Abstract
LixFePO4 orthophosphates and fluorite- and pyrochlore-type zirconate materials are widely considered as functional compounds in energy storage devices, either as electrode or solid state electrolyte. These ceramic materials show enhanced cation exchange and anion conductivity properties that makes them attractive for various energy applications. In this contribution we discuss thermodynamic properties of LixFePO4 and yttria-stabilized zirconia compounds, including formation enthalpies, stability, and solubility limits. We found that at ambient conditions LixFePO4 has a large miscibility gap, which is consistent with existing experimental evidence. We show that cubic zirconia becomes stabilized with Y content of ~8%, which is in line with experimental observations. The computed activation energy of 0.92eV and ionic conductivity for oxygen diffusion in yttria-stabilized zirconia are also in line with the measured data, which shows that atomistic modeling can be applied for accurate prediction of key materials properties. We discuss these results with the existing simulation-based data on these materials produced by our group over the last decade. Last, but not least, we discuss similarities of the considered compounds in considering them as materials for energy storage and radiation damage resistant matrices for immobilization of radionuclides.
Highlights
We apply the linear response method (Cococcioni and de Gironcoli, 2005) with Wannier orbitals as representation of d or f states (Kvashnina et al, 2018) and here we will demonstrate impact of these procedures on the estimation of formation enthalpies and solubility limits of LixFePO4 compound. In this contribution we provide an overview of the recent atomistic modeling activities on the orthophosphates and zirconates, focusing on the information that have been delivered by atomistic modeling activities at Forschungszentrum Jülich and that allowed on many occasions for better characterization of these materials, including long-term thermodynamic stability, thermochemical parameters, and thermal conductivity
As discussed by Ahamer et al (2017) and Guan et al (2020), the oxygen diffusion in yttria-stabilized zirconia is a complex process, which details, could be revealed by combination of computed and measured data. In this contribution we presented an overview of our decadelong atomistic modeling contribution to the research on orthophosphates and zirconates type ceramics
We discussed the atomistic modeling derivation of structural, thermodynamic, and diffusion properties that are of importance for application of these materials as compounds in energy storage devices
Summary
MPO4 orthophosphates, with M cations being transition metals, rare-earth elements or actinides, are ceramic materials of interest in various research fields, including geochronology (Williams et al, 2007), geothermometry (Andrehs and Heinrich, 1998; Mogilevsky, 2007), energy storage (Iyer et al, 2006; Yamada et al, 2006; Dunn et al, 2015; Dong et al, 2017; Cerdas et al, 2018; Li et al, 2018; Phan et al, 2019), and nuclear waste management (Ewing and Wang, 2002; Neumeier et al, 2017a; Schlenz et al, 2018), to name but a few. We apply the linear response method (Cococcioni and de Gironcoli, 2005) with Wannier orbitals as representation of d or f states (Kvashnina et al, 2018) and here we will demonstrate impact of these procedures on the estimation of formation enthalpies and solubility limits of LixFePO4 compound In this contribution we provide an overview of the recent atomistic modeling activities on the orthophosphates and zirconates, focusing on the information that have been delivered by atomistic modeling activities at Forschungszentrum Jülich and that allowed on many occasions for better characterization of these materials, including long-term thermodynamic stability, thermochemical parameters, and thermal conductivity. We especially highlight a cross-linking, interdisciplinary character of our research, from which the general science community could highly benefit
Sign-in/Register to view highlights & summary Sign-in/Register to access full text options 
Free) 
Talk to us
Join us for a 30 min session where you can share your feedback and ask us any queries you have
Schedule a call
