Powering the Future: A Cobalt‐Based Catalyst for Longer‐Lasting Zinc–Air Batteries

Abstract The development of cost‐effective catalysts for zinc–air batteries (ZABs) remain challenging due to the sluggish kinetics of oxygen reduction (ORR) and evolution (OER) at the cathode. In this context, a novel N‐doped graphitic shell‐encapsulated cobalt catalyst is presented as an air electrode with exceptional bifunctional activity, achieving an ORR half‐wave potential ( E _1/2 ) of 0.81 V and an OER overpotential of 349 mV in an alkaline medium. The catalyst demonstrated excellent cycling durability and delivered superior power density in both liquid and solid‐state ZABs. Furthermore, a quasi‐solid‐state ZAB is assembled with the catalyst, and it maintained a stable open‐circuit voltage (OCV) of 1.360 V for >10 000 s. The catalyst achieved a peak power density of 127 mW cm ⁻² —significantly outperforming the benchmark Pt/C + RuO ₂ system (74 mW cm ⁻² ). When two tandem‐junction ZABs are connected in series, they achieved an OCV of 2.75 V and powering a “ZAB” LED strip and a mini fan. Furthermore, Density Functional Theory (DFT) calculations revealed that the enhanced performance resulted from optimized binding energies between the Co@N(py) active sites and reaction intermediates. An in situ Raman study is carried out to understand the catalytic mechanism through transient intermediate detection.