Skip to main content
U.S. flag

An official website of the United States government

Official websites use .gov
A .gov website belongs to an official government organization in the United States.

Secure .gov websites use HTTPS
A lock ( ) or https:// means you’ve safely connected to the .gov website. Share sensitive information only on official, secure websites.

Stacking Faults Assist Lithium-Ion Conduction in a Halide-Based Superionic Conductor

Published

Author(s)

Elias Sebti, Hayden Evans, Hengning Chen, Peter Richardson, Kelly White, Raynald Giovine, Krishna P. Koirala, Yaobin Xu, Eliovardo Gonzalez-Correa, Chongmin Wang, Craig Brown, Anthony Cheetham, Pieremanuele Canepa, Raphaele Clement

Abstract

In the pursuit of urgently-needed, energy dense solid-state batteries for electric vehicle and portable electronics applications, halide solid electrolytes offer a promising path forward with exceptional compatibility against high-voltage oxide electrodes, tunable ionic conductivities, and facile processing. For this family of compounds, synthesis protocols strongly affect cation site disorder and modulate Li+ mobility. In this work, we reveal the presence of a high concentration of stacking faults in the superionic conductor Li3YCl6 and demonstrate a method of controlling its Li+ conductivity by tuning the defect concentration with synthesis and heat treatments at select temperatures. Leveraging complementary insights from variable temperature synchrotron X-ray diffraction, neutron diffraction, solid-state nuclear magnetic resonance, density functional theory, and electrochemical impedance spectroscopy, we identify the nature of planar defects and the role of nonstoichiometry in lowering Li+ migration barriers and increasing Li site connectivity in mechanochemically-synthesized Li3YCl6 . We harness paramagnetic relaxation enhancement to enable 89Y solid-state NMR, and directly contrast the Y-cation site disorder resulting from different preparation methods, demonstrating a potent tool for other researchers studying Y-containing compositions. With heat treatments at temperatures as low as 333 K (60°C), we decrease the concentration of planar defects, demonstrating a simple method for tuning the Li+ conductivity. Findings from this work are expected to be generalizable to other halide solid electrolyte candidates and provide an improved understanding of defect-enabled Li+ conduction in this class of Li-ion conductors.
Citation
Journal of the American Chemical Society
Volume
144
Issue
13

Keywords

Stacking Faults, Ion Conductor, diffraction, solid-state battery

Citation

Sebti, E. , Evans, H. , Chen, H. , Richardson, P. , White, K. , Giovine, R. , Koirala, K. , Xu, Y. , Gonzalez-Correa, E. , Wang, C. , Brown, C. , Cheetham, A. , Canepa, P. and Clement, R. (2022), Stacking Faults Assist Lithium-Ion Conduction in a Halide-Based Superionic Conductor, Journal of the American Chemical Society (Accessed July 12, 2024)

Issues

If you have any questions about this publication or are having problems accessing it, please contact reflib@nist.gov.

Created April 5, 2022, Updated November 29, 2022