Publication date: 10th April 2024
Electrochemical energy storage relies on electrode materials facilitating ion and electron transport. In solid-state batteries, the electrode architecture typically comprises multi-phase composites, including mixed ion-electron conductors (e.g., LixNi8Co1Mn1O2 (NCM)), solid electrolytes (e.g., Li7La3Zr2O12 (LLZO)), and electronically conductive carbon (e.g., carbon black). Charge transport in such heterogeneous systems is intricate and is often erroneously analyzed using traditional theories developed for homogeneous electrodes, leading to a misunderstanding of electrode kinetics in real battery cells.
In this contribution, we present a comprehensive treatment for characterizing the kinetics of composite electrodes. Our approach considers not only the composite's microstructure but also the heterointerfaces between its constituents, significantly influencing electrical and chemical transport phenomena in composites. Employing electrochemical impedance spectroscopy, we identify non-ideal spectra and the corresponding time constants of heterogeneous systems using a generalized transmission line model. Furthermore, to capture the morphological nature of composites, we reconstruct the 3D structure of practical electrodes consisting of NCM, LLZO, and carbon black through transmission X-ray microscopy (TXM). By visualizing concentration propagation during lithium insertion, we unveil the critical roles of size, shape, coating, and contact effects in composites, providing guidelines for rationally designing electrode architectures in solid-state batteries. The treatment developed herein sheds light on understanding and predicting the behaviors of charge carriers in complex electrochemical systems.
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