Ionic Transport Across Interfaces of Solid Glass and Polymer Electrolytes for Lithium Ion Batteries

Abstract

A study of lithium cation transport across solid-solid electrolyte interfaces to identify critical resistances in nanostructured solid electrolytes is reported. Bilayers of glass and polymer thin film electrolytes were fabricated and characterized for this study. The glass electrolyte was lithium phosphorous oxynitride (Lipon), and two polymer electrolytes were studied: poly(methyl methacrylate-co-poly(ethylene glycol) methyl ether methacrylate) and poly(styrene-co-poly(ethylene glycol) methyl ether methacrylate). Both copolymers contained LiClO 4 salt. In bilayers where polymer electrolyte layers are fabricated on top of Lipon, the interfacial resistance dominates transport. At 25 C, the interfacial resistance is at least three times greater than the sum of the Lipon and polymer electrolyte resistances. By reversing the structure and fabricating Lipon on top of the polymer electrolytes, the interfacial resistance is eliminated. Experiments to elucidate the origin of the interfacial resistance in the polymer-on-Lipon bilayers reveal that the solvent mixtures used to fabricate the polymer layers do not degrade the Lipon layer. The importance of the polymer electrolytes' mechanical properties is also discussed.

Lithium Ion Pathway within Li7La3Zr2O12‐Polyethylene Oxide Composite Electrolytes

“…Significant improvement in the ionic conductivity of polymer electrolytes was obtained with the addition of ceramic particles . It was suggested that an amorphous polymer shell formed around filler particles accounts for the increase in ionic conductivity . Finite element simulations also revealed that ion conduction within composite electrolytes mainly occurs at the ceramic–polymer interface.…”

“…It was suggested that an amorphous polymer shell formed around filler particles accounts for the increase in ionic conductivity . Finite element simulations also revealed that ion conduction within composite electrolytes mainly occurs at the ceramic–polymer interface. However, other hypotheses suggested that Li ions diffuse through the ceramic particles .…”

From Liquid- to Solid-State Batteries: Ion Transfer Kinetics of Heteroionic Interfaces

“…Compared to the SE/LE interface, the interfacial resistance and the energy barrier for the ion transport between the SE and the PE are mostly both higher [41]. In most of the published work, the interface resistance and activation energy were reported [41,44,[52][53][54][55][56][57][58], whereas the interface chemistry has been investigated only partially so far.…”

Editors' Choice—Understanding Chemical Stability Issues between Different Solid Electrolytes in All-Solid-State Batteries

“…3,30 Similarly, Zhou et al reported a beneficial effect of the SPE | oxide-based SE | SPE sandwich architecture on cycling behavior and dendrite stability in lithium and sodium ASSB test cells. 32,33 The same setup has been examined with regard to its ability to mitigate the risk of SE breakage as well as contact loss between SE and electrodes, 34 which is a major issue during cycling due to volume expansions. 11 Inspired by this promising concept, we investigated the combination of polymer interlayers with sulfide-based SEs, as they usually feature higher ionic conductivities than oxides.…”