Zinc Single-Atom-Regulated Hard Carbons for High-Rate and Low-Temperature Sodium-Ion Batteries.

Abstract

Hard carbons, as one of the most commercializable anode materials for sodium-ion batteries (SIBs), have to deal with the trade-off between the rate capability and specific capacity or initial Columbic efficiency (ICE), and the fast performance decline at low temperature (LT) remains poorly understood. Here, a comprehensive regulation on the interfacial/bulk electrochemistry of hard carbons through atomic Zn doping is reported, which demonstrates a record-high reversible capacity (546 mAh g^-1 ), decent ICE (84%), remarkable rate capability (140 mAh g^-1 @ 50 A g^-1 ), and excellent LT capacity (443 mAh g^-1 @ -40 °C), outperforming the state-of-the-art literature. This work reveals that the Zn doping can generally induce a local electric field to enable fast bulk Na⁺ transportation, and meanwhile catalyze the decomposition of NaPF₆ to form a robust inorganic-rich solid-electrolyte interphase, which elaborates the underlying origin of the boosted electrochemical performance. Importantly, distinguished from room temperature, the intrinsic Na⁺ migration/desolvation ability of the electrolyte is disclosed to be the crucial rate-determining factors for the SIB performance at LT. This work provides a fundamental understanding on the charge-storage kinetics at varied temperatures.