High temperature induced abundant closed nanopores for hard carbon as high-performance sodium-ion batteries anodes

Abstract

Hard carbon (HC) stands out as the preeminent anode material for sodium-ion batteries (SIBs) which are deployed in expansive energy storage infrastructures. Herein, the large enough graphene nanosheets interlayer and abundant nanopores with a diameter of ∼2.1 nm induced by adjusting the pyrolysis temperature in the thermosetting phenolic resin-derived hard carbon matrix to augment the performance of the sodium ion storage. The presence of sufficiently large carbon interlayers has been proven to provide active sites for reversible adsorption, enabling effective storage of sodium ions in the high-voltage slope region, while also promoting rapid Na+ transport. Meanwhile, forming abundant closed nanopores with larger sizes helps sodium ion storage in the low-voltage plateau region. In the optimized samples, the formation of sufficient long graphene nanosheets with a perfect crystal lattice, which further shrinks to form enclosed nanopores, effectively reduces defective sites and specific surface area. Additionally, the appropriate content of C-O and C=O functional groups contributes to an exceptional initial Coulombic efficiency (ICE) of up to 93%. Simultaneously, the optimized sample HC-1500 contributes to a remarkable plateau capacity of 294 mAh g-1 during the charging process (high reversible capacity of 403 mAh g-1 at 0.1 C). Moreover, based on the microstructure evolution and Na storage behavior of hard carbon, an “adsorption (27%) – filling (73%)” sodium storage mechanism that the sodium storage as a quasi-metallic sodium state is demonstrated. Consequently, this study will offer valuable insights for the development of hard carbon anodes tailored for high-energy practical SIBs, while also advancing the understanding of sodium storage mechanisms.