Structure and thermodynamic stability of hydrogen interstitials in BaZrO3 perovskite oxide from density functional calculations

Mårten E. Björketun, Per G. Sundell, Göran Wahnström

Resultado de la investigación: Article

87 Citas (Scopus)

Resumen

Density functional calculations have been used to study the electronic structure, preferred sites in the lattice, formation energies and vibrational frequencies for hydrogen interstitials in different charge states in the cubic phase of perovskite-structured BaZrO3. By combining ab initio results with thermodynamic modeling, defect formation at finite temperature and pressure has been investigated. We demonstrate how the site selectivity and spatial distribution of dopant atoms in the lattice can be affected by changes in the environmental conditions (atomic chemical potentials, oxygen partial pressure and temperature) used during processing of the material. In addition, we have calculated the thermodynamic parameters of the water uptake reaction for an acceptor-doped BaZrO3 crystal in equilibrium with a humid atmosphere. The interaction energies between a protonic defect and the investigated Ga, Gd, In, Nd, Sc, and Y dopants were found to be attractive, and we show that a simple model of defect association may reproduce an experimentally observed trend in the hydration enthalpy.

Idioma originalEnglish
Páginas (desde-hasta)247-265
Número de páginas19
PublicaciónFaraday Discussions
Volumen134
DOI
EstadoPublished - 2007

Huella dactilar

Oxides
Density functional theory
Hydrogen
interstitials
Thermodynamic stability
thermodynamics
Defects
oxides
defects
hydrogen
Doping (additives)
Thermodynamics
Chemical potential
Vibrational spectra
energy of formation
doped crystals
Hydration
Partial pressure
Spatial distribution
Electronic structure

ASJC Scopus subject areas

  • Physical and Theoretical Chemistry

Citar esto

@article{c4524a11fe854798a974156efe973be2,
title = "Structure and thermodynamic stability of hydrogen interstitials in BaZrO3 perovskite oxide from density functional calculations",
abstract = "Density functional calculations have been used to study the electronic structure, preferred sites in the lattice, formation energies and vibrational frequencies for hydrogen interstitials in different charge states in the cubic phase of perovskite-structured BaZrO3. By combining ab initio results with thermodynamic modeling, defect formation at finite temperature and pressure has been investigated. We demonstrate how the site selectivity and spatial distribution of dopant atoms in the lattice can be affected by changes in the environmental conditions (atomic chemical potentials, oxygen partial pressure and temperature) used during processing of the material. In addition, we have calculated the thermodynamic parameters of the water uptake reaction for an acceptor-doped BaZrO3 crystal in equilibrium with a humid atmosphere. The interaction energies between a protonic defect and the investigated Ga, Gd, In, Nd, Sc, and Y dopants were found to be attractive, and we show that a simple model of defect association may reproduce an experimentally observed trend in the hydration enthalpy.",
author = "Bj{\"o}rketun, {M{\aa}rten E.} and Sundell, {Per G.} and G{\"o}ran Wahnstr{\"o}m",
year = "2007",
doi = "10.1039/b602081j",
language = "English",
volume = "134",
pages = "247--265",
journal = "Faraday Discussions",
issn = "1364-5498",
publisher = "Royal Society of Chemistry",

}

Structure and thermodynamic stability of hydrogen interstitials in BaZrO3 perovskite oxide from density functional calculations. / Björketun, Mårten E.; Sundell, Per G.; Wahnström, Göran.

En: Faraday Discussions, Vol. 134, 2007, p. 247-265.

Resultado de la investigación: Article

TY - JOUR

T1 - Structure and thermodynamic stability of hydrogen interstitials in BaZrO3 perovskite oxide from density functional calculations

AU - Björketun, Mårten E.

AU - Sundell, Per G.

AU - Wahnström, Göran

PY - 2007

Y1 - 2007

N2 - Density functional calculations have been used to study the electronic structure, preferred sites in the lattice, formation energies and vibrational frequencies for hydrogen interstitials in different charge states in the cubic phase of perovskite-structured BaZrO3. By combining ab initio results with thermodynamic modeling, defect formation at finite temperature and pressure has been investigated. We demonstrate how the site selectivity and spatial distribution of dopant atoms in the lattice can be affected by changes in the environmental conditions (atomic chemical potentials, oxygen partial pressure and temperature) used during processing of the material. In addition, we have calculated the thermodynamic parameters of the water uptake reaction for an acceptor-doped BaZrO3 crystal in equilibrium with a humid atmosphere. The interaction energies between a protonic defect and the investigated Ga, Gd, In, Nd, Sc, and Y dopants were found to be attractive, and we show that a simple model of defect association may reproduce an experimentally observed trend in the hydration enthalpy.

AB - Density functional calculations have been used to study the electronic structure, preferred sites in the lattice, formation energies and vibrational frequencies for hydrogen interstitials in different charge states in the cubic phase of perovskite-structured BaZrO3. By combining ab initio results with thermodynamic modeling, defect formation at finite temperature and pressure has been investigated. We demonstrate how the site selectivity and spatial distribution of dopant atoms in the lattice can be affected by changes in the environmental conditions (atomic chemical potentials, oxygen partial pressure and temperature) used during processing of the material. In addition, we have calculated the thermodynamic parameters of the water uptake reaction for an acceptor-doped BaZrO3 crystal in equilibrium with a humid atmosphere. The interaction energies between a protonic defect and the investigated Ga, Gd, In, Nd, Sc, and Y dopants were found to be attractive, and we show that a simple model of defect association may reproduce an experimentally observed trend in the hydration enthalpy.

UR - http://www.scopus.com/inward/record.url?scp=33845490401&partnerID=8YFLogxK

U2 - 10.1039/b602081j

DO - 10.1039/b602081j

M3 - Article

VL - 134

SP - 247

EP - 265

JO - Faraday Discussions

JF - Faraday Discussions

SN - 1364-5498

ER -