Fast Ion Conduction of Sintered Glass-Ceramic Lithium Ion Conductors Investigated by Impedance Spectroscopy and Coaxial Reflection Technique

Abstract

As the ionic conductivity of solid-state lithium ion conductors rises, knowledge of the detailed conductivity mechanisms is harder to obtain due to the limited frequency resolution of the traditional impedance spectrometers. Moreover, the data is easily affected by the local microstructure (i.e. pores, grain-boundaries) and the preparation conditions. The aim of this work is to demonstrate the feasibility of the coaxial reflection technique as a reliable tool to study fast ionic conductors (i.e. σ > 10−4 S cm−1). Especially the relative permittivity can be determined more accurately at room temperature. For the first time the electrical performance of LATP and LLZO manufactured via a scalable top-down glass-ceramic route is evaluated. The density turns out to be a key parameter influencing both relative permittivity and resulting conductivities. For a 100% dense LATP sample the coaxial reflection technique reveals a high grain-core conductivity of 6 × 10−3 S cm−1 similar to the conductivity of ideal single crystals.

Functionalized Thiophosphate and Oxidic Filler Particles for Hybrid Solid Electrolytes

“…[11] Another oxide material lithium aluminum titanium phosphate (LATP) shows a lower skeletal density and high grain-core conductivity (6 mS cm À 1 ), but the overall conductivity is limited by high resistance pathways across grain-boundaries. [12] In addition, LATP is not stable against lithium metal, caused by the redox reaction of Ti 4 + at the anode interface. [13] Thiophosphate SEs such as Li 9.54 Si 1.74 P 1.44 S 11.7 Cl 0.3 show high ionic conductivities up to 25 mS cm À 1 at RT [14] and a lithium transference number of 1.…”

“…Furthermore, materials like LLZO are very brittle resulting in difficult fabrication and the formation of dendrites in spawning cracks and along grain boundaries [11] . Another oxide material lithium aluminum titanium phosphate (LATP) shows a lower skeletal density and high grain‐core conductivity (6 mS cm −1 ), but the overall conductivity is limited by high resistance pathways across grain‐boundaries [12] . In addition, LATP is not stable against lithium metal, caused by the redox reaction of Ti 4+ at the anode interface [13] .…”

Ultrafast Crystallization and Sintering of Li1.5Al0.5Ge1.5(PO4)3 Glass and Its Impact on Ion Conduction

“…This Article (a schematic representation of its content is given in Figure ) contributes to unraveling the impact of UHS on the physical properties and Li + conduction of crystalline LAGP obtained from LAGP glassy powders. These processing conditions (i.e., short processing time and ambient atmosphere) are conducive to the large-scale production of solid-state batteries. , In fact, applying UHS in place of furnace sintering, which has a high impact on energy demand and costs, can represent a viable and less time- and energy-intensive alternative.…”

“…These processing conditions (i.e., short processing time and ambient atmosphere) are conducive to the large-scale production of solidstate batteries. 40,41 In fact, applying UHS in place of furnace sintering, which has a high impact on energy demand and costs, 19 can represent a viable and less time-and energyintensive alternative.…”

High-Content Lithium Aluminum Titanium Phosphate-Based Composite Solid Electrolyte with Poly(ionic liquid) Binder

“…However, current commercial Li-ion batteries are mainly assembled with organic liquid electrolytes, which are leaky, flammable, and volatile, leading to severe security risks [ 4 , 5 , 6 ]. To address the above issues, active ceramic-based solid electrolytes have been designed and fabricated for increasing the security of Li-ion batteries [ 7 ], such as garnet-type lithium lanthanum zirconium oxide [ 8 ], LISICON-type lithium-ion conductor [ 9 ], NASICON-type lithium aluminum titanium phosphate [ 10 ], and perovskite-type lithium lanthanum titanium oxide [ 11 ]. Although these active ceramics have excellent bulk ionic conductivity, the grain, grain boundaries, and their interfaces also exist in the electrolyte films, which dramatically decrease the total conductivity [ 12 , 13 , 14 ].…”