Abstract
Platinum group metal (PGM)-free oxygen reduction reaction (ORR) catalysts are of utmost importance for the rapid development of anion-exchange membrane fuel cell (AEMFC) technology. In this work, we demonstrate the improved ORR performance and stability of Co and Fe oxide-decorated/N-doped reduced graphene oxide (CoOx-Fe3O4/N-rGO) prepared via a hydrothermal method at the low temperature of 150 °C. The catalysts were characterized thoroughly using transmission electron microscopy, high-angle annular dark field-scanning electron microscopy, X-ray diffraction, N2 physisorption, Raman spectroscopy, and X-ray photoelectron spectroscopy to obtain information about morphology, elemental distribution, phases, porosity, defects, and surface elemental compositions. Significant ORR activity improvement (130 mV@-1.5 mA cm−2) was achieved with this catalyst compared to the pristine graphene oxide, and the ORR limiting current was even 12%@0.5 V higher than the commercial Pt/C. The enhanced ORR activity of CoOx-Fe3O4/N-rGO was attributed to the uniform dispersion of Co, Fe, and N on reduced graphene oxide (rGO) sheets. Furthermore, ORR accelerated stress tests revealed excellent durability, suggesting that this material could be a promising and durable catalyst. With a cathode layer of the CoOx-Fe3O4/N-rGO catalyst, we achieved a peak power density of 676 mW cm−2 in an operando H2-O2 AEMFC. To the best of our knowledge, this is the highest reported power density per cathode catalyst mass in a reported PGM-free cathode catalyst. Finally, we quantified the various cell polarization losses as a function of cathode catalyst loadings to obtain insights for future work with AEMFCs based on this catalyst. The improvement in the AEMFC performance using CoOx-Fe3O4/N-rGO as a cathode catalyst can be attributed to the synergistic effects of (i) the high turnover frequency of the transition metals (Co and Fe) for ORR and (ii) the enhancement provided by N doping to the metal distribution and stability.