Oxygen reduction reaction on Pd nanoparticles supported on novel mesoporous carbon materials

Abstract

In this work three mesoporous nitrogen-doped carbon support materials were evaluated for oxygen reduction reaction (ORR) in comparison to Vulcan carbon in 0.1 M KOH and 0.5 M H2SO4 solutions. Palladium nanoparticles were synthesised using citrate method and the average particle size of 3.9 ± 0.6 nm was obtained, which was determined from transmission electron microscopy (TEM) images. Unique porosities of these mesoporous engineered catalyst supports (ECS) were evaluated using the BET method and all of the materials displayed similar microporosity, altrough mesopore distribution varied greatly between these materials. Three different loadings of the Pd catalyst were applied to the support materials (varying between 20-40 wt% of Pd) to evaluate the support ability to disperse a large amount of Pd. By comparing the 40 wt% Pd loaded ECS-003604 and Vulcan XC-72R it can be noted that the Vulcan carbon-supported Pd catalyst is more agglomerated. The agglomeration of this catalyst is also noticeable from cyclic voltammetry (CV) studies, where the PdO reduction peak shifts to more positive values as compared to the mesoporous Pd/C counterparts. The ORR kinetics were explored using the rotating disc electrode (RDE) method. In acidic media a Pd catalyst supported on a bimodal mesoporous ECS material showed highest specific activity for oxygen electroreduction, while in alkaline the activity difference is less noticeable between the Pd-based electrocatalyst materials. One of the mesoporous N-doped carbon supported Pd catalyst was also compared to Pd/Vulcan cathode in single-cell alkaline anion exchange membrane fuel cell and improved peak power density was observed.