Correlating amorphous carbonaceous structure to calendar aging resistance of lithium metal anodes

Active lithium metal anodes (LMAs) suffer from electrolyte corrosion, leading to capacity loss and deterioration of the battery. Although advanced electrolyte and artificial solid electrolyte interface (SEI) have been developed to address this issue, more complexity can be inevitably introduced to intricate battery chemistry system. Herein, this paper proposes a novel mechanism correlating the amorphous carbonaceous structure with the calendar aging resistance of LMAs, based on well-constructed carbon samples (highly amorphous carbon HAC and low amorphous carbon LAC) with similar morphology, elemental compositions and surface functional groups. With more carbon defects serving as nucleation sites, HAC consistently exhibits a lower nucleation overpotential than LAC at various current densities (0.2–4.0 mA cm⁻²), effectively inducing the formation of spherical Li nuclei and facilitating dense deposition. Furthermore, benefiting from larger lattice spacing, HAC enables an anion-rich solvation structure at the interface, thereby promoting the generation of an inorganic-rich SEI. Consequently, the dual-optimization of nucleation and interface results in an enhanced ability of LMAs to resist calendar aging. The correlation between carbon microstructure and the protection of LMAs offers a new pathway for designing next-generation batteries.