Tuning mobility and stability of lithium ion conductors based on lattice dynamics

Muy, Sokseiha; Bachman, John Christopher; Giordano, Livia; Chang, Hung-Ju; Abernathy, D. L.; Bansal, Dipanshu; Delaire, Olivier; Hori, Shingo; Kanno, Ryoji; Maglia, Filippo; Lupart, Saskia; Lamp, Peter; Shao‐Horn, Yang

doi:10.1039/c7ee03364h

Cited by 199 publications

(312 citation statements)

References 66 publications

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“…In addition, the glass has a higher density of Li modes in the low-frequency region. Muy et al 79 have shown that a common feature of fast lithium conductors is low vibration frequencies. These lower frequencies are characteristic of larger thermal displacements, which correlate with a greater probability for migration.…”

Section: Resultsmentioning

confidence: 99%

Low-temperature paddlewheel effect in glassy solid electrolytes

2020

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Glasses are promising electrolytes for use in solid-state batteries. Nevertheless, due to their amorphous structure, the mechanisms that underlie their ionic conductivity remain poorly understood. Here, ab initio molecular dynamics is used to characterize migration processes in the prototype glass, 75Li 2 S-25P 2 S 5 . Lithium migration occurs via a mechanism that combines concerted motion of lithium ions with large, quasi-permanent reorientations of PS 4 3− anions. This latter effect, known as the 'paddlewheel' mechanism, is typically observed in hightemperature crystalline polymorphs. In contrast to the behavior of crystalline materials, in the glass paddlewheel dynamics contribute to Lithium-ion mobility at room temperature. Paddlewheel contributions are confirmed by characterizing spatial, temporal, vibrational, and energetic correlations with Lithium motion. Furthermore, the dynamics in the glass differ from those in the stable crystalline analogue, γ-Li 3 PS 4 , where anion reorientations are negligible and ion mobility is reduced. These data imply that glasses containing complex anions, and in which covalent network formation is minimized, may exhibit paddlewheel dynamics at low temperature. Consequently, these systems may be fertile ground in the search for new solid electrolytes.

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Section: Resultsmentioning

confidence: 99%

Low-temperature paddlewheel effect in glassy solid electrolytes

2020

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“…A first example is the correlation between the diffusion coefficients or Arrhenius barriers of diffusion and the frequencies of specific optical phonons, first presented by Wakamura and Aniya [79][80][81] for halides. Evidence for such correlation has also been found in LISICONs, and in the family of olivines [82], and this descriptor constituted the backbone for a very recent screening for solid-state Li-ion conductors [83]. As a second example, the importance of accessible volume for diffusion [76,84] led to the development of the bond-valence method by Adams and Swenson [85], and several efforts [86,87] employed this inexpensive method for screening purposes.…”

Section: Introductionmentioning

confidence: 94%

High-throughput computational screening for solid-state Li-ion conductors

Kahle

Marcolongo

Marzari

2020

Energy Environ. Sci.

119

106

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We present a computational screening of experimental structural repositories for fast Li-ion conductors, with the goal of finding new candidate materials for application as solid-state electrolytes in next-generation batteries. We start from ∼1400 unique Licontaining materials, of which ∼900 are insulators at the level of density-functional theory. For those, we calculate the diffusion coefficient in a highly automated fashion, using extensive molecular dynamics simulations on a potential energy surface (the recently published pinball model) fitted on first-principles forces. The ∼130 most promising candidates are studied with full first-principles molecular dynamics, first at high temperature and then more extensively for the 78 most promising candidates. The results of the first-principles simulations of the candidate solid-state electrolytes found are discussed in detail.of superionic conductors is the recent discovery of Li-argyrodites [22], with the general formula Li 7 PS 5 X (X=Cl, Br, I) or Li 7 PS 6 (sulphur can be replaced with oxygen, but this reduces the ionic conductivity [23]). Third, Li-containing NASICONs (sodium superionic conductors) are phosphates with the structural formula Li 1+6x X 4+2−x Y 3+x (PO

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“…Recent experimental studies associate a decrease in activation energy with a decrease in the pre-exponential factor and a lower ionic conductivity, suggesting that this factor can provide information about ionic conductivity. [42][43][44][45] Therefore, knowledge of the energy barriers alone is inadequate to support claims about high ionic conductivity within a material. AIMD simulations can provide more complete diffusional information in computational studies.…”

Section: Ab Initio Molecular Dynamics Simulationmentioning

confidence: 99%

“…However, other factors, such as the pre-exponential factor of the Arrhenius relation, are also critical to achieve a high ionic conductivity. The preexponential factor is related to many factors, including anion polarizability, lattice softness, mobile carrier concentration, and the ordering of the mobile-ion sublattice, [42][43][44][45] but design principles that consider these factors have not yet been developed. At the current stage, first-principles computation is required to identify the dopant and exact composition for a particular crystal structural framework to design a fast Li-ion conductor (Section 3.3).…”

Section: Design Principles For Fast Ion Conductorsmentioning

confidence: 99%

Computation-Accelerated Design of Materials and Interfaces for All-Solid-State Lithium-Ion Batteries

Nolan

Zhu

et al. 2018

Joule

303

230

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The all-solid-state lithium-ion battery is a promising next-generation battery technology. However, the realization of all-solid-state batteries is impeded by limited understanding of solid electrolyte materials and solid electrolyte-electrode interfaces. In this review, we present an overview of recently developed computation techniques and their applications in understanding and advancing materials and interfaces in all-solid-state batteries. We review the role of ab initio molecular dynamics simulations in studying fast ion conductors and discuss the capabilities of thermodynamic calculations powered by materials databases for identifying the chemical and electrochemical stability of solid electrolyte materials and solid electrolyte-electrode interfaces. We highlight the computational studies in the design and discovery of new solid electrolyte materials and outline design guidelines for solid electrolytes and their interfaces. We conclude with discussion of future directions in computation techniques, materials development, and interface engineering for all-solid-state lithium-ion batteries.

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Tuning mobility and stability of lithium ion conductors based on lattice dynamics

Abstract: Ionic conductivity and stability of Li-ion conductors are rationalized on the same footing using lattice-dynamics descriptors.

Cited by 199 publications

References 66 publications

Low-temperature paddlewheel effect in glassy solid electrolytes

Low-temperature paddlewheel effect in glassy solid electrolytes

High-throughput computational screening for solid-state Li-ion conductors

Computation-Accelerated Design of Materials and Interfaces for All-Solid-State Lithium-Ion Batteries

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