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

Kahle, Leonid; Marcolongo, Aris; Marzari, Nicola

doi:10.1039/c9ee02457c

Cited by 119 publications

(120 citation statements)

References 277 publications

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“…First-principles computation studies have led to significant progresses in understanding Li-ion diffusion mechanisms and in designing and predicting new SIC materials. [20,26,28,34,35] In this study, we perform a systematic first-principles computational study on lithium metal chloride systems spanning a wide range of Li/cation concentrations and configurations to understand the key factors determining fast Li-ion diffusion in these chloride systems. Using first-principles calculations, we study Li-ion diffusion in over 70 Li-containing chlorides from the Inorganic Crystal Structure Database (ICSD) and identify 19 materials as potential Li-ion conductors.…”

Section: Introductionmentioning

confidence: 99%

Tailoring the Cation Lattice for Chloride Lithium‐Ion Conductors

Liu

Wang

Nolan

et al. 2020

Advanced Energy Materials

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Only a limited number of materials systems have been demonstrated as Li SICs, including Li 10 GeP 2 S 12 (LGPS), [4] garnet Li 7 La 3 Zr 2 O 12 (LLZO), [9,10] and NASICON Li 1.3 Al 0.3 Ti 1.7 (PO 4) 3 (LATP). [11] However, these Li SICs do not have all properties required for ASSLBs. Compared to oxide SICs, sulfide SICs have desired mechanical deformability for forming good interface physical contacts in ASSLB cell assembly, but have narrow electrochemical window, [12,13] poor cathode interface compatibility, [14-16] and poor air/ moisture stability, [5,17] which impede the large-scale commercialization of sulfidebased ASSLBs. Asano et al. discovered Li 3 YCl 6 (LYC) and Li 3 YBr 6 (LYB) as new Li SICs with high Li-ion conductivities on the order of 1 mS cm −1 at RT and with good ASSLB cell performances. [18] In addition to the desired deformable mechanical properties as sulfides, first-principles computation studies [17,19] confirmed that the chloride chemistry in general gives a lower barrier for Li-ion migration, wider electrochemical window, good interface compatibility with cathode, and good air/moisture stability compared to sulfide SEs. With a combination of multiple desired properties, lithium halides, particularly chlorides, are a promising class of Li SICs for SEs in ASSLBs. The chloride anion chemistry is advantageous for Li-ion migration, thanks to the relatively large anion radius, large anion polarizability, and weak interaction with Li-ion. [18-20] Firstprinciples computation confirms that Li-ion migration exhibits a low energy barrier of 0.28 eV in face-centered cubic (fcc) and of 0.29 eV in hexagonal close packed (hcp) Cl − anion sublattices with no cation under typical lattice volume of lithium chlorides. [19] Recent experimental studies reported a series of Licontaining chlorides Li 3 MCl 6 (M = In, Er, Sc) and their doped variations that achieved Li-ion conductivities on the order of 1 mS cm −1 at RT. [19,21-25] While the discovery of new SIC systems in oxides and sulfides is greatly limited by the unique crystal structures required for achieving fast Li-ion conduction, [26-28] Li-containing chlorides with common fcc and hcp anion sublattices exhibit adequately low Li-ion migration barrier, and are a promising chemical space for new Li-ion conductors. A systematic fundamental understanding of chloride Li-ion conductors is essential for guiding the discovery and design new Li-containing chloride SICs. While Li-containing chlorides are common in close-packed fcc and hcp anion sublattices, they All-solid-state Li-ion batteries require Li-ion conductors as solid electrolytes (SEs). Li-containing halides are emerging as a promising class of lithium-ion conductors with good electrochemical stability and other properties needed for SEs in all-solid-state batteries. Compared to oxides and sulfides, Li-ion diffusion mechanisms in Li-containing halides are less well understood, in particular regarding the effects of Li content and cation sublattices, which can be tailored for improving Li-ion conduction...

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Section: Introductionmentioning

confidence: 99%

Tailoring the Cation Lattice for Chloride Lithium‐Ion Conductors

Liu

Wang

Nolan

et al. 2020

Advanced Energy Materials

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“…The 187 trials were constructed as every possible combination of the tested values for each 188 parameter, which are listed below. This high-throughput highly parallel methodology is 189 primarily inspired by high-throughput virtual screening and optimization efforts in 190 materials science such as [57] and [58]. Similar methods have also attained prominence 191 in proteomics, computational chemistry, pharmacology, and many other fields.…”

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confidence: 99%

High-throughput simulations indicate feasibility of navigation by familiarity with a local sensor such as scorpion pectines

