Disorder-induced transition from grain boundary to bulk dominated ionic diffusion in pyrochlores

Perriot, Romain; Dholabhai, Pratik P.; Uberuaga, Blas P.

doi:10.1039/C7NR01373F

Title: Disorder-induced transition from grain boundary to bulk dominated ionic diffusion in pyrochlores

Abstract

In this paper, we use molecular dynamics simulations to investigate the role of grain boundaries (GBs) on ionic diffusion in pyrochlores, as a function of the GB type, chemistry of the compound, and level of cation disorder. We observe that the presence of GBs promotes oxygen transport in ordered and low-disordered systems, as the GBs are found to have a higher concentration of mobile carriers with higher mobilities than in the bulk. Thus, in ordered samples, the ionic diffusion is 2D, localized along the grain boundary. When cation disorder is introduced, bulk carriers begin to contribute to the overall diffusion, while the GB contribution is only slightly enhanced. In highly disordered samples, the diffusive behavior at the GBs is bulk-like, and the two contributions (bulk vs. GB) can no longer be distinguished. There is thus a transition from 2D/GB dominated oxygen diffusivity to 3D/bulk dominated diffusivity versus disorder in pyrochlores. Finally, these results provide new insights into the possibility of using internal interfaces to enhance ionic conductivity in nanostructured complex oxides.

Authors:

^[1]; Dholabhai, Pratik P. ^[1];

^[1]

Los Alamos National Lab. (LANL), Los Alamos, NM (United States)

Publication Date:: Thu May 04 00:00:00 EDT 2017

Research Org.:: Los Alamos National Lab. (LANL), Los Alamos, NM (United States)

Sponsoring Org.:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

OSTI Identifier:: 1402631

Report Number(s):: LA-UR-17-23205
Journal ID: ISSN 2040-3364; TRN: US1703116

Grant/Contract Number:: AC52-06NA25396

Resource Type:: Accepted Manuscript

Journal Name:: Nanoscale

Additional Journal Information:: Journal Volume: 9; Journal Issue: 20; Journal ID: ISSN 2040-3364

Publisher:: Royal Society of Chemistry

Country of Publication:: United States

Language:: English

Subject:: 36 MATERIALS SCIENCE

Citation Formats


                    Perriot, Romain, Dholabhai, Pratik P., and Uberuaga, Blas P. Disorder-induced transition from grain boundary to bulk dominated ionic diffusion in pyrochlores.  United States: N. p., 2017. 
Web.  doi:10.1039/C7NR01373F.

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                    Perriot, Romain, Dholabhai, Pratik P., & Uberuaga, Blas P. Disorder-induced transition from grain boundary to bulk dominated ionic diffusion in pyrochlores.  United States.  https://doi.org/10.1039/C7NR01373F

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                    Perriot, Romain, Dholabhai, Pratik P., and Uberuaga, Blas P. Thu .  
"Disorder-induced transition from grain boundary to bulk dominated ionic diffusion in pyrochlores".  United States.  https://doi.org/10.1039/C7NR01373F.  https://www.osti.gov/servlets/purl/1402631.

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@article{osti_1402631,

  title        = {Disorder-induced transition from grain boundary to bulk dominated ionic diffusion in pyrochlores},

  author       = {Perriot, Romain and Dholabhai, Pratik P. and Uberuaga, Blas P.},

  abstractNote = {In this paper, we use molecular dynamics simulations to investigate the role of grain boundaries (GBs) on ionic diffusion in pyrochlores, as a function of the GB type, chemistry of the compound, and level of cation disorder. We observe that the presence of GBs promotes oxygen transport in ordered and low-disordered systems, as the GBs are found to have a higher concentration of mobile carriers with higher mobilities than in the bulk. Thus, in ordered samples, the ionic diffusion is 2D, localized along the grain boundary. When cation disorder is introduced, bulk carriers begin to contribute to the overall diffusion, while the GB contribution is only slightly enhanced. In highly disordered samples, the diffusive behavior at the GBs is bulk-like, and the two contributions (bulk vs. GB) can no longer be distinguished. There is thus a transition from 2D/GB dominated oxygen diffusivity to 3D/bulk dominated diffusivity versus disorder in pyrochlores. Finally, these results provide new insights into the possibility of using internal interfaces to enhance ionic conductivity in nanostructured complex oxides.},

  doi          = {10.1039/C7NR01373F},

  journal      = {Nanoscale},

  number       = 20,

  volume       = 9,

  place        = {United States},

  year         = {Thu May 04 00:00:00 EDT 2017},

  month        = {Thu May 04 00:00:00 EDT 2017}

}

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Evidence for percolation diffusion of cations and reordering in disordered pyrochlore from accelerated molecular dynamics

