Synergistic Zn and MoS Tailored Co-N/C Environments Enabling Bifunctional ORR/OER Electrocatalysis for Advanced Li-O Batteries.

To better adapt lithium-oxygen batteries (LOBs) and overcome their sluggish oxygen reduction and evolution reactions (ORR/OER) kinetics, designing efficient bifunctional ORR/OER catalytic materials is essential. In this study, we successfully constructed a bifunctional ZnCo-N/C@MoS catalyst by tailoring the Co-N/C center with Zn incorporation and MoS encapsulation. Surprisingly, Zn atoms, which are typically considered to promote the Co atoms isolation, exhibit a promoting effect on the ORR performance of Co-N/C centers and enhance their stability under harsh conditions. Introducing MoS establishes Mo-N coupling centers, enhancing electron transfer and adjusting the charge density of Co active centers, thereby compensating OER activity limitation of ZnCo-N/C. In Li-O batteries, Zn and MoS synergistically optimize intermediate interactions and regulate LiO formation/decomposition, while Zn's environmental adaptability and MoS's encapsulating protection jointly enhance operational stability. Results show that ZnCo-N/C@MoS, serving as the oxygen electrode in Li-O batteries, achieves a low overpotential of 1.01 V, an ultra-high specific capacity of 25,026 mAh g, and a long cycle life of 298 cycles. This work achieves bifunctionality in single-atom catalysts through precise dual modulation of the catalytic environment, providing a novel strategy for the development of lithium-oxygen batteries.