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In this study, we have developed a one-step fabrication method for N and P codoped vertical graphene (NPVG) films as highly efficient electrocatalysts for the oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) in rechargeable Zn-air batteries. Nitrogen gas and black phosphorus (BP) were used as the doping precursors, which were dissociated and ionized into plasma species containing N and P during the HPECVD process. This in-situ doping process was monitored using optical emission spectrometers. The co-doping of N and P occurred through the formation of N, P substitution and BP crystal domains facilitated by reactive plasma radicals. This is different from conventional dopants that utilize a conventional precursor process. The presence of reactive plasma radicals enabled a more efficient and precise co-doping method, leading to improved performance and unique material properties.

The resulting NPVG films exhibited electron accumulation from the base to the edges, inducing localized electric field enhancement, lower charge transfer barriers, and enhanced bifunctional performance. As a result, the Zn-air battery based on NPVG demonstrated a high peak power density of 164.3 mW cm-2 with excellent cycling stability over 500 hours at a charge-discharge current density of 10 mA cm-2. This performance surpassed that of benchmark cathodes and rivaled recently reported data for cathode catalysts with the same mass loading.

Overall, this work presents a novel and efficient approach for the fabrication of NPVG films, which show great promise for enhancing the performance of rechargeable Zn-air batteries.