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

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, NiS2, and NiCo2S4 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.

Promoting the four electrocatalytic reactions of OER/ORR/HER/MOR using a multi-component metal sulfide heterostructure for zinc-air batteries and water-splitting.

Multi-component metal sulfide heterostructures are promising for multi-functional catalytic activities. In this work, we fabricated a multi-component metal sulfide heterostructure (Co-S-INF, composed of Co3S4 and (Fe, Ni)9S8) with nanoflower morphology clustered with numerous nanosheets by the electrodeposition of cobalt on iron-nickel foam followed by hydrothermal sulfurization treatment. Co-S-INF possesses high multi-functional electrocatalytic properties toward the oxygen evolution reaction (OER), oxygen reduction reaction (ORR), hydrogen evolution reaction (HER), and methanol oxidation reaction (MOR). In particular, the ORR potential at 10 mA cm-2 is 0.682 V, and the OER, HER, and MOR potentials at 100 mA cm-2 are 1.478 V, 0.289 V, and 1.417 V, respectively. By using Co-S-INF, the aqueous ZAB with an ultrahigh peak power density of 332.30 mW cm-2 and an overall water splitting (OWS) device with a low splitting voltage of 1.82 V at 100 mA cm-2 can be obtained. In addition, the OWS potential can be further decreased to 1.70 V at a current density of 100 mA cm-2 with the assistance of MOR at the anode accompanying the production of the high value-added formate. Our work opens the way for the application and development of multi-functional electrocatalysts.