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

Sokseiha Muy; Johannes Voss; Roman Schlem; Raimund Koerver; Stefan J Sedlmaier; Filippo Maglia; Peter Lamp; Wolfgang G Zeier; Yang Shao-Horn

doi:10.1016/j.isci.2019.05.036

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

iScience. 2019 Jun 28:16:270-282. doi: 10.1016/j.isci.2019.05.036. Epub 2019 May 29.

Authors

Sokseiha Muy¹, Johannes Voss², Roman Schlem³, Raimund Koerver⁴, Stefan J Sedlmaier⁴, Filippo Maglia⁴, Peter Lamp⁴, Wolfgang G Zeier³, Yang Shao-Horn⁵

Affiliations

¹ Research Laboratory of Electronics, Massachusetts Institute of Technology, Cambridge, MA 02139, USA. Electronic address: sokseiha@mit.edu.
² SUNCAT Center for Interface Science and Catalysis, SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, CA 94025, USA. Electronic address: vossj@slac.stanford.edu.
³ Institute of Physical Chemistry & Center for Materials Research, Justus-Liebig-University Giessen, Heinrich-Buff-Ring 17, 35392 Giessen, Germany.
⁴ Research Battery Technology, BMW Group, 80788 Munich, Germany.
⁵ Research Laboratory of Electronics, Massachusetts Institute of Technology, Cambridge, MA 02139, USA; Department of Materials Science and Engineering, Massachusetts Institute of Technology, Cambridge, MA 02139, USA.

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.

Keywords: Computational Method in Materials Science; Energy Materials; Solid State Physics.