Lowering the Interfacial Resistance in Li6.4La3Zr1.4Ta0.6O12|Poly(Ethylene Oxide) Composite Electrolytes

Role of Filler Content and Morphology in LLZO/PEO Membranes

“…Therefore, tuning such an interface with similar approaches to achieve low resistance values is difficult. A relatively low resistance of 500 Ω cm 2 at 20 C for the PEO-LiTFSI/LLZO pellet interface was reported by Kuhnert et al (2020) by a facile surface treatment of LLZTO. However, the interface resistance is still too high to promote Li-ion migration throughout the whole electrolyte.…”

“…The lower Li-ion conductivity of PEO containing a higher amount of LLZO indicates that LLZO does not actively take part in the long-range Li-ion transport by providing fast ion-transport tracks, which is related to the high interface resistance between PEO and LLZO (Brogioli et al, 2019;Kuhnert et al, 2020). Hence, any further addition of LLZO filler leads to a narrowing or blocking of the Li-ion migration channels by restricted chain mobility (Zheng and Hu, 2018;Schneider, 2017), which reduces the Li-ion conductivity (Chen et al, 2018).…”

The role of polymers in lithium solid-state batteries with inorganic solid electrolytes

“…54 If the materials are immiscible, possible interactions between the atoms and molecules of the two phases include: 54,55 (1) chemical interactions, where electrons from both materials are shared between the two phases in the form of covalent bonds, hydrogen bonds and Lewis acid-base interactions. A typical example is the graing of polymer chains on ceramic particles; 56,57 (2) electrostatic interactions, where localized charged terminal groups in the ceramic and/or polymer interact with each other. The electrostatic forces are especially relevant with ceramic nanoparticles given their high surface to volume ratio and specic localized charge; 58 (3) dispersive interactions, where van der Waals forces between the atoms and molecules of the two materials dominate the interactionthe geckos' ability to adhere to almost any surface has been shown to be linked to this type; 59 and (4) mechanical interactions, where the microstructure at the micro-and nanoscale mechanically interlocks the two phases, this being the main mechanism of common polymer-based coatings, such as polytetrauoroethylene coatings on non-stick cookware.…”

“…In the context of the polymer-ISE interfaces for electrochemical applications, the nature of such interactions is rarely investigated. 56 However, such a mechanistic understanding of the phenomena governing the atomic and molecular dynamics at the interface is key for the design of better performing composites. In practical electrochemical devices, close contact between the inorganic and polymer phases is necessary, as fast transfer of the charge carriers across the boundary between the two materials is required to achieve good battery performance.…”

Electrochemical Impedance Spectroscopy of PEO-LATP Model Multilayers: Ionic Charge Transport and Transfer

“… 24 Indeed, the SPE/CE interface could add a significant resistance compared to that of the bulk electrolyte. 25 − 27 Consequently, it is crucial to study SPE/CE/SPE model assemblies in an attempt to probe separately the contributions of ionic migration in the bulk and interfacial ionic charge transfer to determine their governing factors. More generally, the study of the ionic charge transfer mechanism occurring at the interface between a liquid electrolyte (LE) or an SPE and a solid Li + conductor by means of such a model cell can be extended to the electrode active material/electrolyte interface, following the approach of Ogumi et al 28 − 30 While at the electrolyte/electrode interface an electrochemical charge transfer reaction involving a mixed ionic/electronic exchange occurs, at the electrolyte/ceramic interface, an ionic charge transfer reaction takes place.…”