DOE OSTI2024
Hard carbon anodes have emerged as promising candidates for sodium-ion batteries due to their inherent advantages. Nevertheless, the surface imperfections in these materials often culminate in irreversible electrolyte consumption, fostering the development of a heterogeneous and fragile solid electrolyte interface (SEI), thereby compromising the initial Coulombic efficiency (ICE). Here, drawing inspiration from the catalytic potential of C=O (carbonyl) bonds in directing preferential salt reduction, we introduce a novel strategy that leverages the modulation of the binder, a long-term overlooked pivotal components in the electrode process. Specifically, Polymethyl methacrylate (PMMA), abundant in C=O groups, is partially substituted for PVDF, ensuring robust adhesion of the electrode material to the current collector while preserving superior mechanical properties. The accurate combination of two binders with delightful compatibility in the state-of-art electrode process, can promote a uniform formation of the SEI on the hard carbon surface enriched in inorganic components, which can ensure long-term interfacial stability and suppresses excessive solvent decomposition and facilitates Na + transfer at the interface. Consequently, the initial Coulombic efficiency of the hard carbon anode with 70 %PMMA binder achieves 86 %, with prominent cycling stability (88 % capacity retention over 500 cycles) at a high current density of 1.2 A g −1 . When paired with high loading cathodes to assemble the pouch cell, it also demonstrates stable operational scenarios.