Low-Voltage Li ₂ O ₂ Prelithiation Enabled by Catalytic Networks for High-Energy Lithium-Ion Batteries

The integration of high-capacity anodes into lithium-ion batteries (LIBs) is hindered by severe initial lithium loss, which limits achievable energy density. Cathode prelithiation offers a promising solution, but conventional sacrificial agents like Li2O2 require impractically high decomposition voltages (>4.7 V vs Li/Li+), which can lead to side reactions between the electrolytes and cathode materials. Here, we report a catalytic prelithiation system comprising nanosized Li2O2 and a RuO2/CNT network that reduces the decomposition potential to a practical 4.2 V while achieving 97.3% lithium utilization, as further supported by density functional theory (DFT) calculations revealing the lowered Li2O2 decomposition barrier. A strategically designed bilayer coating architecture ensures efficient oxygen management and promotes a stable, LiF-rich cathode interphase. Consequently, in NCM811||graphite full cells, this strategy delivers a 19.2% enhancement in initial energy density (to 361.7 Wh kg–1), along with improved capacity retention and a robust solid electrolyte interphase (SEI), providing a scalable pathway toward next-generation high-energy batteries.