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

• Main Authors: Abernathy, Douglas L. (Author), Bansal, Dipanshu (Author), Delaire, Olivier (Author), Hori, Satoshi (Author), Kanno, Ryoji (Author), Maglia, Filippo (Author), Lupart, Saskia (Author), Lamp, Peter (Author), Muy, Sokseiha (Contributor), Bachman, Chris (Contributor), Giordano, Livia (Contributor), Chang, Hao Hsun (Contributor), Shao-Horn, Yang (Contributor)
• Other Authors: Massachusetts Institute of Technology. Department of Materials Science and Engineering (Contributor), Massachusetts Institute of Technology. Department of Mechanical Engineering (Contributor), Massachusetts Institute of Technology. Research Laboratory of Electronics (Contributor)
• Format: Article
• Language: English
• Published: Royal Society of Chemistry, 2019-03-22T21:17:18Z.
• Subjects: Article
• Online Access: Get fulltext

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.
United States. National Science Foundation. Graduate Research Fellowship Program (Grant 1122374)
Taiwan. Ministry of Science and Technology (Grant 102-2917-I-564-006-A1)
United States. National Science Foundation (Award DMR-0819762)
United States. National Energy Research Scientific Computing Center (Contract DE-AC02-05CH11231)
Extreme Science and Engineering Discovery Environment (Grant ACI-1548562)