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An Interdisciplinary View of Interfaces: Perspectives Regarding Emergent Phase Formation

Journal Article · · Journal of Electrochemical Energy Conversion and Storage
DOI:https://doi.org/10.1115/1.4037583· OSTI ID:1470190
 [1]
  1. Department of Materials Science and Engineering, Clemson University, Clemson, SC 29634 e-mail: 

A perspective on emergent phase formation is presented using an interdisciplinary approach gained by working at the “interface” between diverse application areas, including solid oxide fuel cells (SOFCs) and ionic membrane systems, solid state lithium batteries, and ceramics for nuclear waste immobilization. The grain boundary interfacial characteristics of model single-phase materials in these application areas, including (i) CeO2, (ii) Li7La3Zr2O12 (LLZO), and (iii) hollandite of the form BaxCsyGa2x+yTi8-2x-yO16, as well as the potential for emergent phase formation in composite systems, are discussed. The potential physical properties resulting from emergent phase structure and distribution are discussed, including an overview of existing three-dimensional (3D) imaging techniques recently used for characterization. Finally, an approach for thermodynamic characterization of emergent phases based on melt solution calorimetry is outlined, which may be used to predict the energy landscape including phase formation and stability of complex multiphase systems.

Research Organization:
Energy Frontier Research Centers (EFRC) (United States). Center for Hierarchical Waste Form Materials (CHWM)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
DOE Contract Number:
SC0016574
OSTI ID:
1470190
Journal Information:
Journal of Electrochemical Energy Conversion and Storage, Vol. 15, Issue 1; ISSN 2381-6872
Publisher:
ASME
Country of Publication:
United States
Language:
English

References (84)

