Synergistic Zn and MoS2 Tailored Co−N/C Environments Enabling Bifunctional ORR/OER Electrocatalysis for Advanced Li−O2 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@MoS₂ catalyst by tailoring the Co−N/C center with Zn incorporation and MoS₂ 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 MoS₂ 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−O₂ batteries, Zn and MoS₂ synergistically optimize intermediate interactions and regulate LiO₂ formation/decomposition, while Zn′s environmental adaptability and MoS₂′s encapsulating protection jointly enhance operational stability. Results show that ZnCo−N/C@MoS₂, serving as the oxygen electrode in Li−O₂ batteries, achieves a low overpotential of 1.01 V, an ultra-high specific capacity of 25,026 mAh g⁻¹, 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.