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Factors affecting cyclic durability of all-solid-state lithium batteries using poly(ethylene oxide)-based polymer electrolytes and recommendations to achieve improved performance

Faglioni, Francesco and Merinov, Boris and Goddard, William A., III and Kozinsky, Boris (2018) Factors affecting cyclic durability of all-solid-state lithium batteries using poly(ethylene oxide)-based polymer electrolytes and recommendations to achieve improved performance. Physical Chemistry Chemical Physics, 20 (41). pp. 26098-26104. ISSN 1463-9076. https://resolver.caltech.edu/CaltechAUTHORS:20181003-130917687

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Abstract

A detailed experimental analysis of the factors affecting cyclic durability of all-solid-state lithium batteries using poly(ethylene oxide)-based polymer electrolytes was published in EES by Nakayama et al. We use quantum mechanics to interpret these results, identifying processes involved in the degradation of rechargeable lithium batteries based on polyethylene oxide (PEO) polymer electrolyte with LiTFSI. We consider that ionization of the electrolyte near the cathode at the end of the recharge step is probably responsible for this degradation. We find that an electron is likely removed from PEO next to a TFSI anion, triggering a sequence of steps leading to neutralization of a TFSI anion and anchoring of another TFSI to the PEO. This decreases the polymer conductivity near the cathode, making it easier to ionize additional PEO and leading to complete degradation of the battery. We refer to this as the Cathode Overpotential Driven Ionization of the Solvent (CODIS) model. We suggest possible ways to confirm experimentally our interpretation and propose modifications to suppress or reduce electrolyte degradation.


Item Type:Article
Related URLs:
URLURL TypeDescription
https://dx.doi.org/10.1039/C8CP05440ADOIArticle
http://www.rsc.org/suppdata/c8/cp/c8cp05440a/c8cp05440a1.pdfPublisherSupporting Information
ORCID:
AuthorORCID
Faglioni, Francesco0000-0002-3327-8848
Merinov, Boris0000-0002-2783-4262
Goddard, William A., III0000-0003-0097-5716
Kozinsky, Boris0000-0002-0638-539X
Additional Information:© Royal Society of Chemistry 2018. The article was received on 27 Aug 2018, accepted on 26 Sep 2018 and first published on 26 Sep 2018. There are no conflicts to declare. BVM and WAG thank LGChem, NSF (CBET 1512759), and ONR (N00014-18-1-2155) for partial support.
Funders:
Funding AgencyGrant Number
LGChemUNSPECIFIED
NSFCBET-1512759
Office of Naval Research (ONR)N00014-18-1-2155
Other Numbering System:
Other Numbering System NameOther Numbering System ID
WAG1304
Issue or Number:41
Record Number:CaltechAUTHORS:20181003-130917687
Persistent URL:https://resolver.caltech.edu/CaltechAUTHORS:20181003-130917687
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:90096
Collection:CaltechAUTHORS
Deposited By: Donna Wrublewski
Deposited On:03 Oct 2018 20:54
Last Modified:03 Oct 2019 20:22

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