Upcycling Spent Lithium‐Ion Batteries: Constructing Bifunctional Catalysts Featuring Long‐Range Order and Short‐Range Disorder for Lithium‐Oxygen Batteries

Abstract Upcycling of high‐value metals (M = Ni, Co, Mn) from spent ternary lithium‐ion batteries to the field of lithium‐oxygen batteries is highly appealing, yet remains a huge challenge. In particular, the alloying of the recovered M components with Pt and applied as cathode catalysts have not yet been reported. Herein, a fresh L1 2 ‐type Pt 3 M medium‐entropy intermetallic nanoparticle is first proposed, confined on N‐doped carbon matrix (L1 2 ‐Pt 3 (Ni 1/3 Co 1/3 Mn 1/3 )@N‐C) based on spent 111 typed LiNi 1‐x‐y Mn x Co y O 2 cathode. This well‐defined catalyst combines both features of long‐range order L1 2 face‐centered cubic structure and short‐range disorder in M sites. The former contributes to enhancing the structural stability, and the latter further facilitates deeply activating the catalytic activity of Pt sites. Experiments and theoretical results demonstrate that the local coordination environment and electronic distribution of Pt are both fundamentally modulated via surrounding disordered Ni, Co, and Mn atoms, which greatly optimize the affinity toward oxygen‐containing intermediates and facilitate the deposition/decomposition kinetics of the thin‐film Li 2 O 2 discharge products. Specifically, the L1 2 ‐Pt 3 (Ni 1/3 Co 1/3 Mn 1/3) @N‐C catalyst exhibits an ultra‐low overpotential of 0.48 V and achieves 220 cycles at 400 mA g −1 under 1000 mAh g −1 . The work provides important insights for the recycling of spent lithium‐ion batteries into advanced catalyst‐related applications.