Li1.5La1.5MO6 (M = W6+, Te6+) as a new series of lithium-rich double perovskites for all-solid-state lithium-ion batteries

Marco Amores; Hany El-Shinawi; Innes McClelland; Stephen R Yeandel; Peter J Baker; Ronald I Smith; Helen Y Playford; Pooja Goddard; Serena A Corr; Edmund J Cussen

doi:10.1038/s41467-020-19815-5

Li_1.5La_1.5MO₆ (M = W⁶⁺, Te⁶⁺) as a new series of lithium-rich double perovskites for all-solid-state lithium-ion batteries

Nat Commun. 2020 Dec 15;11(1):6392. doi: 10.1038/s41467-020-19815-5.

Authors

Marco Amores¹, Hany El-Shinawi^{1

2}, Innes McClelland¹, Stephen R Yeandel³, Peter J Baker⁴, Ronald I Smith⁴, Helen Y Playford⁴, Pooja Goddard³, Serena A Corr^{5

6}, Edmund J Cussen^{7

8}

Affiliations

¹ Department of Chemical and Biological Engineering, University of Sheffield, Sheffield, S1 3JD, UK.
² The Faraday Institution, Harwell Campus, Didcot, OX1 0RA, UK.
³ Department of Chemistry, Loughborough University, Epinal Way, Loughborough, LE11 3TU, UK.
⁴ ISIS Pulsed Neutron and Muon Source, STFC Rutherford Appleton Laboratory, Harwell Science and Innovation Campus, Didcot, Oxfordshire, OX11 0QX, UK.
⁵ Department of Chemical and Biological Engineering, University of Sheffield, Sheffield, S1 3JD, UK. s.corr@sheffield.ac.uk.
⁶ Department of Materials Science and Engineering, University of Sheffield, Sheffield, S1 3JD, UK. s.corr@sheffield.ac.uk.
⁷ Department of Chemical and Biological Engineering, University of Sheffield, Sheffield, S1 3JD, UK. e.j.cussen@sheffield.ac.uk.
⁸ Department of Materials Science and Engineering, University of Sheffield, Sheffield, S1 3JD, UK. e.j.cussen@sheffield.ac.uk.

Abstract

Solid-state batteries are a proposed route to safely achieving high energy densities, yet this architecture faces challenges arising from interfacial issues between the electrode and solid electrolyte. Here we develop a novel family of double perovskites, Li_1.5La_1.5MO₆ (M = W⁶⁺, Te⁶⁺), where an uncommon lithium-ion distribution enables macroscopic ion diffusion and tailored design of the composition allows us to switch functionality to either a negative electrode or a solid electrolyte. Introduction of tungsten allows reversible lithium-ion intercalation below 1 V, enabling application as an anode (initial specific capacity >200 mAh g^-1 with remarkably low volume change of ∼0.2%). By contrast, substitution of tungsten with tellurium induces redox stability, directing the functionality of the perovskite towards a solid-state electrolyte with electrochemical stability up to 5 V and a low activation energy barrier (<0.2 eV) for microscopic lithium-ion diffusion. Characterisation across multiple length- and time-scales allows interrogation of the structure-property relationships in these materials and preliminary examination of a solid-state cell employing both compositions suggests lattice-matching avenues show promise for all-solid-state batteries.