The effect of GGA functionals on the oxygen reduction reaction catalyzed by Pt(111) and FeN4 doped graphene.

The effect of different generalized gradient approximation (GGA) functionals (BLYP, PW91, PBE, and RPBE) on the oxygen reduction reaction (ORR) catalyzed by Pt(111) and FeN4 doped graphene was investigated. The results indicate that all of the screened GGA functionals are accurate enough to calculate the property of isolated ORR species. However, the calculated results of the ORR on the catalyst surface are greatly affected by the choice of functional. For Pt(111) catalyst, PW91 and PBE proved to be better functionals to investigate ORR on its surface, while for FeN4-doped graphene, BLYP was demonstrated to be the most suitable functional to study the electrocatalytic ORR properties, based on analyzing the adsorption of ORR species, reaction energies of ORR steps, and the adsorption structure of the O2 molecule. Graphical abstract Effects of generalized gradient approximation (GGA) functionals on oxygen reduction reactions (ORR).