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      The solid-state Li-ion conductor Li\(_7\)TaO\(_6\): A combined computational and experimental study

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          Abstract

          We study the oxo-hexametallate Li\(_7\)TaO\(_6\) with first-principles and classical molecular dynamics simulations, obtaining a low activation barrier for diffusion of \(\sim\)0.29 eV and a high ionic conductivity of \(5.7 \times 10^{-4}\) S cm\(^{-1}\) at room temperature (300 K). We find evidence for a wide electrochemical stability window from both calculations and experiments, suggesting its viable use as a solid-state electrolyte in next-generation solid-state Li-ion batteries. To assess its applicability in an electrochemical energy storage system, we performed electrochemical impedance spectroscopy measurements on multicrystalline pellets, finding substantial ionic conductivity, if below the values predicted from simulation. We further elucidate the relationship between synthesis conditions and the observed ionic conductivity using X-ray diffraction, inductively coupled plasma optical emission spectrometry, and X-ray photoelectron spectroscopy, and study the effects of Zr and Mo doping.

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          Origin of Outstanding Stability in the Lithium Solid Electrolyte Materials: Insights from Thermodynamic Analyses Based on First-Principles Calculations.

          First-principles calculations were performed to investigate the electrochemical stability of lithium solid electrolyte materials in all-solid-state Li-ion batteries. The common solid electrolytes were found to have a limited electrochemical window. Our results suggest that the outstanding stability of the solid electrolyte materials is not thermodynamically intrinsic but is originated from kinetic stabilizations. The sluggish kinetics of the decomposition reactions cause a high overpotential leading to a nominally wide electrochemical window observed in many experiments. The decomposition products, similar to the solid-electrolyte-interphases, mitigate the extreme chemical potential from the electrodes and protect the solid electrolyte from further decompositions. With the aid of the first-principles calculations, we revealed the passivation mechanism of these decomposition interphases and quantified the extensions of the electrochemical window from the interphases. We also found that the artificial coating layers applied at the solid electrolyte and electrode interfaces have a similar effect of passivating the solid electrolyte. Our newly gained understanding provided general principles for developing solid electrolyte materials with enhanced stability and for engineering interfaces in all-solid-state Li-ion batteries.
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            High electronic conductivity as the origin of lithium dendrite formation within solid electrolytes

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              Pseudopotentials periodic table: From H to Pu

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                Author and article information

                Journal
                24 October 2019
                Article
                1910.11079
                78f8eaa0-c248-42a2-ab48-d3b7ede3218c

                http://arxiv.org/licenses/nonexclusive-distrib/1.0/

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                Custom metadata
                cond-mat.mtrl-sci

                Condensed matter
                Condensed matter

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