Accelerating Triple Transport in Zinc‐Air Batteries and Water Electrolysis by Spatially Confining Co Nanoparticles in Breathable Honeycomb‐Like Macroporous N‐Doped Carbon

Rational engineering electrode structure to achieve an efficient triple-phase contact line is vital for applications such as in zinc-air batteries and water electrolysis. Herein, a facile "MOF-in situ-leaching and confined-growth-MOF" strategy is developed to construct a breathable trifunctional electrocatalyst based on N-doped graphitic carbon with Co nanoparticles spatially confined in an inherited honeycomb-like macroporous structure (denoted as Co@HMNC). The unique orderly arranged macroporous channels and the "ships in a bottle" confinement effect jointly expedite the triple transport, endowing the catalysts with fast reaction kinetics. As a result, the obtained Co@HMNC catalyst presents superb trifunctional performance with a positive half-wave potential (E1/2 ) of 0.90 V for oxygen reduction reaction (ORR), and low overpotentials of 318 and 51 mV for oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) at 10 mA cm-2 , respectively. The Co@HMNC-based liquid Zn-air battery reaches a large specific capacity of 859 mA h gZn-1 , a high-power density of 198 mW cm-2 , and long-term stability for 375 h, suggesting its promise for actual applications.