Carbon Monoxide-Tolerant Platinum Nanoparticle Catalysts on Defect-Engineered Graphene

We studied catalytic performance, particularly tolerance against CO poisoning and particle migration, of Pt nanoparticles dispersed on graphene using ab initio calculations. It was shown that the binding of Pt nanoparticles to graphene and the molecular adsorption on Pt can be controlled by introducing defects on graphene. Pt d-band center is a key parameter that is tailored by such defect formation. It is observed that the binding energy difference between H2 and CO is well correlated with the d-band center, whereas individual H2 and CO binding energies are not. Relative occupation ratio of H2 on Pt in a CO environment showed that Pt nanoparticles can tolerate CO more than does bulk Pt when the particles are deposited on nitrogen-doped graphene.