Abstract
Pt-based catalysts are the most active materials for the oxygen reduction reaction in Zn-air batteries; however, most Pt-based catalysts are unfavorable for the adsorption of OOH* intermediates, which hampers battery efficiency. To address this, a strategy for precisely constructing Pt-Co alloy atomic configurations enables the immobilization and controlled release of OOH* intermediates during the four-electron O2 reduction reaction. Using the synthetic Pt1Co alloy nanoparticles encapsulated in N-doped carbon nanotubes (Pt1Co-NP@NCNTs) as an example, characterization via synchrotron-radiation X-ray absorption fine structure and high-angle annular dark-field scanning transmission electron microscopy confirms that Pt single atoms are uniformly dispersed on Co nanoparticles. In situ attenuated total reflectance-surface enhanced infrared absorption spectroscopy further verifies that these Pt1Co alloy nanoparticles facilitate the immobilization of OOH* intermediates and the release of OH* intermediates, ensuring efficient H2O production through the four-electron pathway. As a result, the Pt1Co-NP@NCNTs exhibit outstanding oxygen reduction reaction activity with a high half-wave potential of 0.90 V vs. RHE, and when integrated into Zn-air batteries, they deliver a high power density of 141 mW cm-2 and an ultralong lifespan exceeding 300 hours at 10 mA cm-2, outperforming most Pt-based electrocatalysts in rechargeable Zn-air batteries.

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