Defect-Mediated Faceted Lithium Nucleation on Carbon Composite Substrates

Abstract

The formation of uniform, nondendritic seeds is essential to realizing dense lithium (Li) metal anodes and long-life batteries. Here, we discover that faceted Li seeds with a hexagonal shape can be uniformly grown on carbon-polymer composite films. Our investigation reveals the critical role of carbon defects in serving as the nucleation sites for their formation. Tuning the density and spatial distribution of defects enables the optimization of conditions for faceted seed growth. Raman spectral results confirm that lithium nucleation indeed starts at the defect sites. The uniformly distributed crystalline seeds facilitate low-porosity Li deposition, effectively reducing Li pulverization during cycling and unlocking the fast-charging ability of Li metal batteries. At a 1 C rate, full cells using LiNi_0.8Mn_0.1Co_0.1O₂ cathode (4.5 mA h cm^–2) paired with a lithium anode grown on carbon composite films achieve a 313% improvement in cycle life compared to baseline cells. Polymer composites with carbonaceous materials rich in defects are scalable, low-cost substrates for high-rate, high-energy-density batteries.