Uncorrelated Lithium-Ion Hopping in a Dynamic Solvent-Anion Network

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dc.contributor.authorYu, Deyangen
dc.contributor.authorTroya, Diegoen
dc.contributor.authorKorovich, Andrew G.en
dc.contributor.authorBostwick, Joshua E.en
dc.contributor.authorColby, Ralph H.en
dc.contributor.authorMadsen, Louis A.en
dc.date.accessioned2023-09-29T13:28:46Zen
dc.date.available2023-09-29T13:28:46Zen
dc.date.issued2023-03en
dc.description.abstractLithium batteries rely crucially on fast charge and mass transport of Li+ in the electrolyte. For liquid and polymer electrolytes with added lithium salts, Li+ couples to the counter-anion to form ionic clusters that produce inefficient Li+ transport and lead to Li dendrite formation. Quantification of Li+ transport in glycerol-salt electrolytes via NMR experiments and MD simulations reveals a surprising Li+-hopping mechanism. The Li+ transference number, measured by ion-specific electrophoretic NMR, can reach 0.7, and Li+ diffusion does not correlate with nearby ion motions, even at high salt concentration. Glycerol's high density of hydroxyl groups increases ion dissociation and slows anion diffusion, while the close proximity of hydroxyls and anions lowers local energy barriers, facilitating Li+ hopping. This system represents a bridge between liquid and inorganic solid electrolytes, thus motivating new molecular designs for liquid and polymer electrolytes to enable the uncorrelated Li+-hopping transport needed for fast-charging and all-solid-state batteries.en
dc.description.notesThis material is based upon work supported by the U.S. Department of Energy’s Office of Energy Efficiency and Renewable Energy (EERE) under award No. DE-EE0008860. This research was also supported in part by the National Science Foundation under Award DMR 1810194. The authors gratefully acknowledge Prof. Rui Qiao at Virginia Tech for beneficial discussions.en
dc.description.sponsorshipU.S. Department of Energy?s Office of Energy Efficiency and Renewable Energy (EERE) [DE-EE0008860]; National Science Foundation [DMR 1810194]en
dc.description.versionPublished versionen
dc.format.mimetypeapplication/pdfen
dc.identifier.doihttps://doi.org/10.1021/acsenergylett.3c00454en
dc.identifier.issn2380-8195en
dc.identifier.pmid37090169en
dc.identifier.urihttp://hdl.handle.net/10919/116374en
dc.language.isoenen
dc.publisherAmerican Chemical Societyen
dc.rightsCreative Commons Attribution-NonCommercial-NoDerivatives 4.0 Internationalen
dc.rights.urihttp://creativecommons.org/licenses/by-nc-nd/4.0/en
dc.subjectfrequency impedance spectroscopyen
dc.subjectphysicochemical propertiesen
dc.subjecttransference numbersen
dc.subjectconcentrated electrolytesen
dc.subjectdiffusion-coefficientsen
dc.subjectirreversible-processesen
dc.subjectreciprocal relationsen
dc.subjectliquid electrolytesen
dc.subjectself-diffusionen
dc.subjecttransporten
dc.titleUncorrelated Lithium-Ion Hopping in a Dynamic Solvent-Anion Networken
dc.title.serialACS Energy Lettersen
dc.typeArticle - Refereeden
dc.type.dcmitypeTexten

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