Development of a highly active electrocatalyst via ultrafine Pd nanoparticles dispersed on pristine graphene.

A unique synthesis was developed to immobilize Pd nanoparticles on pristine graphene (PG) sheets via a facile supercritical carbon dioxide route. Pristine graphene was obtained by sonication-assisted exfoliation of graphite in an organic solvent. Finely dispersed worm-like Pd nanoparticles are homogeneously deposited on the hydrophobic graphene surfaces. The combination of pristine graphene sheets and well-dispersed Pd nanoparticles provided large electrochemically active surface areas (ECSA) for both direct formic acid fuel cell (DFAFC) and methanol fuel cell (DMFC). The ECSA values are more than twice as large as those of reduced graphene oxide and carbon nanotube based counterparts or six times those of conventional XC-72 carbon black. Significant enhancements were also observed in the electrocatalytic activity and stability measurements. The excellent electrochemical property of Pd/PG is attributable to the well-preserved graphene structure that ensures electrical conductivity and stability of the composite. Its large surface area also allows for the deposition of small size and high dispersion of the Pd nanoparticles. This straightforward synthesis offers a new pathway for developing highly active electrocatalysts based on pristine graphene with fully optimized properties.