Soft‐Hard Synergistic Bicontinuous Conductive Network in SiO _x /Nitrogen‐Doped Laser‐Induced Graphene/Cu Composites for Durable Lithium‐Ion Batteries

ABSTRACT

Silicon‐based anodes are limited by severe volume fluctuations and sluggish charge‐transfer kinetics. Although metallic coatings can improve electronic conductivity, continuous dense coatings may impede electrolyte access, and lithium‐ion transport. Herein, a soft‐hard synergistic bicontinuous conductive network strategy is proposed to fabricate a SiO _x /nitrogen‐doped laser‐induced graphene/Cu (SiO _x /NLIG/Cu) composite. Deep eutectic solvent (DES)‐derived nitrogen‐doped active sites combine with super‐lyophilic NLIG matrix to spatially guide the electrodeposition of an interconnected percolation network, rather than an ionic blocking layer. This bicontinuous configuration decouples electronic and ionic transport. The porous NLIG framework serves as a strain buffer and a low‐tortuosity ion conduit, while the interpenetrating Cu network maintains electrical continuity and structural integrity. This conductive framework is associated with the formation of a stable, LiF‐rich solid electrolyte interphase, enhancing the lithium‐ion diffusion coefficient by one order of magnitude. The binder‐free anode delivers an initial lithiation capacity of 1820.6 mAh g ⁻¹ with an initial Coulombic efficiency of 86.3% at 0.1 A g ⁻¹ . It also exhibits enhanced durability, achieving 86.4% capacity retention after 1000 cycles at 2.0 A g ⁻¹ . Full cells assembled with LiNi _0.8 Co _0.1 Mn _0.1 O ₂ cathodes achieve an active‐material‐level gravimetric energy density of 614.7 Wh kg ⁻¹ . This soft‐hard synergy strategy provides a versatile solution to high‐performance lithium‐ion batteries.