Rapid Large‐Scale Morphological Control and Interface Functionalization Enable All‐Weather LiFePO ₄ Cathode Material

ABSTRACT LiFePO 4 has been widely adopted as a dominant cathode material for Li‐ion batteries; however, its unsatisfactory charge‐transport capability and sluggish ionic‐diffusion kinetics greatly hinder its power performance, especially in cold winter conditions. Herein, we propose a scalable super‐liquid‐film‐reactor (SLFR) with an interface‐coating combined strategy to achieve rapid large‐scale functionalization of the LiFePO 4 (M‐LFP@cP) cathode with greatly boosted ionic diffusion. The kilogram‐scale LiFePO 4 is transient nanostructured by the SLMR reactor in seconds, significantly shortening the Li + diffusion pathway and circumventing the crystal damage that occurs during conventional ball‐milling over hours. The new N─Fe bond anchored on the LiFePO 4 surface substantially reduces the Li + diffusion barrier and favors rapid Li + diffusion at the interface, thereby suppressing interfacial side reactions and active lithium loss during cycling. Furthermore, in situ experiments and DFT analyses systematically elucidate the structure‐activity relationship of rate‐dependent failure behavior and functionalization. The new M‐LFP@cP material exhibits nearly 100% theoretical reversible capacity (168.7 mAh g −1 at 0.1 C), ultrahigh rate capability (50 C), remarkable capacity retention of 83.0% after 1000 cycles at 5 C, and stable charge‐discharge capability over an ultra‐wide temperature range from −30 to 60°C, fully demonstrating the broad industrialization prospects of all‐weather LiFePO 4 power batteries.