Accelerating lithium-ion pre-desolvation and transport via glassy MOF for fast-charging and high-energy-density lithium-ion batteries

Abstract Conventional graphite anodes in lithium-ion batteries (LIBs) suffer from limited fast-charging capability and lithium dendrite growth, particularly at high current densities. This work introduces a glassy metal-organic framework (MOF glass) that simultaneously enables facile lithium-ion pre-desolvation and fast Li⁺ transport. The MOF glass-coated graphite (Glass@Graphite) forms a distinctive double-layer structure during initial discharge: an electron-insulating outer layer with rigid 2.93 Å pores that facilitates facile Li⁺ pre-desolvation, and a Li₃P-rich inner layer that ensures rapid lithium-ion conduction. The outer layer's pre-desolvation effect generates a highly aggregated electrolyte within MOF channels, promoting formation of a stable anion-derived LiF-dominated solid electrolyte interphase. The resulting partially desolvated Li⁺ species readily penetrate the ion-conducting inner layer, enabling ultrafast diffusion. When coupled with LiNi₀.₈Co₀.₁Mn₀.₁O₂ (NCM-811) cathodes, the NCM-811//Glass@Graphite full cells demonstrate remarkable fast-charging performance (88% capacity retention after 1000 cycles at high current of 4 C). A practical 2.36 Ah pouch-cell achieves an energy density of 283 Wh/kg while maintaining over 80% capacity after 300 cycles. This approach presents a transformative strategy for developing fast-charging, high-energy-density LIBs.