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The defect and N-doping engineering are critical to developing the highly efficient metal-free electrocatalysts for oxygen reduction reaction (ORR), mainly because they can efficiently regulate the geometric/electronic structures and sur-/interface properties of the carbon matrix. Herein, we provide a facile and scalable strategy for the large-scale synthesis of N-doped porous carbon nanosheets (NPCNs) with hierarchical pore structure, only involving solvothermal and pyrolysis processes. Additionally, the turnover frequency of ORR (TOF ORR ) was calculated by taking into account the electron-transfer number ( n ). Benefiting from the trimodal pore structures, high specific surface area, a higher pore volume, high-ratio mesopores, massive vacancies/long-range structural defects, and high-content pyridinic-N (~2.1%), the NPCNs-1000 shows an excellent ORR activity (1600 rpm, j  s = ~5.99 mA cm -2 ), a selectivity to four-electron ORR (~100%) and a superior stability in both the three-electrode tests (CP test for 7500 s at 0.8 V, Δ j  s = ~0.58 mA cm -2 ) and Zn-Air battery (a negligible loss of 0.08 V within 265 h). Besides, the experimental results indicate that the enhancement of ORR activity mainly originates from the defects and pyridinic-N. More significantly, this work is expected to realize green and efficient energy storage and conversion along with the carbon peaking and carbon neutrality goals.

2D Zinc-Based Metal–Organic Complexes Derived N-Doped Porous Carbon Nanosheets as Durable Air Cathode for Rechargeable Zn–Air Batteries