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

Abstract

Lithium ion conductivity in many structural families can be tuned by many orders of magnitude, with some rivaling that of liquid electrolytes at room temperature. Unfortunately, fast lithium conductors exhibit poor stability against lithium battery electrodes. In this article, we report a fundamentally new approach to alter ion mobility and stability against oxidation of lithium ion conductors using lattice dynamics. By combining inelastic neutron scattering measurements with density functional theory, fast lithium conductors were shown to have low lithium vibration frequency or low center of lithium phonon density of states. On the other hand, lowering anion phonon densities of states reduces the stability against electrochemical oxidation. Olivines with low lithium band centers but high anion band centers are promising lithium ion conductors with high ion conductivity and stability. Such findings highlight new strategies in controlling lattice dynamics to discover new lithium ion conductors with enhanced conductivity and stability.

Authors:
 [1];  [1]; ORCiD logo [2];  [1]; ORCiD logo [3];  [3];  [4];  [5];  [5]; ORCiD logo [6];  [6];  [6]; ORCiD logo [1]
  1. Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
  2. Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States); Univ. di Milano-Bicocca, Milano (Italy)
  3. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  4. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Duke Univ., Durham, NC (United States)
  5. Tokyo Inst. of Technology, Yokohama (Japan)
  6. BMW Group, Munich (Germany)
Publication Date:
Research Org.:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC); Univ. of California, Oakland, CA (United States); Duke Univ., Durham, NC (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division; USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1493940
Alternate Identifier(s):
OSTI ID: 1543789
Grant/Contract Number:  
AC02-05CH11231; SC0016166
Resource Type:
Published Article
Journal Name:
Energy & Environmental Science
Additional Journal Information:
Journal Volume: 11; Journal Issue: 4; Journal ID: ISSN 1754-5692
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; Chemistry; Energy & Fuels; Engineering; Environmental Sciences & Ecology

Citation Formats

Muy, Sokseiha, Bachman, John C., Giordano, Livia, Chang, Hao -Hsun, Abernathy, Douglas L., Bansal, Dipanshu, Delaire, Olivier, Hori, Satoshi, Kanno, Ryoji, Maglia, Filippo, Lupart, Saskia, Lamp, Peter, and Shao-Horn, Yang. Tuning mobility and stability of lithium ion conductors based on lattice dynamics. United States: N. p., 2018. Web. doi:10.1039/c7ee03364h.
Muy, Sokseiha, Bachman, John C., Giordano, Livia, Chang, Hao -Hsun, Abernathy, Douglas L., Bansal, Dipanshu, Delaire, Olivier, Hori, Satoshi, Kanno, Ryoji, Maglia, Filippo, Lupart, Saskia, Lamp, Peter, & Shao-Horn, Yang. Tuning mobility and stability of lithium ion conductors based on lattice dynamics. United States. doi:10.1039/c7ee03364h.
Muy, Sokseiha, Bachman, John C., Giordano, Livia, Chang, Hao -Hsun, Abernathy, Douglas L., Bansal, Dipanshu, Delaire, Olivier, Hori, Satoshi, Kanno, Ryoji, Maglia, Filippo, Lupart, Saskia, Lamp, Peter, and Shao-Horn, Yang. Tue . "Tuning mobility and stability of lithium ion conductors based on lattice dynamics". United States. doi:10.1039/c7ee03364h.
@article{osti_1493940,
title = {Tuning mobility and stability of lithium ion conductors based on lattice dynamics},
author = {Muy, Sokseiha and Bachman, John C. and Giordano, Livia and Chang, Hao -Hsun and Abernathy, Douglas L. and Bansal, Dipanshu and Delaire, Olivier and Hori, Satoshi and Kanno, Ryoji and Maglia, Filippo and Lupart, Saskia and Lamp, Peter and Shao-Horn, Yang},
abstractNote = {Lithium ion conductivity in many structural families can be tuned by many orders of magnitude, with some rivaling that of liquid electrolytes at room temperature. Unfortunately, fast lithium conductors exhibit poor stability against lithium battery electrodes. In this article, we report a fundamentally new approach to alter ion mobility and stability against oxidation of lithium ion conductors using lattice dynamics. By combining inelastic neutron scattering measurements with density functional theory, fast lithium conductors were shown to have low lithium vibration frequency or low center of lithium phonon density of states. On the other hand, lowering anion phonon densities of states reduces the stability against electrochemical oxidation. Olivines with low lithium band centers but high anion band centers are promising lithium ion conductors with high ion conductivity and stability. Such findings highlight new strategies in controlling lattice dynamics to discover new lithium ion conductors with enhanced conductivity and stability.},
doi = {10.1039/c7ee03364h},
journal = {Energy & Environmental Science},
number = 4,
volume = 11,
place = {United States},
year = {2018},
month = {2}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
DOI: 10.1039/c7ee03364h

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Cited by: 18 works
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