Journal Article Perriot, Romain ; Uberuaga, Blas P. ; Zamora, Richard J. ; ... - Nature Communications

Diffusion in complex oxides is critical to ionic transport, radiation damage evolution, sintering, and aging. In complex oxides such as pyrochlores, anionic diffusion is dramatically affected by cation disorder. However, little is known about how disorder influences cation transport. Here, we report results from classical and accelerated molecular dynamics simulations of vacancy-mediated cation diffusion in Gd₂Ti₂O₇ pyrochlore, on the microsecond timescale. We find that diffusion is slow at low levels of disorder, while higher disorder allows for fast diffusion, which is then accompanied by antisite annihilation and reordering, and thus a slowing of cation transport. Cation diffusivity is therefore notmore »« less
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https://doi.org/10.1038/s41467-017-00708-z

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Title: Disorder-induced transition from grain boundary to bulk dominated ionic diffusion in pyrochlores

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Oxygen ion diffusivity in strained yttria stabilized zirconia: where is the fastest strain? journal, January 2010

Pipe diffusion at dislocations in UO2 journal, April 2014

Dislocations in SrTiO 3 : Easy To Reduce but Not so Fast for Oxygen Transport journal, April 2015

Connection between oxygen-ion conductivity of pyrochlore fuel-cell materials and structural change with composition and temperature journal, April 2000

Review of A2B2O7 pyrochlore response to irradiation and pressure journal, October 2010

Molecular dynamics study of the effect of doping and disorder on diffusion in gadolinium zirconate journal, October 1998

Point Defects in Oxides: Tailoring Materials Through Defect Engineering journal, August 2011

Cation size effects in oxygen ion dynamics of highly disordered pyrochlore-type ionic conductors journal, September 2008

Response to Comment on "Colossal Ionic Conductivity at Interfaces of Epitaxial ZrO2:Y2O3/SrTiO3 Heterostructures" journal, April 2009

Defects and diffusion in pyrochlore structured oxides journal, October 1998

Microstructure design for fast oxygen conduction journal, November 2015

Ion Beam-Induced Amorphization of the Pyrochlore Structure-Type: A Review journal, January 2003

Grain boundaries in dielectric and mixed-conducting ceramics journal, February 2000

Fast Parallel Algorithms for Short-Range Molecular Dynamics journal, March 1995

GBstudio: A Builder Software on Periodic Models of CSL Boundaries for Molecular Simulation journal, January 2006

Computational Study of Oxygen Diffusion along a [100] Dislocations in the Perovskite Oxide SrTiO 3 journal, May 2016

Atomic disorder in Gd 2 Zr 2 O 7 pyrochlore journal, May 2015

Colossal Ionic Conductivity at Interfaces of Epitaxial ZrO2:Y2O3/SrTiO3 Heterostructures journal, August 2008

Grain Boundary Blocking Effect in Zirconia: A Schottky Barrier Analysis journal, January 2001

Oxygen diffusion in nanocrystalline yttria-stabilized zirconia: the effect of grain boundaries journal, January 2008

Grain boundary stoichiometry and interactions with defects in SrTiO3 journal, January 2012

Effects of Oxygen Vacancies and Reaction Conditions on Oxygen Reduction Reaction on Pyrochlore-Type Lead-Ruthenium Oxide journal, November 2014

Radiation Tolerance of Complex Oxides journal, August 2000

Optimization of synthesis conditions for rare-earth titanate based oxygen ion conductors journal, January 2013

Pyrochlore to Fluorite Transition: The Y 2 (Ti 1– x Zr x ) 2 O 7 (0.0 ≤ x ≤ 1.0) System journal, November 2012

Fast ion conductivity in strained defect-fluorite structure created by ion tracks in Gd2Ti2O7 journal, November 2015

Grain boundary conductivity of high purity neodymium-doped ceria nanosystem with and without the doping of molybdenum oxide journal, November 2007

Diffusion along grain boundaries and dislocations in oxides, alkali halides and carbides journal, March 1984

Ionic conduction in the Gd2Ti2O7−Gd2Zr2O7 system journal, September 1988

Ion irradiation of novel yttrium/ytterbium-based pyrochlores: The effect of disorder journal, December 2011

