Integrated manufacturing of REciclable multi-material COmposites for the TRANSport sector

This work fabricates honeycomb?like covalent organic frameworks vertically aligned on graphene oxide (HCCOF?GO) via one?pot colloidal assembly as an ASEI. The abundant binding sites significantly reduce the nucleation barrier, while the nanochannels enhance desolvation via confinement, anchor anions, and facilitate graded SEI formation, enabling homogeneous Li? flux and dendrite?free LMBs.This study pioneers vertically aligned honeycomb covalent organic framework (HCCOF) on graphene oxide (HCCOF?GO) through one?pot colloidal assembly, establishing a paradigm for interface?engineered 2D heterostructures in lithium metal batteries (LMBs). Mechanistically, the vertical COF alignment via interfacial ?–? conjugation preserves intrinsic 1.15 nm hexagonal pores while integrating Go's electron transport capabilities. When deployed as an artificial solid?electrolyte interphase (ASEI), this architecture demonstrates triple functionalities: i) “lithiophilic” nanopores enabling dendrite?free Li+ flux (migration barrier 0.29 eV), ii) polarized interfaces regulating anion?solvent coordination, and iii) gradient organic–inorganic solid electrolyte interphase (SEI) formation. The modified anodes achieve record Li+ transference number (tLi+ = 0.96) with ultra?long cyclability (>3000 h at 10 mA cm?2, 10 mAh cm?2) and minimal polarization (?V = 13 mV). Competitive electrochemical performance across diverse battery configurations confirms practical viability: the HCCOF?GO@Li?NCM811 full cell retains 81.1% of its initial capacity after 100 cycles at a practical loading of 4.5 mAh cm?2. Corresponding pouch cells (368 Wh kg?1) maintain 82.3% capacity retention after 40 cycles, while HCCOF?GO@Li?LCO cell demonstrates remarkable cycling stability (500 cycles@80.3%) at a high voltage of 4.7 V.

» Publication Date: 17/10/2025

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