Co‐doping‐induced electronic reconfiguration of nanosized ZnS for facilitating oxygen reduction reaction in flexible aluminum–air batteries

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The development of high‐performance and cost‐efficient catalysts holds great significance in facilitating oxygen reduction reaction (ORR), which is a pivotal process in next‐generation energy storage devices, such as aluminum–air batteries. Transition metal sulfides have been proposed as promising non‐noble metal ORR catalysts. However, achieving platinum (Pt)‐comparable activity remains a challenge. Herein, a Co‐doping‐triggered electronic reconfiguration strategy is reported to tune the charge distribution and coordination state of ZnS nanoparticles anchored on N, S co‐doped carbon (ZnS/NSC), thereby optimizing the intermediate adsorption kinetics and promoting ORR activity. The half‐wave potential of 0.87 V as well as 100‐h continuous durability are obtained by Co‐doped ZnS/NSC in alkaline media. In addition, the solid‐state aluminum–air battery is further assembled by using Co‐doped ZnS/NSC as a cathode catalyst, achieving a maximum peak density of 100 mW·cm −2 and discharge duration over 55 h. Density functional theory (DFT) calculations reveal that high electronegative Co‐doping is beneficial for the construct of charge‐transfer avenue and optimization of intermediate adsorption procedure. This study presents an efficient approach for preparing metal sulfides with high catalytic activity toward ORR in flexible metal–air batteries.