A Kinetic‐Thermodynamic Synergy to Enhance {110} Texture for Stable Lithium Metal Anodes

ABSTRACT Lithium metal anodes (LMAs) are critical for developing next‐generation high‐energy‐density batteries, while uncontrolled dendrite growth and low Coulombic efficiency hinder their practical application. Engineering the crystallographic texture during lithium (Li) deposition to favor the {110} orientation is a promising strategy to suppress dendrite formation and improve performance. Here, we present a synergistic approach that combines deposition thermodynamics and kinetics to achieve a dominant {110} texture. By depositing Li on a lithiophilic tin (Sn)‐modified copper substrate at a high current density, the alloying reaction between Li and Sn yields a deposition interlayer composed of Sn and Li─Sn intermetallics that regulates both Li diffusivity and adsorption during initial deposition. Two‐dimensional Li nucleation and planar growth in larger grain sizes are achieved, thereby minimizing the total surface energy and promoting {110} texture formation. This effect, coupled with the kinetic selection of fast‐growing {110} planes, triples the volume fraction of the desired {110} texture while suppressing the competing {111} counterpart. When paired with a LiFePO 4 cathode, the resulting full cell exhibits stable cycling under practical conditions of a low negative‐to‐positive ratio and a lean electrolyte loading. This co‐regulation of deposition thermodynamics and kinetics offers a novel and effective strategy for fabricating high‐performance, dendrite‐free LMAs.