Abstract

This study examines the effect of pretreatment and doping to enhance the ORR activity of multiwalled carbon nanotubes (MWCNTs). Melamine and thio-urea are chosen as precursors for mono and co-doping, respectively. A series of samples with pristine and pretreated CNTs are prepared and characterized physicochemically by Raman spectroscopy, X-ray photoelectron spectroscopy (XPS) and transmission electron microscopy (TEM) and electrochemically by cyclic voltammetry (CV) and linear sweep voltammetry (LSV). The obtained results show that co-doping is an effective way for improving ORR activity, due to the synergistic effect of N and S for changing the charge and spin density, respectively. Moreover, thio-urea favors the proportion of pyridinic and graphitic nitrogen configurations within doped samples. As a consequence, our synthesis method gives samples with superior ORR activity. The maximum ORR activity is obtained for NS-OX-CNTs which shows an over potential of 0.95 V vs RHE at 0.1 mA/cm2, which is comparable to Pt/C (0.98 V vs RHE). The electron transfer number (n) is calculated as 3.9 at 0.4 V which suggests that the ORR proceeds through a dominant 4 e− path. These comparable half-cell results to that of Pt/C pave the way for further testing as cathode materials for anion exchange membrane fuel cells (AEMFC).Graphical abstract

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