared with 54 ± 2 and 52 ± 2 kJ/mol from computation. Volumetric thermal expansion for cubic ZrO2 and HfO2 are similar and reach (4 ± 1)·10−5/K from experiment and (5 ± 1)·10−5/K from computation. An agreement with experiment renders confidence in values obtained exclusively from computation: namely heat capacity of cubic HfO2 and ZrO2, volume change on melting, and thermal expansion of the liquid to 3127 °C. Computed oxygen diffusion coefficients indicate that above 2400 °C pure ZrO2 is an excellent oxygen conductor, perhaps even better than YSZ.
format	article
author	Qi-Jun Hong Sergey V. Ushakov Denys Kapush Chris J. Benmore Richard J. K. Weber Axel van de Walle Alexandra Navrotsky
author_facet	Qi-Jun Hong Sergey V. Ushakov Denys Kapush Chris J. Benmore Richard J. K. Weber Axel van de Walle Alexandra Navrotsky
author_sort	Qi-Jun Hong
title	Combined computational and experimental investigation of high temperature thermodynamics and structure of cubic ZrO2 and HfO2
title_short	Combined computational and experimental investigation of high temperature thermodynamics and structure of cubic ZrO2 and HfO2
title_full	Combined computational and experimental investigation of high temperature thermodynamics and structure of cubic ZrO2 and HfO2
title_fullStr	Combined computational and experimental investigation of high temperature thermodynamics and structure of cubic ZrO2 and HfO2
title_full_unstemmed	Combined computational and experimental investigation of high temperature thermodynamics and structure of cubic ZrO2 and HfO2
title_sort	combined computational and experimental investigation of high temperature thermodynamics and structure of cubic zro2 and hfo2
publisher	Nature Portfolio
publishDate	2018
url	https://doaj.org/article/994cd5f41e9b43cbb2500fb8d7e945e6
work_keys_str_mv	AT qijunhong combinedcomputationalandexperimentalinvestigationofhightemperaturethermodynamicsandstructureofcubiczro2andhfo2 AT sergeyvushakov combinedcomputationalandexperimentalinvestigationofhightemperaturethermodynamicsandstructureofcubiczro2andhfo2 AT denyskapush combinedcomputationalandexperimentalinvestigationofhightemperaturethermodynamicsandstructureofcubiczro2andhfo2 AT chrisjbenmore combinedcomputationalandexperimentalinvestigationofhightemperaturethermodynamicsandstructureofcubiczro2andhfo2 AT richardjkweber combinedcomputationalandexperimentalinvestigationofhightemperaturethermodynamicsandstructureofcubiczro2andhfo2 AT axelvandewalle combinedcomputationalandexperimentalinvestigationofhightemperaturethermodynamicsandstructureofcubiczro2andhfo2 AT alexandranavrotsky combinedcomputationalandexperimentalinvestigationofhightemperaturethermodynamicsandstructureofcubiczro2andhfo2
_version_	1718387890630688768

Combined computational and experimental investigation of high temperature thermodynamics and structure of cubic ZrO2 and HfO2

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