Efficiently Re‐Utilizing the High‐Value Metals in the Spent LiNi _1−x−y Mn _x Co _y O ₂ for the Trifunctional Electrocatalysts by a Novel One‐Pot Method

Abstract Traditional hydrometallurgy methods for recycling the spent lithium‐ion battery materials face some challenges, including the complex processes, and difficulties in separating Ni/Co/Mn. To address these issues, this work proposes a simple one‐pot method to achieve a high Li leaching efficiency (99.2%) and simultaneously transform the majority of Ni (99.5%) and Co (99.9%) into a high‐performance multifunctional electrocatalyst (LNMCO‐HS‐180). LNMCO‐HS‐180 with single‐phase structure shows a hollow microsphere morphology. LNMCO‐HS‐180 can efficiently catalyze the oxygen reduction (ORR), oxygen evolution (OER), and methanol oxidation reactions (MOR), with the ORR half‐wave potential of 0.732 V and, OER potential of 1.469 V at 10 mA cm ⁻² . This is mainly attributed to the unique hollow microsphere morphology, suitable Ni/Co/Mn oxidation states, and reduction in the free energy barriers for OER and ORR. Additionally, LNMCO‐HS‐180 exhibits an MOR potential of only 1.43 V at 100 mA cm ⁻² and excellent formate selectivity (>99%).