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Title: High-Throughput Screening of Solid-State Li-Ion Conductors Using Lattice-Dynamics Descriptors

Abstract

Low lithium-ion migration barriers have recently been associated with low average vibrational frequencies or phonon band centers, further helping identify descriptors for superionic conduction. To further explore this correlation, here we present the computational screening of ~14,000 Li-containing compounds in the Materials Project database using a descriptor based on lattice dynamics reported recently to identify new promising Li-ion conductors. An efficient computational approach was optimized to compute the average vibrational frequency or phonon band center of ~1,200 compounds obtained after pre-screening based on structural stability, band gap, and their composition. Combining a low computed Li phonon band center with large computed electrochemical stability window and structural stability, 18 compounds were predicted to be promising Li-ion conductors, one of which, Li3ErCl6, has been synthesized and exhibits a reasonably high room-temperature conductivity of 0.05–0.3 mS/cm, which shows the promise of Li-ion conductor discovery based on lattice dynamics.

Authors:
ORCiD logo; ; ; ; ; ; ; ;
Publication Date:
Research Org.:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC); SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division; German Research Foundation (DFG)
OSTI Identifier:
1530007
Alternate Identifier(s):
OSTI ID: 1623679
Grant/Contract Number:  
AC02-05CH11231; AC02-76SF00515; ZE 1010/4-1
Resource Type:
Published Article
Journal Name:
iScience
Additional Journal Information:
Journal Name: iScience Journal Volume: 16 Journal Issue: C; Journal ID: ISSN 2589-0042
Publisher:
Elsevier
Country of Publication:
Netherlands
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Science & Technology - Other Topics; Computational Method in Materials Science; Energy Materials; Solid State Physics

Citation Formats

Muy, Sokseiha, Voss, Johannes, Schlem, Roman, Koerver, Raimund, Sedlmaier, Stefan J., Maglia, Filippo, Lamp, Peter, Zeier, Wolfgang G., and Shao-Horn, Yang. High-Throughput Screening of Solid-State Li-Ion Conductors Using Lattice-Dynamics Descriptors. Netherlands: N. p., 2019. Web. doi:10.1016/j.isci.2019.05.036.
Muy, Sokseiha, Voss, Johannes, Schlem, Roman, Koerver, Raimund, Sedlmaier, Stefan J., Maglia, Filippo, Lamp, Peter, Zeier, Wolfgang G., & Shao-Horn, Yang. High-Throughput Screening of Solid-State Li-Ion Conductors Using Lattice-Dynamics Descriptors. Netherlands. https://doi.org/10.1016/j.isci.2019.05.036
Muy, Sokseiha, Voss, Johannes, Schlem, Roman, Koerver, Raimund, Sedlmaier, Stefan J., Maglia, Filippo, Lamp, Peter, Zeier, Wolfgang G., and Shao-Horn, Yang. Wed . "High-Throughput Screening of Solid-State Li-Ion Conductors Using Lattice-Dynamics Descriptors". Netherlands. https://doi.org/10.1016/j.isci.2019.05.036.
@article{osti_1530007,
title = {High-Throughput Screening of Solid-State Li-Ion Conductors Using Lattice-Dynamics Descriptors},
author = {Muy, Sokseiha and Voss, Johannes and Schlem, Roman and Koerver, Raimund and Sedlmaier, Stefan J. and Maglia, Filippo and Lamp, Peter and Zeier, Wolfgang G. and Shao-Horn, Yang},
abstractNote = {Low lithium-ion migration barriers have recently been associated with low average vibrational frequencies or phonon band centers, further helping identify descriptors for superionic conduction. To further explore this correlation, here we present the computational screening of ~14,000 Li-containing compounds in the Materials Project database using a descriptor based on lattice dynamics reported recently to identify new promising Li-ion conductors. An efficient computational approach was optimized to compute the average vibrational frequency or phonon band center of ~1,200 compounds obtained after pre-screening based on structural stability, band gap, and their composition. Combining a low computed Li phonon band center with large computed electrochemical stability window and structural stability, 18 compounds were predicted to be promising Li-ion conductors, one of which, Li3ErCl6, has been synthesized and exhibits a reasonably high room-temperature conductivity of 0.05–0.3 mS/cm, which shows the promise of Li-ion conductor discovery based on lattice dynamics.},
doi = {10.1016/j.isci.2019.05.036},
journal = {iScience},
number = C,
volume = 16,
place = {Netherlands},
year = {Wed May 29 00:00:00 EDT 2019},
month = {Wed May 29 00:00:00 EDT 2019}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
https://doi.org/10.1016/j.isci.2019.05.036

Citation Metrics:
Cited by: 120 works
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Figures / Tables:

Figure 1 Figure 1: Schematic of the HT Screening as well as Various Correlations Studied in This Work. Electronic and phonon-related descriptors were shown to correlate with the migration barrier Em and electrochemical stability of lithium-ion conductors. Data points in red correspond to oxides, whereas those in brown correspond to sulfides andmore » were taken from previous work (Muy et al., 2018b).« less

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