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dc.contributor.authorRincón, M. 
dc.contributor.authorGarcía Daza, F.A.
dc.contributor.authorRanque, P.
dc.contributor.authorAguesse, F.
dc.contributor.authorCarrasco, J.
dc.contributor.authorAkhmatskaya, E.
dc.description.abstractUnlocking the full potential of solid-state electrolytes (SSEs) is key to enabling safer and more-energy dense technologies than today’s Li-ion batteries. In particular, composite materials comprising a conductive, flexible polymer matrix embedding ceramic filler particles are emerging as a good strategy to provide the combination of conductivity and mechanical and chemical stability demanded from SSEs. However, the electrochemical activity of these materials strongly depends on their polymer/ceramic interfacial Li-ion dynamics at the molecular scale, whose fundamental understanding remains elusive. While this interface has been explored for nonconductive ceramic fillers, atomistic modeling of interfaces involving a potentially more promising conductive ceramic filler is still lacking. We address this shortfall by employing molecular dynamics and enhanced Monte Carlo techniques to gain unprecedented insights into the interfacial Li-ion dynamics in a composite polymer-ceramic electrolyte, which integrates polyethylene oxide plus LiN(CF3SO2)2 lithium imide salt (LiTFSI), and Li-ion conductive cubic Li7La3Zr2O12 (LLZO) inclusions. Our simulations automatically produce the interfacial Li-ion distribution assumed in space-charge models and, for the first time, a long-range impact of the garnet surface on the Li-ion diffusivity is unveiled. Based on our calculations and experimental measurements of tensile strength and ionic conductivity, we are able to explain a previously reported drop in conductivity at a critical filler fraction well below the theoretical percolation threshold. Our results pave the way for the computational modeling of other conductive filler/polymer combinations and the rational design of composite SSEs.en_US
dc.description.sponsorship-Juan de la Cierva grant IJC2018-037214-I, -PID2019-106519RB-I00, as -HPC-Europa3 grant HPC17ERWTO -AI in BCAM, EXP. 2019/0043en_US
dc.rightsReconocimiento-NoComercial-CompartirIgual 3.0 Españaen_US
dc.subjectsolid-state electrolytes, space-charge models, Li-ion batteries, polymer-ceramic electrolyte, molecular dynamics, solid-solid interface, GSHMCen_US
dc.titleUnveiling Interfacial Li-Ion Dynamics in Li7La3Zr2O12/PEO(LiTFSI) Composite Polymer-Ceramic Solid Electrolytes for All-Solid-State Lithium Batteriesen_US
dc.relation.projectIDinfo:eu-repo/grantAgreement/AEI/Plan Estatal de Investigación Científica y Técnica y de Innovación 2017-2020/PID2019-104927GB-C22en_US
dc.relation.projectIDinfo:eu-repo/grantAgreement/Gobierno Vasco/BERC/BERC.2018-2021en_US
dc.relation.projectIDinfo:eu-repo/grantAgreement/Gobierno Vasco/ELKARTEKen_US
dc.journal.titleACS Applied Materials and Interfacesen_US

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Reconocimiento-NoComercial-CompartirIgual 3.0 España
Except where otherwise noted, this item's license is described as Reconocimiento-NoComercial-CompartirIgual 3.0 España