Cell-Shearing Chemistry Directed Closed-Pore Regeneration in Biomass-Derived Hard Carbons for Ultrafast Sodium Storage.

Abstract

The closed-pore structure of hard carbons holds the key to high plateau capacity and rapid diffusion kinetics when applied as sodium-ion battery (SIB) anodes. However, understanding and establishing the structure-electrochemistry relationship still remains a significant challenge. This work, for the first time, introduces an innovative deep eutectic solvent (DES) cell-shearing strategy to precisely tailor the cell structure of natural bamboo and consequently the closed-pore in its derived hard carbons. The DES shearing force effectively modifies the pore architecture by simultaneously shearing and dissolving amorphous components to form closed pore cores with adjustable sizes, as well as disintegrating crystalline cellulose through generation of competing hydrogen bonds to elaborately tune the pore wall thickness and ordering. The optimized closed-pore structure featuring appropriate pore size (∼2 nm) and ultra-thin (1-3 layers) disordered pore walls, exhibits abundant active sites and delivers rapid ion diffusion kinetics and high reaction reversibility. Consequently, a high reversible capacity of 422 mAh g-1 at 30 mA g-1 along with an exceptional rate capability (318.6 mAh g-1 at 6 A g-1) are achieved, outperforming almost all previous reported hard carbons. The new concept of cell-shearing chemistry for closed-pore regeneration significantly advances the applications of biomass materials for energy storage.