External Pressure Affecting Dendrite Growth and Dissolution in Lithium Metal Batteries During Cycles

Lithium (Li) metal has garnered significant attention as the preferred anode for high-energy lithium metal batteries. However, safety concerns arising from the growth of Li dendrites have hindered the advancement of Li metal batteries. In this study, we first elucidate the impact of external pressure and internal stress on dendrite growth and dissolution behavior of Li metal batteries during continuous charging-discharging cycles, employing a developed electrochemomechanical phase-field model. A typical parameter is defined to calculate the amount of dead Li that affects the electrochemical performance of Li metal batteries during multiple cycles. The underlying mechanisms of dendrites observed from in situ experiments are explained through the developed phase-field model. After charging/discharging, dendrites with a treelike structure yield a greater amount of dead Li compared to those with a needlelike configuration. Increasing the pressure appropriately can effectively reduce the growth points of dendrites and suppress the Li dendrite growth. Excessive pressure not only induces dendritic fractures that lead to the formation of dead Li but also undermines the battery performance. The accumulated internal stress might threaten the structural stability of the Li metal, thereby influencing the evolution of the Li dendrite morphology. A reasonable strategy is proposed to strike a balance between external pressure and the growth and dissolution of Li dendrites. These findings offer valuable insights into the judicious application of pressure to mitigate the advancement of electroplating reactions.