Bimetallic Pd-Co Nanoparticles Supported on Nitrogen-Doped Reduced Graphene Oxide as Efficient Electrocatalysts for Formic Acid Electrooxidation

Abstract

In this work, bimetallic PdxCoy nanoparticles supported on nitrogen-doped reduced graphene oxide catalysts were synthesized and tested for formic acid oxidation as potentially efficient and durable electrocatalysts. Graphene oxide was nitrogen doped through hydrothermal chemical reduction with urea as a nitrogen source. The PdxCoy nanoparticles were deposited on the nitrogen-doped graphene oxide support using the impregnation-reduction method with sodium borohydride as a reducing agent and sodium citrate dihydrate as a stabilizing agent. The structural features, such as phases, composition, oxidation states, and particle sizes, of the nanoparticles were characterized using X-ray diffraction, transmission electron microscopy, scanning electron microscopy–energy-dispersive X-ray spectroscopy, and X-ray photoelectron spectroscopy. The Pd nanoparticle sizes in Pd1Co1/N-rGO, Pd/N-rGO, and Pd1Co1/CNT were 3.5, 12.51, and 4.62 nm, respectively. The electrochemical performance of the catalysts was determined by CO stripping, cyclic voltammetry, and chronoamperometry. Pd1Co1/N-rGO showed the highest mass activity of 4833.12 mA–1 mg Pd, which was twice that of Pd1Co1/CNT. Moreover, Pd1Co1/N-rGO showed a steady-state current density of 700 mA–1 mg Pd after 5000 s in chronoamperometry carried out at +0.35 V. Apart from the well-known bifunctional effect of Co, nitrogen-doped graphene contributed to the performance enhancement of the Pd1Co1/N-rGO catalyst.