Redox-Active Ligand-Stabilized Lithium Iron Phosphate Nanoparticles for High-Performance Lithium-Ion Battery Cathode...

Developing cathodes that simultaneously deliver high capacity, superior rate capability, and long-term cycling stability remains a major challenge in lithium-ion batteries. Here, we report a high-performance textile cathode constructed via interfacial interaction-mediated assembly of high-energy porphyrin (PP) ligand-stabilized LiFePO₄ nanoparticles (LFP NPs). For this, 19 nm LFP NPs with olivine-type intercalation mechanism were covalently integrated with amine-functionalized PP to enable multi-electron redox activity, followed by encapsulation with multi-walled carbon nanotube (MWCNT) multilayers. Subsequent thermal annealing transformed the MWCNT layers into a covalently cross-linked conductive network. As a result, the textile cathode delivers an unprecedented specific capacity of ~260 mAh g^-1 at ~0.1 C, excellent rate capability, and retains over 93% of its initial capacity after 2,000 cycles at 1 C with nearly 100% Coulombic efficiency. This work highlights interfacial interaction-mediated ligand assembly as a powerful strategy for next-generation high-capacity and durable cathodes.