Effects of sintering temperature on interfacial structure and interfacial resistance for all-solid-state rechargeable lithium batteries

Sintering processes yield a mutual diffusion region at the electrode/solid electrolyte interface, which is considered as a crucial problem for developing large-sized all-solid-state rechargeable lithium batteries with high power density. This work focuses on the interface between LiNi1/3Co1/3Mn1/3O2 (NMC) and NASICON-structured Li+ conductive glass ceramics solid electrolyte (Li2O-Al2O3-SiO2-P2O5-TiO2-circle divide GeO2: LATP sheet (AG-01)), and investigates the effects of sintering temperature on interfacial structure and interfacial resistance at the NMC/LATP sheet. Thin films of NMC were fabricated on the LATP sheets at 700 degrees C or 900 degrees C as a model system. We found that the thickness of the mutual diffusion region was almost the same, ca. 30 nm, in these two samples, but the NMC film prepared at 900 degrees C had three orders of magnitude larger interfacial resistance than the NMC film prepared at 700 degrees C. Around the interface between the NMC film prepared at 900 degrees C and the LATP sheet, Co in the NMC accumulates as a reduced valence and lithium-free impurity crystalline phase will be also formed. These two problems must contribute to drastic increasing of interfacial resistance. Formation of de-lithiated NMC around the interface and its thermal instability at higher temperature may be considerable reason to induce these problems. (C) 2016 Elsevier B.V. All rights reserved.