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

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posted on 21.12.2020, 10:16 by Marco Amores, Hany El-Shinawi, Innes McClelland, Stephen R Yeandel, Peter J Baker, Ronald I Smith, Helen Y Playford, Pooja GoddardPooja Goddard, Serena A Corr, Edmund J Cussen
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, Li1.5La1.5MO6 (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.

Funding

Design and high throughput microwave synthesis of Li-ion battery materials

Engineering and Physical Sciences Research Council

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Faraday Institution (SOLBAT, Grant No. FIRG007)

MATERIALS CHEMISTRY HIGH END COMPUTING CONSORTIUM

Engineering and Physical Sciences Research Council

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HIGH END COMPUTING MATERIALS CHEMISTRY CONSORTIUM

Engineering and Physical Sciences Research Council

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Proposal for a Tier 2 Centre - HPC Midlands Plus

Engineering and Physical Sciences Research Council

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History

School

  • Science

Department

  • Chemistry

Published in

Nature Communications

Volume

11

Issue

1

Publisher

Nature Research

Version

VoR (Version of Record)

Rights holder

© The Authors

Publisher statement

This is an Open Access Article. It is published by Nature Research under the Creative Commons Attribution 4.0 International Licence (CC BY 4.0). Full details of this licence are available at: https://creativecommons.org/licenses/by/4.0/

Acceptance date

27/10/2020

Publication date

2020-12-15

Copyright date

2020

ISSN

2041-1723

eISSN

2041-1723

Language

en

Depositor

Dr Pooja Goddard. Deposit date: 19 December 2020

Article number

6392