First-principles prediction of disordering tendencies in pyrochlore oxides journal, March 2009

Diffusion mechanisms in Cu grain boundaries journal, August 2000

Blocking Grain Boundaries in Yttria-Doped and Undoped Ceria Ceramics of High Purity journal, January 2003

Observation of Giant Diffusivity Along Dislocation Cores journal, March 2008

Oxygen Diffusion in SrTiO 3 and Related Perovskite Oxides journal, August 2015

Tunability of structure from ordered to disordered and its impact on ionic conductivity behavior in the Nd2−yHoyZr2O7 (0.0 ≤ y ≤ 2.0) system journal, January 2012

Forging Fast Ion Conducting Nanochannels with Swift Heavy Ions: The Correlated Role of Local Electronic and Atomic Structure journal, December 2016

A brief review of the ionic conductivity enhancement for selected oxide electrolytes journal, October 2007

Structure and Mobility of Defects Formed from Collision Cascades in MgO journal, March 2004

Disorder in Pyrochlore Oxides journal, August 2000

Comment on "Colossal Ionic Conductivity at Interfaces of Epitaxial ZrO2:Y2O3/SrTiO3 Heterostructures" journal, April 2009

Fast-Ion Conducting Y2(Zr Ti1-)2O7 Pyrochlores: Neutron Rietveld Analysis of Disorder Induced by Zr Substitution journal, June 1995

Ion Irradiation of Ternary Pyrochlore Oxides journal, July 2009

Temperature dependence of the radiation tolerance of nanocrystalline pyrochlores A2Ti2O7 (A = Gd, Ho and Lu) journal, May 2016

Atomic-Scale Structure and Stability of the Low-Index Surfaces of Pyrochlore Oxides journal, May 2016

Ionic transport in nano-sized systems journal, November 2004

Modelling and characterization of mixed ionic-electronic conduction in Gd2(Ti1 − xMnx)2O7 + y journal, July 1996

Uranium vacancy mobility at the Σ5 symmetric tilt and Σ5 twist grain boundaries in UO2 journal, October 2015

Predicted pyrochlore to fluorite disorder temperature for A 2 Zr 2 O 7 compositions journal, June 2004

Defect formation energies in A 2 B 2 O 7 pyrochlores journal, October 2015

The relationship between grain boundary structure, defect mobility and grain boundary sink efficiency journal, March 2015

Oxygen Pipe Diffusion in Sapphire Basal Dislocation journal, January 2006

Ionic conductivity in oxide heterostructures: the role of interfaces journal, October 2010

Termination chemistry-driven dislocation structure at SrTiO3/MgO heterointerfaces journal, September 2014

Derivative Crystal Structures journal, January 1947

Structural vs. intrinsic carriers: contrasting effects of cation chemistry and disorder on ionic conductivity in pyrochlores journal, January 2015

Edge dislocation slows down oxide ion diffusion in doped CeO2 by segregation of charged defects journal, February 2015

Insights into dynamic processes of cations in pyrochlores and other complex oxides journal, January 2015

Surface and interface mass transport in ionic materials journal, September 1988

Self-diffusion near symmetrical tilt grain boundaries in UO2 matrix: A molecular dynamics simulation study journal, July 2009

Radiation-induced amorphization resistance and radiation tolerance in structurally related oxides journal, February 2007

The interaction of oxygen vacancies with grain boundaries in monoclinic HfO2 journal, November 2009

Predicted structure and stability of A 4 B 3 O 12 δ -phase compositions journal, November 2009

Effect of oxygen partial pressure on the bulk and grain-boundary components of conductivity in (Yb1−xCax)2Ti2O7−δ (x=0, 0.05, 0.1) solid solutions journal, July 2013

Novel potentials for modelling defect formation and oxygen vacancy migration in Gd2Ti2O7 and Gd2Zr2O7 pyrochlores journal, January 2012

Electrical conductivity anomaly around fluorite–pyrochlore phase boundary journal, March 2003

Electrical properties of the grain boundaries of oxygen ion conductors: Acceptor-doped zirconia and ceria journal, February 2006

Prediction of Rare-Earth A 2 Hf 2 O 7 Pyrochlore Phases journal, August 2002

Defect chemistry and ion transport in nanostructured materials Part II. Aspects of nanoionics journal, February 2003

Single-ion tracks in Gd 2 Zr 2 − x Ti x O 7 pyrochlores irradiated with swift heavy ions journal, June 2009

