Weakly Solvating Few-Layer-Carbon Interface toward High Initial Coulombic Efficiency and Cyclability Hard Carbon Anodes

The carbonaceous anodes in sodium ion batteries suffer from low initial Coulombic efficiency (ICE) and poor cyclability due to rampant solid electrolyte interface (SEI) growth. The concept of the weakly solvating electrolyte (WSE) has been popularized for SEI regulation on the anode by adjusting the cation solvation structure. Nevertheless, the effects on the solvation sheath from the electrode/electrolyte interface are ignored in most WSE applications. In this work, we extend the WSE from the bulk electrolyte to the electrolyte/carbon interface. By recycling asphalt wastes into sp2 C enriched few-layer carbon on hard carbon, a weakly solvating interface is fabricated with lower adsorption energy to electrolyte solvent molecules than a pristine anode (−0.89 vs −1.08 eV for Na/diglyme). Accordingly, more anionic groups are attracted into the solvent-weakened solvation sheath during sodiation (2.30 vs 1.96 coordination number for PF6–). The anion-mediated contact ion pairs facilitate a thin, inorganic-rich SEI layer with a homogeneous distribution, which confers a high ICE of 97.9% and a high capacity of 335.6 mA h g–1 at 1 C (89.5% retention, 1000 cycles). The full battery also manifests an energy density of 209 W h kg–1. This interfacial design is applicable in both ether- and ester-based electrolytes, which is promising in cost-effective modification for carbonaceous electrodes.