Ultrasonic Plasma Engineering Toward Facile Synthesis of Single?Atom M?N4/N?Doped Carbon (M = Fe, Co

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As bifunctional oxygen evolution/reduction electro-catalysts, transition-metal-based single-atom-doped nitrogen–carbon (NC) matrices are promising successors of the corresponding noble-metal-based catalysts, offering the advantages of ultrahigh atom utili-zation efficiency and surface active energy. However, the fabrication of such matrices (e.g., well-dispersed single-atom-doped M-N4/NCs) often requires numerous steps and tedious processes. Herein, ultra-sonic plasma engineering allows direct carbonization in a precursor solution containing metal phthalocyanine and aniline. When combin-ing with the dispersion effect of ultrasonic waves, we successfully fabricated uniform single-atom M-N4 (M = Fe, Co) carbon catalysts with a production rate as high as 10 mg min?1. The Co-N4/NC pre-sented a bifunctional potential drop of ΔE = 0.79 V, outperforming the benchmark Pt/C-Ru/C catalyst (ΔE = 0.88 V) at the same catalyst loading. Theoretical calculations revealed that Co-N4 was the major active site with superior O2 adsorption–desorption mechanisms. In a practical Zn–air battery test, the air electrode coated with Co-N4/NC exhibited a specific capacity (762.8 mAh g?1) and power density (101.62 mW cm?2), exceeding those of Pt/C-Ru/C (700.8 mAh g?1 and 89.16 mW cm?2, respectively) at the same catalyst loading. Moreo-ver, for Co-N4/NC, the potential difference increased from 1.16 to 1.47 V after 100 charge–discharge cycles. The proposed innovative and scalable strategy was concluded to be well suited for the fabrication of single-atom-doped carbons as promising bifunctional oxygen evolution/reduction electrocatalysts for metal–air batteries.
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