Alloying effects on superionic conductivity in lithium indium halides for all-solid-state batteries

Zevgolis, Alysia; Wood, Brandon C.; Mehmedović, Zerina; Hall, Alex T.; Alves, Thomaz Coelho; Adelstein, Nicole

doi:10.1063/1.5011378

Cited by 36 publications

(52 citation statements)

References 28 publications

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“…We note that significant deviations in the polarization of Br and Cl were also shown to be correlated with Li + diffusion events in our previous work on Li 3 InBr 6 and Li 3 InBr 6−x Cl x [41,42].…”

Section: (C) Polarization Effects On Vacancy Interactionssupporting

confidence: 68%

Impacts of vacancy-induced polarization and distortion on diffusion in solid electrolyte Li ₃ OCl

Mehmedović

Wei

Grieder

et al. 2021

Phil. Trans. R. Soc. A.

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Lithium-rich oxychloride antiperovskites are promising solid electrolytes for enabling next-generation batteries. Here, we report a comprehensive study varying Li + concentrations in Li 3 OCl using ab initio molecular dynamics simulations. The simulations accurately capture the complex interactions between Li + vacancies ( V Li ′ ), the dominant mobile species in Li 3 OCl . The V Li ′ polarize and distort the host lattice, inducing additional non-vacancy-mediated diffusion mechanisms and correlated diffusion events that reduce the activation energy barrier at concentrations as low as 1.5% V Li ′ . Our analyses of discretized diffusion events in both space and time illustrate the critical interplay between correlated dynamics, polarization and local distortion in promoting ionic conductivity in Li 3 OCl . This article is part of the Theo Murphy meeting issue ‘Understanding fast-ion conduction in solid electrolytes’.

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Section: (C) Polarization Effects On Vacancy Interactionssupporting

confidence: 68%

Impacts of vacancy-induced polarization and distortion on diffusion in solid electrolyte Li ₃ OCl

Mehmedović

Wei

Grieder

et al. 2021

Phil. Trans. R. Soc. A.

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“…Another material, Li 3 InCl 6 , has been reported to have a RT conductivity of approximately 1 mS/cm, making it a correct model prediction. 9 Very little is reported in the literature regarding the remaining 19 materials to our knowledge.…”

mentioning

confidence: 99%

“…DFT-MD of Zevgolis et al9 for Li 3 InCl 6 ). Aside from Li 3 InCl 6 and Li 6 Ho(BO 3 ) 3 , none of these materials have reported DFT or experimental conductivity values in the literature to our…”

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confidence: 99%

Machine Learning-Assisted Discovery of Solid Li-Ion Conducting Materials

et al. 2018

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We discover many new crystalline solid materials with fast single crystal Li ion conductivity at room temperature, discovered through density functional theory simulations guided by machine learning-based methods. The discovery of new solid Li superionic conductors is of critical importance to the development of safe all-solid-state Li-ion batteries. With a predictive universal structure-property relationship for fast ion conduction not well understood, the search for new solid Li ion conductors has relied largely on trial-and-error computational and experimental searches over the last several decades. In this work, we perform a guided search of materials space with a machine learning (ML)-based prediction model for material selection and density functional theory molecular dynamics (DFT-MD) simulations for calculating ionic conductivity.These materials are screened from over 12,000 experimentally synthesized and characterized candidates with very diverse structures and compositions. When compared to a random search of materials space, we find that the ML-guided search is 2.7 times more likely to identify fast Li ion conductors, with at least a 45x improvement in the log-average of room temperature Li ion conductivity. The F1 score of the ML-based model is 0.50, 3.5 times better than the F1 score expected from completely random guesswork. In a head-to-head competition against six Ph.D. students working in the field, we find that the ML-based model doubles the F1 score of human experts in its ability to identify fast Li-ion conductors from atomistic structure with a thousandfold increase in speed, clearly demonstrating the utility of this model for the research community. In addition to having high predicted Li-ion conductivity, all materials reported here lack transition metals to enhance stability against reduction by Li metal anode, and are predicted to exhibit low electronic conduction, high stability against oxidation, and high thermodynamic stability, making them promising candidates for solid-state electrolyte applications on these several essential metrics.

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“…These factors include the role of various forms of inherent crystallographic disorder within the host-framework substructure [18,[26][27][28] and the presence of occupational disorder of the mobile-ion species across available sites [29][30][31]. Other studies have analysed fast-ion conduction by considering ways in which a given system may be 'frustrated', where competing energetic considerations prevent the mobile ions from adopting a single ordered low-energy configuration, with these mobile ions instead sampling a large number of disordered configurations with similar energies [18,26,[32][33][34][35]. In other materials, fast-ion conduction has been associated with specific hostframework dynamics, such as dynamical 'breathing' of diffusion-limiting bottlenecks [22], or polyanion rotations that may directly couple to the motion of the charge-carrying ions [24,[36][37][38].…”

Section: Introductionmentioning

confidence: 99%

Understanding fast-ion conduction in solid electrolytes

Morgan

2021

Phil. Trans. R. Soc. A.

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The ability of some solid materials to exhibit exceptionally high ionic conductivities has been known since the observations of Michael Faraday in the nineteenth century (Faraday M. 1838 Phil. Trans. R. Soc. 90 ), yet a detailed understanding of the atomic-scale physics that gives rise to this behaviour remains an open scientific question. This theme issue collects articles from researchers working on this question of understanding fast-ion conduction in solid electrolytes. The issue opens with two perspectives, both of which discuss concepts that have been proposed as schema for understanding fast-ion conduction. The first perspective presents an overview of a series of experimental NMR studies, and uses this to frame discussion of the roles of ion–ion interactions, crystallographic disorder, low-dimensionality of crystal structures, and fast interfacial diffusion in nanocomposite materials. The second perspective reviews computational studies of halides, oxides, sulfides and hydroborates, focussing on the concept of frustration and how this can manifest in different forms in various fast-ion conductors. The issue also includes five primary research articles, each of which presents a detailed analysis of the factors that affect microscopic ion-diffusion in specific fast-ion conducting solid electrolytes, including oxide-ion conductors Gd 2 Zr 2 O 7 and Bi 4 V 2 O 11 , lithium-ion conductors Li 6 PS 5 Br and Li 3 OCl , and the prototypical fluoride-ion conductor β - PbF 2 . This article is part of the Theo Murphy meeting issue ‘Understanding fast-ion conduction in solid electrolytes’.

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Alloying effects on superionic conductivity in lithium indium halides for all-solid-state batteries

Cited by 36 publications

References 28 publications

Impacts of vacancy-induced polarization and distortion on diffusion in solid electrolyte Li ₃ OCl

Impacts of vacancy-induced polarization and distortion on diffusion in solid electrolyte Li ₃ OCl

Machine Learning-Assisted Discovery of Solid Li-Ion Conducting Materials

Understanding fast-ion conduction in solid electrolytes

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Alloying effects on superionic conductivity in lithium indium halides for all-solid-state batteries

Cited by 36 publications

References 28 publications

Impacts of vacancy-induced polarization and distortion on diffusion in solid electrolyte Li 3 OCl

Impacts of vacancy-induced polarization and distortion on diffusion in solid electrolyte Li 3 OCl

Machine Learning-Assisted Discovery of Solid Li-Ion Conducting Materials

Understanding fast-ion conduction in solid electrolytes

Contact Info

Product

Resources

About

Impacts of vacancy-induced polarization and distortion on diffusion in solid electrolyte Li ₃ OCl

Impacts of vacancy-induced polarization and distortion on diffusion in solid electrolyte Li ₃ OCl