Operando imaging of crystal structure and orientation in all components of all-solid-state-batteries

TL;DR

This study uses operando synchrotron X-ray micro-diffraction imaging to simultaneously observe crystal structure and orientation changes in all components of an all-solid-state battery during operation, revealing how these factors influence reaction mechanisms.

Contribution

It introduces a comprehensive real-time imaging technique to analyze interactions and structural evolutions in all-solid-state batteries, linking crystal orientation with reaction mechanisms.

Findings

LiCoO2 reaction depends on crystal orientation

Delithiation limited by Li-rich interface in dense electrodes

Li metal orientation influenced by Ti current collector

Abstract

A comprehensive understanding of interactions between cathode, electrolyte, anode, and packaging during battery operation is crucial for advancing performances but remains overlooked due to the lack of characterisation technics capable of measuring these components simultaneously. We perform a holistic investigation of a compact all-solid-state-battery using operando synchrotron X-ray micro-diffraction imaging. We image in real time and simultaneously the lattice parameter and crystal orientation of the dense LiCoO2 cathode, the Ti current collector and the electrodeposited Li metal anode. We reveal that reaction mechanism of LiCoO2 depends on the crystal orientation, and that, in dense electrodes as opposed to porous ones, the delithiation is limited by the formation of a Li-rich insulating interface. Li metal crystal orientation is found to be influenced initially by the Ti texture and to change within minutes during plating and stripping. These results demonstrate the power of X-ray imaging to link reaction mechanism and grain orientation during non-equilibrium processes.