Abstract
Summary Two-phase reactions are prevalent in Li-ion batteries, whereas the underlying dynamics of phase separation in a real electrode still remain elusive, since numerous electrode particles constitute a formidably complex system for existing experimental techniques. Here we present an intriguing oscillatory phenomenon in the typical phase-separating electrode material Li 4 Ti 5 O 12 . During galvanostatic processes, the voltage oscillates due to the discrete nature of multi-particle phase-separating reactions, and the subtle oscillatory signals allow us to evaluate the fraction of actively phase-separating particles in real time. Through the analysis of oscillatory phenomena, we unveil the dependence of the active fraction on the depth of charge/discharge, cycling current, and working temperature, considerably deepening our understanding of the multi-particle phase-separation reaction. Moreover, it is the first time that electrochemical oscillations have been identified in rechargeable battery systems, opening up a new frontier for both theoretical and experimental researchers.
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