Study of bulk and grain-boundary conductivity of Ln2+xHf2−xO7−δ (Ln = Sm-Gd; x = 0, 0.096) pyrochlores journal, May 2009

Oxygen ion conduction and structural disorder in conductive oxides journal, December 1994

Nanoscale Manipulation of Pyrochlore: New Nanocomposite Ionic Conductors journal, September 2001

High ionic conductivity in the pyrochlore-type Gd2−yLayZr2O7 solid solution (0≤y≤1) journal, November 2008

Oxygen ion diffusivity in strained yttria stabilized zirconia: where is the fastest strain?
journal, January 2010

Pipe diffusion at dislocations in UO2
journal, April 2014

Dislocations in SrTiO ₃ : Easy To Reduce but Not so Fast for Oxygen Transport
journal, April 2015

Connection between oxygen-ion conductivity of pyrochlore fuel-cell materials and structural change with composition and temperature
journal, April 2000

Review of A2B2O7 pyrochlore response to irradiation and pressure
journal, October 2010

Molecular dynamics study of the effect of doping and disorder on diffusion in gadolinium zirconate
journal, October 1998

Point Defects in Oxides: Tailoring Materials Through Defect Engineering
journal, August 2011

Cation size effects in oxygen ion dynamics of highly disordered pyrochlore-type ionic conductors
journal, September 2008

Response to Comment on "Colossal Ionic Conductivity at Interfaces of Epitaxial ZrO2:Y2O3/SrTiO3 Heterostructures"
journal, April 2009

Defects and diffusion in pyrochlore structured oxides
journal, October 1998

Microstructure design for fast oxygen conduction
journal, November 2015

Ion Beam-Induced Amorphization of the Pyrochlore Structure-Type: A Review
journal, January 2003

Grain boundaries in dielectric and mixed-conducting ceramics
journal, February 2000

Fast Parallel Algorithms for Short-Range Molecular Dynamics
journal, March 1995

GBstudio: A Builder Software on Periodic Models of CSL Boundaries for Molecular Simulation
journal, January 2006

Computational Study of Oxygen Diffusion along a [100] Dislocations in the Perovskite Oxide SrTiO ₃
journal, May 2016

Atomic disorder in Gd ₂ Zr ₂ O ₇ pyrochlore
journal, May 2015

Colossal Ionic Conductivity at Interfaces of Epitaxial ZrO2:Y2O3/SrTiO3 Heterostructures
journal, August 2008

Grain Boundary Blocking Effect in Zirconia: A Schottky Barrier Analysis
journal, January 2001

Oxygen diffusion in nanocrystalline yttria-stabilized zirconia: the effect of grain boundaries
journal, January 2008

Grain boundary stoichiometry and interactions with defects in SrTiO3
journal, January 2012

Effects of Oxygen Vacancies and Reaction Conditions on Oxygen Reduction Reaction on Pyrochlore-Type Lead-Ruthenium Oxide
journal, November 2014

Radiation Tolerance of Complex Oxides
journal, August 2000

Optimization of synthesis conditions for rare-earth titanate based oxygen ion conductors
journal, January 2013

Pyrochlore to Fluorite Transition: The Y ₂ (Ti _{1– x} Zr _x ) ₂ O ₇ (0.0 ≤ x ≤ 1.0) System
journal, November 2012

Fast ion conductivity in strained defect-fluorite structure created by ion tracks in Gd2Ti2O7
journal, November 2015

Grain boundary conductivity of high purity neodymium-doped ceria nanosystem with and without the doping of molybdenum oxide
journal, November 2007

Diffusion along grain boundaries and dislocations in oxides, alkali halides and carbides
journal, March 1984

Ionic conduction in the Gd2Ti2O7−Gd2Zr2O7 system
journal, September 1988

Ion irradiation of novel yttrium/ytterbium-based pyrochlores: The effect of disorder
journal, December 2011

First-principles prediction of disordering tendencies in pyrochlore oxides
journal, March 2009

Diffusion mechanisms in Cu grain boundaries
journal, August 2000

Blocking Grain Boundaries in Yttria-Doped and Undoped Ceria Ceramics of High Purity
journal, January 2003

Observation of Giant Diffusivity Along Dislocation Cores
journal, March 2008

Oxygen Diffusion in SrTiO ₃ and Related Perovskite Oxides
journal, August 2015

Tunability of structure from ordered to disordered and its impact on ionic conductivity behavior in the Nd2−yHoyZr2O7 (0.0 ≤ y ≤ 2.0) system
journal, January 2012

