Unraveling A lattice lithium supplementation-interfacial catalysis tandem effect for enabling durable lithium-ion full cells

Prelithiation has been widely recognized as an effective strategy to compensate for active lithium loss and enhance the energy density of lithium-ion batteries. This work unlocks a green and efficient La-doped pre-lithiation additive La-Li₂NiO₂. As revealed, such cathode prelithiation material exhibits dual functionality, it can effectively compensate LiFePO₄ for irreversible lattice lithium loss during cycling, and upon completion of the first cycle, it will transform into catalytically active La-LiNiO₂. Interestingly, this transformed material enables reducing the dissociation energy barrier of LiPF₆ while concurrently catalyzing the decomposition of LiPF₆ leading to the formation of a thin, uniform, and LiF-rich cathode/electrolyte interphase (CEI). Compared with the pristine Li‖LiFePO₄ half-cell, benefiting from the tandem effect of lithium supplementation and interface optimization, the Li‖LiFePO₄ with 5 % La-Li₂NiO₂ prelithiation additive exhibits superior rate performance, achieving a specific capacity of 95.2 mAh g^-1 at 10 C rate. Beyond that, the Graphite‖LiFePO₄ with 5 % La-LNO full cells exhibit an 86.0 % capacity retention rate after 1000 cycles even at 5 C condition. This work highlights a new design paradigm for cathode prelithiation additives that integrate efficient lithium compensation and interface regulation, it can deepen the understanding of constructing practical full cells including but not limited to lithium-ion batteries. © 2026 Elsevier B.V.