Strategies for the Analysis of Graphite Electrode Function

Abstract Since the commercialization of lithium‐ion batteries, graphite has been the uncontested material of choice as the negative electrode host structure, and it has therefore been pivotal for their ubiquitous adoption and implementation. Despite extensive research efforts dedicated to discovering and developing alternative anode material candidates, no commercially viable successor has so‐far been identified. Simultaneously, the understanding of graphite electrode function is continuously expanding, and new strategies for rationally improving performance are being explored. Here, the key challenges lie in examining the graphitic material, not only in the pure as‐prepared state, but also when formed into an electrode and during electrochemical cycling, i.e., in situ/operando. A multiscale approach is necessary to accurately relate the (de)lithiation/(de)intercalation mechanisms involved to the observed performance. The present review summarizes conventional techniques and highlights recent advances in the analytical methods used for the characterization of graphite‐based electrode structure and function. The discussion is based on examples from key recent work using innovative analytical strategies to obtain novel insight into the evolution in structure, microstructure, electronic structure, surface chemistry/composition, etc. The deeper understanding of material function gained from these innovative approaches may hold the key for the rational design of next‐generation graphite‐based or ‐inspired electrodes.