Abstract
Phosphorus and boron-doped palladium nanoparticles supported on carbon nanotubes (P-Pd/CNTs and B-Pd/CNTs, respectively) were prepared and evaluated for oxygen reduction reactivity (ORR) in alkaline environments. The prepared catalysts were characterized by X-ray diffraction (XRD), electron probe microanalysis (EMPA), and X-ray photoelectron spectroscopy (XPS). The ORR activity, methanol tolerance, and durability of the prepared catalysts were evaluated in oxygen-saturated 0.1 M potassium hydroxide electrolytes via cyclic voltammetry (CV) and linear sweep voltammetry (LSV) on rotating disk electrodes. The mechanisms and kinetics of ORR were discussed. The results show that P-Pd/CNTs exhibit higher ORR activity than B-Pd/CNTs and Pd/CNTs, higher methanol tolerance than commercial Pt/C, and excellent durability with 90% of the original activity maintained after 1000 voltage cycles. The ORR on P-Pd/CNTs proceeds via a 4-electron reduction process with O2 reduced to H2O directly, during which the rate-determining step is charge transfer at low overpotential and then changes to mass transport at high overpotential.
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