Recycling the Spent LiNi1−x−yMnxCoyO2 Cathodes for High‐Performance Electrocatalysts toward Both the Oxygen Catalytic and Methanol Oxidation Reactions

Abstract The traditional recycling methods of the spent lithium ion batteries (LIBs) involve the intricate and cumbersome steps. This work proposes a facile method of acid leaching followed by the sulfurization treatment to achieve the high Li leaching efficiency, and obtain high‐performance multi‐function electrocatalysts for oxygen reduction (ORR), oxygen evolution (OER), and methanol oxidation reactions (MOR) from the spent LIB ternary cathodes. By this method, the Li leaching efficiency from the spent LIB ternary cathode can reach 98.3%, and the transition metal sulfide heterostructures (LNMCO‐H‐450S) consisting MnS, NiS 2 , and NiCo 2 S 4 phases can be obtained. LNMCO‐H‐450S shows the superior bifunctional oxygen catalytic activities with ORR half‐wave potential of 0.763 V and OER potential at 10 mA cm −2 of 1.561 V, surpassing most of the state‐of‐the‐art electrocatalysts. LNMCO‐H‐450S also demonstrates the superior MOR catalytic activity with the potential at 100 mA cm −2 being 1.37 V. Using LNMCO‐H‐450S as the oxygen catalyst, this work can construct the aqueous and solid‐state zinc‐air batteries with high power density of 309 and 257 mW cm −2 , respectively. This work provides a promising strategy for the efficient recovery of Li, and reutilization of Ni, Co, and Mn from the spent LIB ternary cathodes.