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In this work, non-traditional metal-free polynitrogen chain N8− deposited on a nitrogen-doped carbon nanotubes (PN-NCNT) catalyst was successfully synthesized by a facile cyclic voltammetry (CV) approach, which was further tested in an oxygen reduction reaction (ORR). The formation of PN on NCNT was confirmed by attenuated total reflectance–Fourier transform infrared spectroscopy (ATR-FTIR) and Raman spectroscopy. Partial positive charge of carbon within NCNT facilitated electron transfer and accordingly induced the formation of more PN species compared to CNT substrate as determined by temperature-programmed decomposition (TPD). Rotating disk electrode (RDE) measurements suggested that a higher current density was achieved over PN-NCNT than that on PN-CNT catalyst, which can be attributed to formation of the larger amount of N8− on NCNT. Kinetic study suggested a four-electron pathway mechanism over PN-NCNT. Moreover, it showed long stability and good methanol tolerance, which indicates its great potential application. This work provides insights on designing and synthesizing non-traditional metal-free catalysts for ORR in fuel cells.

N8− Polynitrogen Stabilized on Nitrogen-Doped Carbon Nanotubes as an Efficient Electrocatalyst for Oxygen Reduction Reaction