Experimental visualization of lithium conduction pathways in garnet-type Li7La3Zr2O12

Han, Jiantao; Zhu, Jinlong; Li, Yutao; Yu, Xiaohui; Wang, Shanmin; Wu, Gang; Xie, Hui; Vogel, Sven C.; Izumi, Fujio; Momma, Koichi; Kawamura, Yukihiko; Huang, Yunhui; Goodenough, John B; Zhao, Yusheng

doi:10.1039/c2cc35089k

Cited by 106 publications

(105 citation statements)

References 24 publications

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“…The Li-ion migration pathway is: Li(2)-Li(2 v )⋯Li(1)-Li(2 v )⋯Li(2)-Li(1 v ). Clearly, the Li-ion migration pathway in the compound via Li(1) sites did not bypass Li(1) sites, which is in agreement with experimental and theoretical studies by Goodenough et al [24]. The lithium mobility in cubic garnet is much more complex.…”

Section: Resultssupporting

confidence: 73%

Crystal structure, migration mechanism and electrochemical performance of Cr-stabilized garnet

et al. 2014

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Section: Resultssupporting

confidence: 73%

Crystal structure, migration mechanism and electrochemical performance of Cr-stabilized garnet

et al. 2014

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“…1. This insight leads to the development of the following algorithm: first, the Li nuclear density is estimated from all Li ion trajectories by binning the Li positions to cubic voxels of side length dr. We note that by taking dr = 1 Å the density pattern from the simulation matches well its experimental counterpart as obtained from diffraction35. Second, we select a local density threshold ρ to separate the various spatial regions.…”

Section: Resultsmentioning

confidence: 59%

Data mining of molecular dynamics data reveals Li diffusion characteristics in garnet Li7La3Zr2O12

Chen

Ciucci

2017

Sci Rep

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Understanding Li diffusion in solid conductors is essential for the next generation Li batteries. Here we show that density-based clustering of the trajectories computed using molecular dynamics simulations helps elucidate the Li diffusion mechanism within the Li7La3Zr2O12 (LLZO) crystal lattice. This unsupervised learning method recognizes lattice sites, is able to give the site type, and can identify Li hopping events. Results show that, while the cubic LLZO has a much higher hopping rate compared to its tetragonal counterpart, most of the Li hops in the cubic LLZO do not contribute to the diffusivity due to the dominance of back-and-forth type jumps. The hopping analysis and local Li configuration statistics give evidence that Li diffusivity in cubic LLZO is limited by the low vacancy concentration. The hopping statistics also shows uncorrelated Poisson-like diffusion for Li in the cubic LLZO, and correlated diffusion for Li in the tetragonal LLZO in the temporal scale. Further analysis of the spatio-temporal correlation using site-to-site mutual information confirms the weak site dependence of Li diffusion in the cubic LLZO as the origin for the uncorrelated diffusion. This work puts forward a perspective on combining machine learning and information theory to interpret results of molecular dynamics simulations.

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“…27 The low occupancy on the different sites and the complex distribution of Li + and vacancies across the different lithium positions leads to a critical ratio between vacancy and site occupancy of lithium; this, in combination with the high diffusion pathway degeneracy of the cubic unit cell, leads to very high ionic conductivities in these compounds. 5,7,19 …”

Section: Introductionmentioning

confidence: 99%

Structural limitations for optimizing garnet-type solid electrolytes: a perspective

Zeier

2014

Dalton Trans.

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Lithium ion batteries exhibit the highest energy densities of all battery types and are therefore an important technology for energy storage in every day life. Today's commercially available batteries employ organic polymer lithium conducting electrolytes, leading to multiple challenges and safety issues such as poor chemical stability, leakage and flammability. The next generation lithium ion batteries, namely all solid-state batteries, can overcome these limitations through employing a ceramic Li + conducting electrolyte. In the past decade, there has been a major focus on the structural and ionic transport properties of lithium-conducting garnets, and the extensive research efforts have led to a thorough understanding of the structure-property relationships in this class of materials. However, further improvement seems difficult due to structural limitations. The purpose of this Perspective article is to provide a brief structural overview of Li conducting garnets and the structural influence on the optimization of Li-ionic conductivities.

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Experimental visualization of lithium conduction pathways in garnet-type Li7La3Zr2O12

Cited by 106 publications

References 24 publications

Crystal structure, migration mechanism and electrochemical performance of Cr-stabilized garnet

Crystal structure, migration mechanism and electrochemical performance of Cr-stabilized garnet

Data mining of molecular dynamics data reveals Li diffusion characteristics in garnet Li7La3Zr2O12

Structural limitations for optimizing garnet-type solid electrolytes: a perspective

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