Two-Dimensional Cobalt Sulfide/Iron–Nitrogen–Carbon Holey Sheets with Improved Durability for Oxygen Electrocatalysis

Transition-metal sulfide as a promising bifunctional oxygen electrocatalyst alternative to scarce platinum-group metals has attracted much attention, but it suffers activity loss over time owing to poor structural/compositional stability during catalysis. Herein, we report a self-template method for preparing a two-dimensional cobalt sulfide holey sheet superstructure with hierarchical porosity followed by the encapsulation of thin iron-nitrogen-carbon as a protective layer. The iron-nitrogen-carbon layer to some degree precludes the phase transition of cobalt sulfide underneath and preserves the structural integrity during catalysis, therefore rendering an exceptional durability in terms of no obvious activity loss after 10,000 cycles of the accelerated durability test. It also noticeably enhances the intrinsic activity of cobalt sulfide and does not influence its exposure into the electrolyte, resulting in showing an extraordinary electrochemical performance in terms of a potential difference of 0.69 V for the overall oxygen redox. A rechargeable zinc-air battery assembled by a cobalt sulfide/iron-nitrogen-carbon air cathode delivers approximately 4.2 times higher power density than that without an iron-nitrogen-carbon layer and stably operates for 300 h with a high voltaic efficiency. This work gives a facile and effective strategy for improving the long-term durability of transition-metal sulfide electrocatalysts.