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 LiFePO₄ 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.