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HighlightsSingle-atom M-N 4 /N-doped carbons (M = Fe, Co) prepared as OER/ORR catalysts.    Ultrasonication-assisted plasma engineering used for catalyst synthesis.    Co-N 4 /NC outperformed benchmark commercial catalysts in practical Zn–air battery test.    DFT calculations provided insights into the origin of superior ORR/OER performance.Supplementary Information  The online version contains supplementary material available at 10.1007/s40820-020-00581-4

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Ultrasonic Plasma Engineering Toward Facile Synthesis of Single-Atom M-N4/N-Doped Carbon (M = Fe, Co) as Superior Oxygen Electrocatalyst in Rechargeable Zinc–Air Batteries