In Situ Diffusion Measurements of a NASICON-Structured All-Solid-State Battery Using Muon Spin Relaxation

Innes McClelland; Samuel G Booth; Hany El-Shinawi; Beth I J Johnston; Jasmin Clough; Weimin Guo; Edmund J Cussen; Peter J Baker; Serena A Corr

doi:10.1021/acsaem.0c02722

In Situ Diffusion Measurements of a NASICON-Structured All-Solid-State Battery Using Muon Spin Relaxation

ACS Appl Energy Mater. 2021 Feb 22;4(2):1527-1536. doi: 10.1021/acsaem.0c02722. Epub 2021 Jan 21.

Authors

Innes McClelland^{1

2

3}, Samuel G Booth^{1

3}, Hany El-Shinawi^{1

3}, Beth I J Johnston^{1

3}, Jasmin Clough^{4

3}, Weimin Guo¹, Edmund J Cussen^{4

3}, Peter J Baker^{2

3}, Serena A Corr^{1

3}

Affiliations

¹ Department of Chemical and Biological Engineering, The University of Sheffield, Sheffield, S1 3JD, U.K.
² ISIS Neutron and Muon Source, Science and Technology Facilities Council, Rutherford Appleton Laboratory, Harwell Campus, Didcot, OX11 0QX, U.K.
³ The Faraday Institution, Quad One, Harwell Campus, Didcot, OX11 0RA, U.K.
⁴ Department of Materials Science and Engineering, The University of Sheffield, Sheffield, S1 3JD, U.K.

Abstract

In situ muon spin relaxation is demonstrated as an emerging technique that can provide a volume-averaged local probe of the ionic diffusion processes occurring within electrochemical energy storage devices as a function of state of charge. Herein, we present work on the conceptually interesting NASICON-type all-solid-state battery LiM₂(PO₄)₃, using M = Ti in the cathode, M = Zr in the electrolyte, and a Li metal anode. The pristine materials are studied individually and found to possess low ionic hopping activation energies of ∼50-60 meV and competitive Li⁺ self-diffusion coefficients of ∼10^-10-10^-9 cm² s^-1 at 336 K. Lattice matching of the cathode and electrolyte crystal structures is employed for the all-solid-state battery to enhance Li⁺ diffusion between the components in an attempt to minimize interfacial resistance. The cell is examined by in situ muon spin relaxation, providing the first example of such ionic diffusion measurements. This technique presents an opportunity to the materials community to observe intrinsic ionic dynamics and electrochemical behavior simultaneously in a nondestructive manner.