A Precursor Design Principle for Archipelagic Hard-Carbon Structural Evolution Through Cohesion-Solvation Regulation...

Sodium-ion batteries are central to the development of affordable electrochemical storage for renewable energy integration. Yet hard-carbon anode design lacks a precursor-level principle linking molecular assembly in chemically heterogeneous feedstocks to oxidative stabilization and closed-pore formation. Here we establish a precursor-level cohesion-solvation design principle for regulating molecular selection and assembly in heterogeneous aromatic feedstocks. Toluene-fractionated asphaltene precursors undergo oxidative crosslinking, redirecting carbonization from continuous coke-like growth toward separated turbostratic domains and confined closed pores. A hard-carbon performance screening index (HPSI) quantifies structural and electrochemical performance, while density functional theory (DFT) reveals stronger Na affinity and lower migration barriers in defect-engineered carbon galleries. The solvent-selected AHC-80-1400 delivers 400.1 mAh g^-1 at 0.05 A g^-1 with 87.7% ICE and retains 92.3% capacity after 10 000 cycles, while sustaining wide-temperature sodium storage with 91.8% and 90.4% retention at -20°C and 50°C, respectively. At scale, a 10-kg batch enables a 1.18 Ah NFM||AHC-80-1400 pouch cell, delivering 163.3 Wh kg^-1 and 95.5% retention after 700 cycles. A cradle-to-gate life-cycle assessment (LCA) shows that AHC-80-1400 production reduces climate-change impact by 33.7% relative to Commercial HC. These findings establish precursor-stage molecular selection as a design principle for harnessing feedstock heterogeneity to control carbonization trajectories and electrochemical function.