Scalable Construction of 3D Lithium‐Phosphor Bronze Composite Anodes for Synergistic Lithium Deposition Regulation in High‐Rate Batteries

The practical application of lithium (Li) metal anodes is severely hindered by uncontrolled dendrite growth and infinite volume changes, particularly under high‐rate cycling conditions. Herein, we propose a robust mechanically interlocked Li‐phosphor bronze mesh (Li@PBM) composite anode for high‐rate Li metal batteries (LMBs), fabricated via a facile mechanical rolling process. Both experimental characterizations and phase‐field simulations reveal that the active Sn and P species within the PBM trigger an in situ interfacial reconstruction, which significantly enhances the chemical affinity toward Li. Synergistically, the unique mechanical interlocked structure accommodates volume fluctuations and redistributes the local electric field, guiding uniform Li deposition even at high current densities. Consequently, the Li@PBM||Li@PBM cells demonstrate exceptional cycling stability for over 1000 h at 5 mA cm −2 and 5 mAh cm −2 , whereas the Li||Li cells suffer from large voltage hysteresis and fail within 100 h. Furthermore, pairing with LiFePO 4 (LFP) cathodes (11.2 mg cm −2 ), the LFP||Li@PBM cells achieve 83.5% capacity retention over 500 cycles at 5.0 C (0.75 A g −1 ). In contrast, the LFP||Li counterparts experience rapid capacity decay, retaining only 53.1% capacity after 200 cycles. This work highlights the efficacy of combining alloy chemistry with structural engineering to unlock the potential of high‐rate LMBs.