Theoretical Study Of Stabilities, Electronic And Catalytic Performance Of Supported Platinum On Modified Graphene

Supported platinum nanoparticles have been widely used as electrochemicalcatalysts for direct methanol fuel cells (DMFCs) due to their environment-friendlycharacteristic. Graphene has been considered as one of the most promising candidateas the support for metal nanoparticles due to its fascinating thermal, mechanical andelectrical properties originating from the two-dimensional honeycomb atomicstructure. The high catalytic efficiency of single Pt atom has been confirmed byexperimental work. Moreover, introducing defects to graphene could efficientlypromote its efficiency. The geometry, electronic structure, and catalytic properties forCO oxidation of Pt atom supported on pri-graphene(PG), Haeckelite(H) andStone-Wales-defect-Graphene(SWG) are investigated by DFT calculations. Incontrast to a Pt atom on PG, the defective graphene, especially the Haeckelite,strongly stabilizes the Pt atom and makes it more positive and thus alleviating the COpoisoning. The investigation of adsorbed CO and O2further confirmed the defect ingraphene improved the CO tolerance of the systems. In the end, we calculated thepathway of CO oxidation in three systems. The results showed that theLangmuir-Hinshelwood (LH) reaction of CO+O2â†'CO2+O is favoured as the firststep, and followed by the Eley-Rideal (ER) reaction of CO+Oâ†'CO2. Moreover,the catalytic activities for defective systems are as high as the pristine one. The resultsindicate the benefit of Haeckelite as substrate for Pt atom, and validate the reactivityof catalysts on the atomic-scale with low cost and high activity.