Forging Fast Ion Conducting Nanochannels with Swift Heavy Ions: The Correlated Role of Local Electronic and Atomic Structure
journal, December 2016

A brief review of the ionic conductivity enhancement for selected oxide electrolytes
journal, October 2007

Structure and Mobility of Defects Formed from Collision Cascades in MgO
journal, March 2004

Disorder in Pyrochlore Oxides
journal, August 2000

Comment on "Colossal Ionic Conductivity at Interfaces of Epitaxial ZrO2:Y2O3/SrTiO3 Heterostructures"
journal, April 2009

Fast-Ion Conducting Y2(Zr Ti1-)2O7 Pyrochlores: Neutron Rietveld Analysis of Disorder Induced by Zr Substitution
journal, June 1995

Ion Irradiation of Ternary Pyrochlore Oxides
journal, July 2009

Temperature dependence of the radiation tolerance of nanocrystalline pyrochlores A2Ti2O7 (A = Gd, Ho and Lu)
journal, May 2016

Atomic-Scale Structure and Stability of the Low-Index Surfaces of Pyrochlore Oxides
journal, May 2016

Ionic transport in nano-sized systems
journal, November 2004

Modelling and characterization of mixed ionic-electronic conduction in Gd2(Ti1 − xMnx)2O7 + y
journal, July 1996

Uranium vacancy mobility at the Σ5 symmetric tilt and Σ5 twist grain boundaries in UO2
journal, October 2015

Predicted pyrochlore to fluorite disorder temperature for A ₂ Zr ₂ O ₇ compositions
journal, June 2004

Defect formation energies in A 2 B 2 O 7 pyrochlores
journal, October 2015

The relationship between grain boundary structure, defect mobility and grain boundary sink efficiency
journal, March 2015

Oxygen Pipe Diffusion in Sapphire Basal Dislocation
journal, January 2006

Ionic conductivity in oxide heterostructures: the role of interfaces
journal, October 2010

Termination chemistry-driven dislocation structure at SrTiO3/MgO heterointerfaces
journal, September 2014

Derivative Crystal Structures
journal, January 1947

Structural vs. intrinsic carriers: contrasting effects of cation chemistry and disorder on ionic conductivity in pyrochlores
journal, January 2015

Edge dislocation slows down oxide ion diffusion in doped CeO2 by segregation of charged defects
journal, February 2015

Insights into dynamic processes of cations in pyrochlores and other complex oxides
journal, January 2015

Surface and interface mass transport in ionic materials
journal, September 1988

Self-diffusion near symmetrical tilt grain boundaries in UO2 matrix: A molecular dynamics simulation study
journal, July 2009

Radiation-induced amorphization resistance and radiation tolerance in structurally related oxides
journal, February 2007

The interaction of oxygen vacancies with grain boundaries in monoclinic HfO2
journal, November 2009

Predicted structure and stability of $A_{4} B_{3} O_{12}$ $δ$ -phase compositions
journal, November 2009

Effect of oxygen partial pressure on the bulk and grain-boundary components of conductivity in (Yb1−xCax)2Ti2O7−δ (x=0, 0.05, 0.1) solid solutions
journal, July 2013

Novel potentials for modelling defect formation and oxygen vacancy migration in Gd2Ti2O7 and Gd2Zr2O7 pyrochlores
journal, January 2012

Electrical conductivity anomaly around fluorite–pyrochlore phase boundary
journal, March 2003

Electrical properties of the grain boundaries of oxygen ion conductors: Acceptor-doped zirconia and ceria
journal, February 2006

Prediction of Rare-Earth A ₂ Hf ₂ O ₇ Pyrochlore Phases
journal, August 2002

Defect chemistry and ion transport in nanostructured materials Part II. Aspects of nanoionics
journal, February 2003

Single-ion tracks in ${Gd}_{2} {Zr}_{2 - x} {Ti}_{x} O_{7}$ pyrochlores irradiated with swift heavy ions
journal, June 2009

Study of bulk and grain-boundary conductivity of Ln2+xHf2−xO7−δ (Ln = Sm-Gd; x = 0, 0.096) pyrochlores
journal, May 2009

Oxygen ion conduction and structural disorder in conductive oxides
journal, December 1994

Nanoscale Manipulation of Pyrochlore: New Nanocomposite Ionic Conductors
journal, September 2001

High ionic conductivity in the pyrochlore-type Gd2−yLayZr2O7 solid solution (0≤y≤1)
journal, November 2008