Low‐Platinum Medium‐Entropy Intermetallic Compounds Based on the Synergistic Utilization of Spent Lithium‐Ion Batteries for High‐Efficiency Lithium–Oxygen Batteries

ABSTRACT The resource utilization of high‐value transition metals from traditional waste ternary lithium‐ion batteries holds significant appeal in the field of lithium–oxygen batteries, yet the diversification of utilization routes and the development of innovative strategies remain highly challenging. In this work, we propose for the first time a synergistic recycling strategy: recycling carbon (RC) from spent lithium‐ion battery anodes as a matrix, synergistically utilizing it with recovered transition metals from cathodes to prepare a low‐platinum, medium‐entropy intermetallic compound Pt(NiCoMn) 3 as a cathode catalyst. Both experimental and theoretical results demonstrate that the Joule heating alloying of recycled NiCoMn with Pt not only creates an ordered, medium‐entropy coordination environment within the low‐Pt intermetallic compound, inducing lattice distortion, but also triggers electron transfer from Ni/Co/Mn to highly electronegative Pt. This lattice distortion and local electron redistribution reposition the center of the Pt d‐band, while Ni/Co/Mn orbital hybridization with Pt optimizes the electronic structure of the catalytic center, promoting the deposition and decomposition kinetics of thin‐film Li 2 O 2 discharge products. Electrochemical testing shows that the Pt(NiCoMn) 3 @RC catalyst exhibits a low overpotential of 0.35 V and achieves a cycle life of 319 cycles at 400 mA g −1 and 1000 mAh g −1 .