Unraveling the Rate‐Dependent Stability of Metal Anodes and Its Implication in Designing Cycling Protocol

Abstract It is widely recognized that a high current rate ( J ) speeds up dendrite formation and thus shortens the cycle life of metal anodes. Here, an anomalous correlation is reported between elevated J and deposition/stripping stability (decrease–increase–decrease), leading to the relative maximum stability at a moderate J . Complementary theoretical and experimental analyses suggest that such a complex relationship lies in high J 's dual and contradictory roles in kinetics and thermodynamics. The well‐known former renders decreased Sand's time (τ) and deteriorative cyclic stability, while the commonly overlooked latter provides larger extra energy that accelerates nucleation rate (ν n ). Using Zn metal anode as a model system, the ν n and τ controlled nucleation‐growth process is unambiguously revealed, both of which are closely related to J . Based on these findings, an initial high J discharge strategy is developed to produce abundant nuclei for uniform metal growth at standard J in the subsequent process. The protocol increases the Zn deposition/stripping lifetime from 303 to 2500 h under a cycling capacity of 1 mAh cm −2 without resorting to electrode/electrolyte modification. Furthermore, such a concept can be readily extended to Li/K metal anodes with significantly enhanced cycle life, demonstrating its universality for developing high‐performance metal batteries.