Phase stability, electrochemical stability and ionic conductivity of the Li10±1MP2X12 (M = Ge, Si, Sn, Al or P, and X = O, S or Se) family of superionic conductors
Reads0
Chats0
TLDR
In this article, the phase stability, electrochemical stability and Li+ conductivity of the Li10±1MP2X12 (M = Ge, Si, Sn, Al or P, and X = O, S or Se) family of superionic conductors using first principles calculations were investigated.Abstract:
We present an investigation of the phase stability, electrochemical stability and Li+ conductivity of the Li10±1MP2X12 (M = Ge, Si, Sn, Al or P, and X = O, S or Se) family of superionic conductors using first principles calculations. The Li10GeP2S12 (LGPS) superionic conductor has the highest Li+ conductivity reported to date, with excellent electrochemical performance demonstrated in a Li-ion rechargeable battery. Our results show that isovalent cation substitutions of Ge4+ have a small effect on the relevant intrinsic properties, with Li10SiP2S12 and Li10SnP2S12 having similar phase stability, electrochemical stability and Li+ conductivity as LGPS. Aliovalent cation substitutions (M = Al or P) with compensating changes in the Li+ concentration also have a small effect on the Li+ conductivity in this structure. Anion substitutions, however, have a much larger effect on these properties. The oxygen-substituted Li10MP2O12 compounds are predicted not to be stable (with equilibrium decomposition energies >90 meV per atom) and have much lower Li+ conductivities than their sulfide counterparts. The selenium-substituted Li10MP2Se12 compounds, on the other hand, show a marginal improvement in conductivity, but at the expense of reduced electrochemical stability. We also studied the effect of lattice parameter changes on the Li+ conductivity and found the same asymmetry in behavior between increases and decreases in the lattice parameters, i.e., decreases in the lattice parameters lower the Li+ conductivity significantly, while increases in the lattice parameters increase the Li+ conductivity only marginally. Based on these results, we conclude that the size of the S2− is near optimal for Li+ conduction in this structural framework.read more
Citations
More filters
Journal ArticleDOI
Python Materials Genomics (pymatgen): A robust, open-source python library for materials analysis
Shyue Ping Ong,William D. Richards,Anubhav Jain,Geoffroy Hautier,Michael Kocher,Shreyas Cholia,Dan Gunter,Vincent Chevrier,Kristin A. Persson,Gerbrand Ceder +9 more
TL;DR: The pymatgen library as mentioned in this paper is an open-source Python library for materials analysis that provides a well-tested set of structure and thermodynamic analyses relevant to many applications, and an open platform for researchers to collaboratively develop sophisticated analyses of materials data obtained both from first principles calculations and experiments.
Journal ArticleDOI
Inorganic Solid-State Electrolytes for Lithium Batteries: Mechanisms and Properties Governing Ion Conduction
John Christopher Bachman,Sokseiha Muy,Alexis Grimaud,Hao-Hsun Chang,Nir Pour,Simon Franz Lux,Odysseas Paschos,Filippo Maglia,Saskia Lupart,Peter Lamp,Livia Giordano,Yang Shao-Horn +11 more
TL;DR: Insight is provided into the physical parameters affecting the diffusion process, to allow for more efficient and target-oriented research on improving solid-state ion conductors.
Journal ArticleDOI
Negating interfacial impedance in garnet-based solid-state Li metal batteries
Xiaogang Han,Yunhui Gong,Kun Kelvin Fu,Xingfeng He,Gregory T. Hitz,Jiaqi Dai,Alexander J. Pearse,Boyang Liu,Howard Wang,Gary W. Rubloff,Yifei Mo,Venkataraman Thangadurai,Eric D. Wachsman,Liangbing Hu +13 more
TL;DR: Experimental and computational results reveal that the oxide coating enables wetting of metallic lithium in contact with the garnet electrolyte surface and the lithiated-alumina interface allows effective lithium ion transport between the lithium metal anode and garnets electrolyte.
Journal ArticleDOI
Origin of Outstanding Stability in the Lithium Solid Electrolyte Materials: Insights from Thermodynamic Analyses Based on First-Principles Calculations
Yizhou Zhu,Xingfeng He,Yifei Mo +2 more
TL;DR: The results suggest that the outstanding stability of the solid electrolyte materials is not thermodynamically intrinsic but is originated from kinetic stabilizations, and general principles for developing solid electrolytes materials with enhanced stability and for engineering interfaces in all-solid-state Li-ion batteries are provided.
Journal ArticleDOI
Interface Stability in Solid-State Batteries
William D. Richards,Lincoln J. Miara,Yan Wang,Jae Chul Kim,Gerbrand Ceder,Gerbrand Ceder,Gerbrand Ceder +6 more
TL;DR: In this article, the thermodynamics of formation of resistive interfacial phases are examined and the predicted interfacial phase formation is well correlated with experimental interfacial observations and battery performance.
References
More filters
Journal ArticleDOI
Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set.
Georg Kresse,Jürgen Furthmüller +1 more
TL;DR: An efficient scheme for calculating the Kohn-Sham ground state of metallic systems using pseudopotentials and a plane-wave basis set is presented and the application of Pulay's DIIS method to the iterative diagonalization of large matrices will be discussed.
Journal ArticleDOI
Projector augmented-wave method
TL;DR: An approach for electronic structure calculations is described that generalizes both the pseudopotential method and the linear augmented-plane-wave (LAPW) method in a natural way and can be used to treat first-row and transition-metal elements with affordable effort and provides access to the full wave function.
Journal ArticleDOI
Revised effective ionic radii and systematic studies of interatomic distances in halides and chalcogenides
TL;DR: The effective ionic radii of Shannon & Prewitt [Acta Cryst. (1969), B25, 925-945] are revised to include more unusual oxidation states and coordinations as mentioned in this paper.
Journal ArticleDOI
Canonical dynamics: Equilibrium phase-space distributions
TL;DR: The dynamical steady-state probability density is found in an extended phase space with variables x, p/sub x/, V, epsilon-dot, and zeta, where the x are reduced distances and the two variables epsilus-dot andZeta act as thermodynamic friction coefficients.
Journal ArticleDOI
Building better batteries
TL;DR: Researchers must find a sustainable way of providing the power their modern lifestyles demand to ensure the continued existence of clean energy sources.