Molecular-Sieve-Like MOF-Glass Interphase Enabling Predesolvation for Ultra-High Nickel Cathodes

Ultra-high nickel layered cathodes (Ni ≥ 90%) are pivotal for next-generation high-energy-density lithium-ion batteries, yet they suffer from severe interfacial instability and structural fatigue. Herein, we report a molecular-sieve-like MOF-glass interphase constructed via a low-temperature (175 °C) liquid-infusion technique. Leveraging capillary forces, the molten Zn–P–dmbIm MOF penetrates deep into intergranular voids, forming an ultra-thin (∼5 nm) and highly conformal encapsulation layer. The sub-nanometer pores (2.9 Å) of the MOF-glass function as an efficient ionic sieve to facilitate Li+ pre-desolvation, fundamentally intercepting electrolyte decomposition and transition metal dissolution. Electrochemical evaluations demonstrate that the MOF@NCM90 cathode delivers an exceptional specific capacity of 156.0 mAh g–1 at a high rate of 5 C, significantly outperforming the bare counterpart (118.2 mAh g–1). Moreover, it achieves a superior capacity retention of 80.0% after 500 cycles at 1 C. The universality of this strategy is further underscored in extreme Ni-rich systems: the near-pure-nickel MOF@NCM96 cathode retains 85.5% of its capacity over 200 cycles. This work demonstrates that precise molecular-scale control of desolvation kinetics is a transformative paradigm for enabling ultra-stable, high-capacity, and fast-charging lithium-ion batteries.