Show simple item record

dc.contributor.authorHobold, Gustavo M.
dc.contributor.authorKhurram, Aliza
dc.date.accessioned2020-06-04T12:00:46Z
dc.date.available2020-06-04T12:00:46Z
dc.date.issued2020-02
dc.identifier.issn0897-4756
dc.identifier.urihttps://hdl.handle.net/1721.1/125667
dc.description.abstractFormation of stable solid electrolyte interphases (SEI) that protect Li against continuous electrolyte reduction is one of the remaining challenges to enable safe, secondary high-energy Li batteries with minimal capacity loss. However, SEI formation pathways remain difficult to experimentally pinpoint, even with the most well-known carbonate electrolytes and graphite anodes, and especially on Li. Using a custom electrochemical cell coupled to a gas chromatograph (GC), dynamic gas-phase signatures of interphase reactions during a first Li plating step in EC/DMC were monitored as a function of cell chemistry and operational parameters. The operando nature of these experiments allows distinction to be drawn between gases formed chemically by the reaction of metallic Li and electrolyte, vs those evolved electrochemically, i.e., through electron-transfer and reaction with Li+. Quantification of gas evolution molar ratios during cycling enables determination of specific interphase reactions and their branching ratios dominating active SEI formation. We find that SEI-repair mechanisms are sensitive to the choice of the electrolyte salt (LiPF6/LiClO4/LiTFSI), solvent fluorination, and current density. In particular, SEIs resulting from solvent decarbonylation and/or decarboxylation - leading to enhanced CO and/or CO2 evolution - are the most stable, providing a simple and descriptive gas-phase signature indicative of high Coulombic efficiencies of Li plating/stripping.en_US
dc.language.isoen
dc.publisherAmerican Chemical Society (ACS)en_US
dc.relation.isversionofhttps://dx.doi.org/10.1021/acs.chemmater.9b04550en_US
dc.rightsCreative Commons Attribution 4.0 International licenseen_US
dc.rights.urihttps://creativecommons.org/licenses/by/4.0/en_US
dc.sourceACSen_US
dc.titleOperando Gas Monitoring of Solid Electrolyte Interphase Reactions on Lithiumen_US
dc.typeArticleen_US
dc.identifier.citationHobold, Gustavo M., Aliza Khurram and Betar M. Gallant. “Chemistry of Materials” Chemistry of Materials, vol. 32, no. 6, 2020, pp. 2341-2352 © 2020 The Author(s)en_US
dc.contributor.departmentMassachusetts Institute of Technology. Department of Mechanical Engineeringen_US
dc.relation.journalChemistry of Materialsen_US
dc.eprint.versionFinal published versionen_US
dc.type.urihttp://purl.org/eprint/type/JournalArticleen_US
eprint.statushttp://purl.org/eprint/status/PeerRevieweden_US
dc.date.updated2020-05-18T15:28:18Z
dspace.date.submission2020-05-18T15:28:22Z
mit.journal.volume32en_US
mit.journal.issue6en_US
mit.licensePUBLISHER_CC


Files in this item

Thumbnail

This item appears in the following Collection(s)

Show simple item record