ACS Nano 2025, 19, 18, 17589–17605
Upcycling Spent Cathodes from Li–Ion Batteries into a High-Entropy Alloy Catalyst with Reverse Electron Transfer for Li–O2 Batteries
Peng Wang*, Shan Guo, Yongbin Xu, Xinyi Yuan, Yu Tian, Binchao Xu, Zhijun Zhao, Yuxiao Wang, Jianwei Li, Xiaojun Wang, Zhiming Liu*
We report a general synthesis of ultrafine αNiCoMn (α = Pt, Ir, Ru) high-entropy alloy (HEA) nanoparticles anchored on a nitrogen-doped carbon (N–C) support through a facile one-step Joule heating, which serves as a high-efficiency catalyst for Li–O2 batteries. Solution alloying of recycled NiCoMn with Pt group metals facilitates catalytic efficiency through 3d–5d electronic interactions and the high-entropy assembly effect. Both experimental and calculation results reveal that, driven by rapid, nonequilibrium thermal shock, electron transfer defies conventional expectations, where the electrons are inclined to transfer from the higher electronegative Pt to the surrounding NiCoMn atoms. This interesting reverse local charge redistribution and orbital hybridization endow Pt with an elevated d-band center and an optimized electronic structure.