Abstract
Developing efficient and stable transition metal oxygen evolution reaction (OER) catalysts is crucial for clean energy technologies, while recycling spent lithium‐ion batteries (LIBs) faces challenges of high energy consumption and low added value. Herein, we propose a green strategy to recover valuable metals from spent LIBs and convert them into high‐performance OER catalysts. Using spent LiNi
0.33
Co
0.33
Mn
0.33
O
2
(NCM111) cathodes as raw material, metal ions were extracted by acid leaching, followed by a one‐step hydrothermal synthesis on nickel foam to fabricate a MnFeCoNiCu metal–organic framework catalyst (MFCNC‐
X
). The results demonstrate that MFCNC‐150 synthesized at 150 °C exhibits a unique petal‐like stacked morphology, high specific surface area, and excellent hydrophilicity. Benefiting from the regulation of the electronic structure induced by the multi‐metal synergistic effect and interactions among multi‐metal active sites, MFCNC‐150 exhibits outstanding OER activity in 1 M KOH electrolyte, with an overpotential of only 237 mV at a current density of 10 mA cm
−2
, a Tafel slope of 56.35 mV dec
−1
, and long‐term stability exceeding 120 h. Electrochemical characterization and post‐reaction analysis reveal surface restructuring during OER process, forming active metal hydroxide sites. This work offers novel insights for high‐value recycling of spent LIBs and development of efficient transition metal OER catalysts.