Electronic-State Polarization Engineering-Regulated Fluorinated Covalent Organic Framework Nanocables for Fast...

Covalent organic frameworks (COFs) are promising anode materials for lithium-ion batteries (LIBs) owing to their tunable porous structures and abundant redox-active sites; however, insufficient electronic-structure regulation and sluggish kinetics severely limit their rate capability and cycling stability. Herein, an electronic-state polarization engineering strategy is proposed by in situ constructing fluorinated COF nanocables enriched with multipolar C─F units on conductive carbon nanotube scaffolds to form a high-performance anode (F-COF@CNT). The strong polarity of C─F bonds induces localized electronic polarization within the COF framework, enhancing electrostatic attraction toward Li⁺ and accelerating ion transport. Combined GITT analysis and density functional theory calculations reveal a reduced Li⁺ diffusion barrier and a sustained diffusion coefficient on the order of 10^-11 cm² s^-1. Meanwhile, the interconnected CNTs network provides continuous electron-transport pathways, effectively mitigating interfacial polarization and structural degradation. As a result, the F-COF@CNT anode delivers 496.32 mAh g^-1 at 0.1 A g^-1 and maintains 281.21 mAh g^-1 after 2000 cycles at 2.0 A g^-1. An NCM811||F-COF@CNT full cell retains 105.94 mAh g^-1 after 500 cycles, demonstrating excellent practical stability. This work establishes electronic-state polarization engineering as a general strategy to overcome kinetic limitations in organic framework anodes.