LAUSR

Transition-metal sulfide is pursued for replacing scare platinum-group metals for oxygen electrocatalysis and is of great importance in developing low-cost, high-performance rechargeable metal-air batteries. We report herein a facile cationic-doping strategy for preparing nickel-doped cobalt sulfide embedded into a mesopore-rich hydrangea-like carbon nanoflower. Nickel cations are introduced to induce the formation of Co3+-active species and more oxygen vacancies due to higher electronegativity and smaller ionic radius, thereby strengthening the intrinsic activity for oxygen electrocatalysis. Moreover, hydrangea-like superstructure composed of interconnected carbon cages provides abundant accessible active sites and hierarchical porosity. As a result, it shows excellent catalytic performance with a superior mass activity for the oxygen reduction reaction to the state-of-the-art Pt/C catalyst and a low overpotential of 314 mV at 10 mA cm-2 for the oxygen evolution reaction. When used as an air cathode for the rechargeable Zn-air battery, it delivers a peak power density of 96.3 mW cm-2 and stably operates over 214 h. This work highlights the importance of cationic doping in strengthening the electrocatalytic performance of 3d-transition-metal chalcogenides.