Elucidating the nature of grain boundary resistance in lithium lanthanum titanate

Adam R. Symington; Marco Molinari; James A. Dawson; Joel M. Statham; John Purton; Pieremanuele Canepa; Stephen C. Parker

doi:10.1039/d0ta11539h

Elucidating the nature of grain boundary resistance in lithium lanthanum titanate

Adam R. Symington, Marco Molinari, James A. Dawson, Joel M. Statham, John Purton, Pieremanuele Canepa, Stephen C. Parker

Research output: Contribution to journal › Article › peer-review

49 Citations (SciVal)

Abstract

Solid electrolytes for all-solid-state batteries are generating remarkable research interest as a means to improve the safety, stability and performance of rechargeable batteries. Solid electrolytes are often polycrystalline and the effect that grain boundaries have on the material properties is often not fully characterised. Here, we present a comprehensive molecular dynamics study that quantifies the effect of grain boundaries on Li-ion transport in perovskite Li_3xLa_(2/3)−xTiO₃(0 <x< 0.16) (LLTO). Our results predict that grain boundaries hinder Li-ion conductivity by 1 to 2 orders of magnitude compared to the bulk. We attribute the poor Li-ion conductivity of the grain boundaries to significant structural alterations at the grain boundaries. Our detailed analysis provides important insight into the influence of grain boundary structure on transport of Li-ions in solid electrolyte materials.

Original language	English
Pages (from-to)	6487-6498
Number of pages	12
Journal	Journal of Materials Chemistry A
Volume	9
Issue number	10
Early online date	29 Jan 2021
DOIs	https://doi.org/10.1039/d0ta11539h
Publication status	Published - 14 Mar 2021

Bibliographical note

Funding Information:
Computations were run on Balena HPC facility at the University of Bath and the ARCHER UK National Supercomputing Service via our membership of the High-End Computing Materials Chemistry Consortium (HEC MCC) funded by the EPSRC (EP/ L000202, EP/R029431). We are grateful to the UK Materials and Molecular Modelling Hub for computational resources, which is partially funded by the EPSRC (EP/P020194/1). P. C. acknowledges funding from the National Research Foundation under his NRF Fellowship NRFF12-2020-0012 and the ANR-NRF NRF2019-NRF-ANR073 Na-MASTER. The Monte Carlo calculations used computing resources provided by STFC Scientic Computing Department's SCARF cluster.

Funding

Computations were run on Balena HPC facility at the University of Bath and the ARCHER UK National Supercomputing Service via our membership of the High-End Computing Materials Chemistry Consortium (HEC MCC) funded by the EPSRC (EP/ L000202, EP/R029431). We are grateful to the UK Materials and Molecular Modelling Hub for computational resources, which is partially funded by the EPSRC (EP/P020194/1). P. C. acknowledges funding from the National Research Foundation under his NRF Fellowship NRFF12-2020-0012 and the ANR-NRF NRF2019-NRF-ANR073 Na-MASTER. The Monte Carlo calculations used computing resources provided by STFC Scientic Computing Department's SCARF cluster.

ASJC Scopus subject areas

General Chemistry
Renewable Energy, Sustainability and the Environment
General Materials Science

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

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10.1039/d0ta11539hLicence: CC BY-NC

Cite this

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abstract = "Solid electrolytes for all-solid-state batteries are generating remarkable research interest as a means to improve the safety, stability and performance of rechargeable batteries. Solid electrolytes are often polycrystalline and the effect that grain boundaries have on the material properties is often not fully characterised. Here, we present a comprehensive molecular dynamics study that quantifies the effect of grain boundaries on Li-ion transport in perovskite Li3xLa(2/3)−xTiO3(0 ",

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Elucidating the nature of grain boundary resistance in lithium lanthanum titanate

Abstract

Bibliographical note

Funding

ASJC Scopus subject areas

UN SDGs

Access to Document

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Critical mass application on emergent nanomaterials

Cite this

Elucidating the nature of grain boundary resistance in lithium lanthanum titanate

Abstract

Bibliographical note

Funding

ASJC Scopus subject areas

UN SDGs

Access to Document

Other files and links

Fingerprint

Projects

Critical mass application on emergent nanomaterials

Cite this