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Insights into Soft Short Circuit-based Degradation of Lithium Metal Batteries

Published version
Peer-reviewed

Repository DOI


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Authors

Larner, Rebecca 
Choi, Yoonseong 

Abstract

The demand for an extended range of electric vehicles has created a renaissance of interest in replacing the common metal-ion with higher energy-density metal-anode batteries. However, the potential battery safety issues associated with lithium metal cell use must be addressed to enable lithium metal battery chemistries. A considerable performance gap between lithium (Li) symmetric cells and practical Li batteries motivated us to explore the correlation between the shape of voltage traces and degradation. We coupled impedance spectroscopy and operando NMR and used the new approach to show that transient (i.e., soft) shorts form in realistic conditions for battery applications; however, they are typically overlooked, as their electrochemical signatures are often not distinct. The typical rectangular-shaped voltage trace, widely considered ideal, was proven, under the conditions studied here, to be a result of soft shorts. Recoverable soft-shorted cells were demonstrated during a symmetric cell polarisation experiment, defining a new type of critical current density, the current density at which the soft shorts are not reversible. Moreover, we demonstrated that soft shorts, detected via electrochemical impedance spectroscopy (EIS) and validated via operando NMR, are predictive towards the formation of hard shorts, showing the potential use of EIS as a relatively low-cost and non-destructive method for early detection of catastrophic shorts and battery failure while demonstrating the strength of operando NMR as a research tool for metal plating in lithium batteries.

Description

Acknowledgements: JBF and SM gratefully acknowledge funding by the Faraday Institute through the LiSTAR (FIRG014, FIRG058) and NEXGENNa (FIRG018). CPG acknowledges support from an ERC Advanced Investigator Grant (EC H2020 ERC 835073) and a Royal Society Research Professorship (RP\R1\180147).

Keywords

34 Chemical Sciences, 3406 Physical Chemistry, 7 Affordable and Clean Energy

Journal Title

Faraday Discussions

Conference Name

Journal ISSN

1359-6640
1364-5498

Volume Title

Publisher

Royal Society of Chemistry
Sponsorship
Faraday Institution (via University Of St Andrews) (NEXGENNA)
Faraday Institution (NEXGenna)
Faraday Institution (via University Of St Andrews) (NEXGenna)
Royal Society (RP/R1/180147)
European Commission Horizon 2020 (H2020) ERC (835073)
JBF and SM gratefully acknowledge funding by the Faraday Institute through the LiSTAR (FIRG014, FIRG058) and NEXGENNa (FIRG018). C.P.G. acknowledges support from an ERC Advanced Investigator Grant (EC H2020 ERC 835073) and a Royal Society Research Professorship (RP\R1\180147).