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Insights into Multiphase Reactions during Self-Discharge of Li-S Batteries

Wen, G; Rehman, S; Tranter, TG; Ghosh, D; Chen, Z; Gostick, JT; Pope, MA; (2020) Insights into Multiphase Reactions during Self-Discharge of Li-S Batteries. Chemistry of Materials , 32 (11) pp. 4518-4526. 10.1021/acs.chemmater.0c00235. Green open access

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Abstract

Lithium-sulfur (Li-S) batteries are promising next-generation rechargeable energy storage systems due to their high energy density and use of abundant and inexpensive materials. However, rapid self-discharge and poor cycling stability due to the solubility of intermediate polysulfide conversion products have slowed their commercialization. Herein, we provide a detailed account of the multiphasic reactions occurring during the self-discharge of a Li-S battery held at various depth of discharge (DOD) through both simulation and experiment. For the first time, self-discharge of a full Li-S battery is simulated using a 1D model to describe reactions at both the anode and cathode. The model accurately describes experimentally derived results obtained over the longest durations of self-discharge studied to date (140 h). This validated model was used to follow the reversible and irreversible capacity loss caused by shuttling and precipitation of insoluble Li2S2 and Li2S as a function of DOD. While the most rapid self-discharge is observed at low DOD, this also leads to the smallest irreversible loss. The results suggest that resting a Li-S battery near 2.1 V minimizes both reversible and irreversible losses.

Type: Article
Title: Insights into Multiphase Reactions during Self-Discharge of Li-S Batteries
Open access status: An open access version is available from UCL Discovery
DOI: 10.1021/acs.chemmater.0c00235
Publisher version: https://doi.org/10.1021/acs.chemmater.0c00235
Language: English
Additional information: This version is the author accepted manuscript. For information on re-use, please refer to the publisher’s terms and conditions.
UCL classification: UCL
UCL > Provost and Vice Provost Offices > UCL BEAMS
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Engineering Science
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Engineering Science > Dept of Chemical Engineering
URI: https://discovery.ucl.ac.uk/id/eprint/10107554
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