Defect and transport properties of nanocrystalline CeO 2− x journal July 1996
High proton conduction in grain-boundary-free yttrium-doped barium zirconate films grown by pulsed laser deposition journal September 2010
Epitaxial and Polycrystalline Gadolinia-Doped Ceria Cathode Interlayers for Low Temperature Solid Oxide Fuel Cells journal January 2011
Interaction between chromia forming alloy interconnects and air electrode of solid oxide fuel cells journal August 1997
Chromium Poisoning and Degradation at (La,Sr)MnO[sub 3] and (La,Sr)FeO[sub 3] Cathodes for Solid Oxide Fuel Cells journal January 2010
Ceria-based solid electrolytes journal January 1996
Thermodynamics of solid electrolytes and related oxide ceramics based on the fluorite structure journal January 2010
Titanates, zirconates, aluminates and ferrites as waste forms for actinide immobilization journal September 2016
Garnet nuclear waste forms – Solubility at repository conditions journal January 2014
Ionic conductivities of hollandites journal April 1978
A-site compositional effects in Ga-doped hollandite materials of the form BaxCsyGa2x+yTi8−2x−yO16: implications for Cs immobilization in crystalline ceramic waste forms journal June 2016
Multiple grain boundary transitions in ceramics: A case study of alumina journal September 2007
Atomic structural environment of grain boundary segregated Y and Zr in creep resistant alumina from EXAFS journal September 1999
Complexion: A new concept for kinetic engineering in materials science journal October 2007
Partial electronic and ionic conduction in nanocrystalline ceria: role of space charge journal January 2004
On the Conductivity Mechanism of Nanocrystalline Ceria journal January 2002
Micro-ionics: next generation power sources journal January 2009
Space–charge theory applied to the grain boundary impedance of proton conducting BaZr0.9Y0.1O3−δ journal March 2010
The Oxygen Permeation Properties of Nanocrystalline CeO[sub 2] Thin Films journal January 2010
Chemical Expansion: Implications for Electrochemical Energy Storage and Conversion Devices journal July 2014
Reduction reactions in doped ceria ceramics studied by dilatometry journal January 1993
Modifying the barriers for oxygen-vacancy migration in fluorite-structured CeO 2 electrolytes through strain: a computer simulation study journal January 2012
“Stretching” the energy landscape of oxides—Effects on electrocatalysis and diffusion journal February 2014
The effect of mechanical twisting on oxygen ionic transport in solid-state energy conversion membranes journal June 2015
Strain induced ionic conductivity enhancement in epitaxial Ce 0.9 Gd 0.1 O 2−δ thin films journal January 2012
Segregation Effects at Grain Boundaries in Fluorite-Structured Ceramics journal September 2002
Direct evidence of dopant segregation in Gd-doped ceria journal February 2011
Thermally-Induced Dopant Segregation Effects on the Space Charge Layer and Ionic Conductivity of Nanocrystalline Gadolinia-Doped Ceria journal January 2016
Grain boundary blocking of ionic conductivity in nanocrystalline yttria-doped ceria thin films journal July 2015
Microstructure design for fast oxygen conduction journal November 2015
Enhancing grain boundary ionic conductivity in mixed ionic–electronic conductors journal April 2015
Novel Fast Lithium Ion Conduction in Garnet-Type Li 5 La 3 M 2 O 12 (M = Nb, Ta) journal March 2003
Fast Lithium Ion Conduction in Garnet-Type Li7La3Zr2O12 journal October 2007
Effect of microstructure and surface impurity segregation on the electrical and electrochemical properties of dense Al-substituted Li 7 La 3 Zr 2 O 12 journal January 2014
Synthesis and structure analysis of tetragonal Li7La3Zr2O12 with the garnet-related type structure journal August 2009
Crystal Structure of Fast Lithium-ion-conducting Cubic Li 7 La 3 Zr 2 O 12 journal January 2011
Al-doped Li7La3Zr2O12 synthesized by a polymerized complex method journal October 2011
Effect of substitution (Ta, Al, Ga) on the conductivity of Li7La3Zr2O12 journal May 2012
Electron microscopy characterization of hot-pressed Al substituted Li7La3Zr2O12 journal February 2012
Effect of calcining and Al doping on structure and conductivity of Li 7 La 3 Zr 2 O 12 journal November 2014
Synthesis of single phase cubic Al-substituted Li7La3Zr2O12 by solid state lithiation of mixed hydroxides journal October 2015
High lithium ion conductive Li7La3Zr2O12 by inclusion of both Al and Si journal May 2011
Synthesis and high Li-ion conductivity of Ga-stabilized cubic Li7La3Zr2O12 journal June 2012
Stabilization of cubic lithium-stuffed garnets of the type “Li7La3Zr2O12” by addition of gallium journal March 2013
Ga-substituted Li7La3Zr2O12: An investigation based on grain coarsening in garnet-type lithium ion conductors journal February 2017
Tetragonal vs. cubic phase stability in Al – free Ta doped Li 7 La 3 Zr 2 O 12 (LLZO) journal January 2014
Reversible ion exchange and structural stability of garnet-type Nb-doped Li7La3Zr2O12 in water for applications in lithium batteries journal May 2015
W-Doped Li7La3Zr2O12 Ceramic Electrolytes for Solid State Li-ion Batteries journal October 2015
Microstructural characterization of single-crystalline potassium hollandite nanowires journal December 2008
Low-Temperature Phase of Sodium Priderite, NaxCrxTi8–xO16, with a Monoclinic Hollandite Structure journal June 1999
Hollandite cathodes for lithium ion batteries. 2. Thermodynamic and kinetics studies of lithium insertion into BaMMn7O16 (M=Mg, Mn, Fe, Ni) journal May 2001
Disposal of high-level nuclear wastes: a geological perspective journal April 1985
HIPed Tailored Hollandite Waste Forms for the Immobilization of Radioactive Cs and Sr journal May 2009
Structural Evolution in Hollandite Solid Solutions Across the A‐Site Compositional Range from Ba 1.33 Ga 2.66 Ti 5.34 O 16 to Cs 1.33 Ga 1.33 Ti 6.67 O 16 journal August 2016
Oxygen permeability of nanocrystalline Ce0.8Gd0.2O1.9–CoFe2O4 mixed-conductive films journal December 2006
Oxygen Permeation Properties of Ceria-Ferrite-Based Composites journal July 2004
Influence of Microstructure and Surface Activation of Dual-Phase Membrane Ce 0.8 Gd 0.2 O 2−δ -FeCo 2 O 4 on Oxygen Permeation journal September 2015
Characterization of 3D interconnected microstructural network in mixed ionic and electronic conducting ceramic composites journal January 2014
Gallium-Doped Li 7 La 3 Zr 2 O 12 Garnet-Type Electrolytes with High Lithium-Ion Conductivity journal January 2017
All solid state lithium batteries based on lamellar garnet-type ceramic electrolytes journal December 2015
Interface-Engineered All-Solid-State Li-Ion Batteries Based on Garnet-Type Fast Li + Conductors journal July 2016
Investigating the all-solid-state batteries based on lithium garnets and a high potential cathode – LiMn 1.5 Ni 0.5 O 4 journal January 2016
Origin of Outstanding Stability in the Lithium Solid Electrolyte Materials: Insights from Thermodynamic Analyses Based on First-Principles Calculations journal October 2015
Electrochemical Stability of Li 10 GeP 2 S 12 and Li 7 La 3 Zr 2 O 12 Solid Electrolytes journal January 2016
First-Principles Studies on Cation Dopants and Electrolyte|Cathode Interphases for Lithium Garnets journal May 2015
Melt processed single phase hollandite waste forms for nuclear waste immobilization: Ba1.0Cs0.3A2.3Ti5.7O16; A=Cr, Fe, Al journal January 2014
Melt processed multiphase ceramic waste forms for nuclear waste immobilization journal November 2014
Cold crucible induction melter test for crystalline ceramic waste form fabrication: A feasibility assessment journal April 2017
Preparation and Properties of the Ln 2 Ti 2 O 7 -Type Rare Earth Titanate journal July 1964
Phase relations and high temperature-XRD studies of Gd2−xNdxTi2O7 solid solutions journal January 2007
The durability of synroc journal August 1992
Single phase melt processed powellite (Ba,Ca)MoO4 for the immobilization of Mo-rich nuclear waste journal February 2013
Three-dimensional microstructural imaging methods for energy materials journal January 2013
Three-dimensional quantification of composition and electrostatic potential at individual grain boundaries in doped ceria journal January 2016
Electrochemical fields within 3D reconstructed microstructures of mixed ionic and electronic conducting devices journal November 2016
Dispersion, connectivity and tortuosity of hierarchical porosity composite SOFC cathodes prepared by freeze-casting journal February 2015
Three‐dimensional mapping of crystalline ceramic waste form materials journal April 2017
Critical path-driven property and performance transitions in heterogeneous microstructures journal February 2017
Progress and New Directions in Calorimetry: A 2014 Perspective journal October 2014
Synthesis, characterization and thermochemistry of Cs-, Rb- and Sr-substituted barium aluminium titanate hollandites journal April 2015
Thermochemical study of trivalent-doped ceria systems: CeO 2 –MO 1.5 (M = La, Gd, and Y) journal December 2006
A Calorimetric Study of the Lanthanide Aluminum Oxides and the Lanthanide Gallium Oxides: Stability of the Perovskites and the Garnets journal December 1998
Current-induced transition from particle-by-particle to concurrent intercalation in phase-separating battery electrodes journal September 2014
High-Energy Cathode Materials (Li 2 MnO 3 –LiMO 2 ) for Lithium-Ion Batteries journal March 2013