Locking Rich Lattice Strain at Atomic Level Within L1₂ Intermetallic Pt₃Co Nanocrystal Catalysts for High‐Performance Li‐O₂ Batteries

Due to enhanced d ‐ d orbital hybridization, lattice‐strained Pt‐based catalysts are promising for Li‐O 2 batteries. However, the formed lattice strains as a meta‐stable state are inclined to readily escape from the bulk crystal lattice to the edge, consequently deteriorating their activity and durability. Herein, how to construct a stable lattice strain poses a severe challenge. Here, an innovative atomic strain engineering‐driven approach is proposed to synthesize Pt 3 Co intermetallic nanoparticles confined on N‐doped carbon matrix via unsteady thermal shock and ultrafast crystallization strategy, which features rich kinetically well‐locked compressive strain (CS r ‐Pt 3 Co NPs@N‐C). Therein, the firmly trapped lattice distortion contributes to coordination environment modulation and local charge rearrangements, facilitating the stimulation of the Pt sites. The ordered L1 2 bulk configuration further benefits overall structural stability. Experimental and theoretical results demonstrate that the d ‐band center of the Pt sites in CS r ‐Pt 3 Co NPs@N‐C undergoes a negative shift, significantly optimizing the adsorption strength toward oxygen‐containing intermediates. This contributes to modulating the morphology and distribution characteristics of Li 2 O 2 . Specifically, the CS r ‐Pt 3 Co NPs@N‐C catalyst harvests an overpotential of 0.38 V and long‐term stability over 309 cycles at 200 mA g −1 . This work provides a new perspective on catalyst design for metal‐air batteries and beyond via atomic‐scale strain engineering.