Musaelian

Gaffin

2020

Preprint

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Scorpions have arguably the most elaborate "tongues" on the planet: two paired ventral combs, called pectines, that are covered in thousands of chemo-tactile peg sensilla and that sweep the ground as the animal walks. Males use their pectines to detect female pheromones during the mating season, but females have pectines too: What additional purpose must the pectines serve? Why are there so many pegs? We take a computational approach to test the hypothesis that scorpions use their pectines to navigate by chemo-textural familiarity in a manner analogous to the visual navigation-by-scene-familiarity hypothesis for hymenopteran insects. We have developed a general model of navigation by familiarity with a local sensor and have chosen a range of plausible parameters for it based on the existing behavioral, physiological, morphological, and neurological understanding of the pectines. Similarly, we constructed virtual environments based on the scorpion's native sand habitat. Using a novel methodology of highly parallel high-throughput simulations, we comprehensively tested 2160 combinations of sensory and environmental properties in each of 24 different situations, giving a total of 51,840 trials. Our results show that navigation by familiarity with a local pectine-like sensor is feasible. Further, they suggest a subtle interplay between "complexity" and "continuity" in navigation by familiarity and give June 10, 2020 1/34 the surprising result that more complexity -more detail and more information -is not always better for navigational performance. Author summaryScorpions' pectines are intricate taste-and-touch sensory appendages that brush the ground as the animal walks. Pectines are involved in detecting pheromones, but their exquisite complexity -a pair of pectines can have around 100,000 sensory neuronssuggests that they do more. One hypothesis is "Navigation by Scene Familiarity," which explains how bees and ants use their compound eyes to navigate home: the insect visually scans side to side as it moves, compares what it sees to scenes learned along a training path, and moves in the direction that looks most familiar. We propose that the scorpions' pectines can be used to navigate similarly: instead of looking around, they sweep side to side sensing local chemical and textural information. We crafted simulated scorpions based on current understanding of the pectines and tested their navigational performance in virtual versions of the animals' sandy habitat. Using a supercomputer, we varied nine environmental, sensory, and situational properties and ran a total of 51,840 trials of simulated navigation. We showed that navigation by familiarity with a local sensor like the pectines is feasible. Surprisingly, we also found that having a more detailed landscape and/or a more sensitive sensor is not always optimal.Introduction 1 Scorpions present at least two unanswered scientific mysteries: the selection pressure 2 that maintains their pectines -two ornate, sensitive, and energetically expensive 3 sensory organs on t...

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“…Thanks to these efforts, AiiDA has seen a rise in its use and adoption for research projects [14][15][16][17][18][36][37][38][39][40][41][42][43] (see also aiida.net/science for a more complete overview of recently published work that has employed AiiDA). The community of plugin developers has also grown substantially and as of May 2020 the plugin registry (see "The Plugin System") hosts 49 plugin packages, including for BigDFT 44 , CASTEP 45 , CP2K 46 , CRYSTAL 47 , FLEUR (flapw.de), Gaussian 48 , GULP 49 , Phonopy 50 , Quantum ESPRESSO 21 , Raspa 51 , Siesta 52 , VASP 22 , Wannier90 53 , Yambo 54 and many more.…”

Section: Code Quality Testing and Continuous Integrationmentioning

confidence: 99%

AiiDA 1.0, a scalable computational infrastructure for automated reproducible workflows and data provenance

et al. 2020

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The ever-growing availability of computing power and the sustained development of advanced computational methods have contributed much to recent scientific progress. These developments present new challenges driven by the sheer amount of calculations and data to manage. Next-generation exascale supercomputers will harden these challenges, such that automated and scalable solutions become crucial. In recent years, we have been developing AiiDA (aiida.net), a robust open-source high-throughput infrastructure addressing the challenges arising from the needs of automated workflow management and data provenance recording. Here, we introduce developments and capabilities required to reach sustained performance, with AiiDA supporting throughputs of tens of thousands processes/hour, while automatically preserving and storing the full data provenance in a relational database making it queryable and traversable, thus enabling high-performance data analytics. AiiDA’s workflow language provides advanced automation, error handling features and a flexible plugin model to allow interfacing with external simulation software. The associated plugin registry enables seamless sharing of extensions, empowering a vibrant user community dedicated to making simulations more robust, user-friendly and reproducible.

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

Cited by 119 publications

References 277 publications

Tailoring the Cation Lattice for Chloride Lithium‐Ion Conductors

Tailoring the Cation Lattice for Chloride Lithium‐Ion Conductors

High-throughput simulations indicate feasibility of navigation by familiarity with a local sensor such as scorpion pectines

AiiDA 1.0, a scalable computational infrastructure for automated reproducible workflows and data provenance

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