Exploration of Long-Life Pt/Heteroatom-Doped Graphene Catalysts in Hydrogen Atmosphere

[Image: see text] We investigated the H and H(2) adsorption effects on the stability of a Pt atom on various heteroatom-doped graphene supports using first-principles calculations based on density functional theory. We show that H and H(2) adsorptions on the Pt atom weaken the interaction between the Pt atom and graphene support and decrease the adsorption energy of Pt atoms. H(2) adsorption on Pt atoms decreases the adsorption energy of Pt atoms on all graphene supports by more than 30%, whereas H adsorption only affects pristine, O-, and S-doped graphene. These results indicate that the hydrogen atmosphere enhances the detachment of Pt catalysts. However, the B-, O-, Si-, P-doped, and monovacant graphene still maintained large adsorption energies of PtH and PtH(2) of more than 1.5 eV. In addition, the diffusion barriers of PtH and PtH(2) on pristine graphene were calculated to be less than 0.07 eV, which further demonstrated that H and H(2) enhance the degradation of Pt catalysts. Even after H and H(2) adsorptions on a Pt atom, O-, Si-, P-doped, and monovacant graphene still maintained large diffusion barriers of more than 1 eV. Therefore, we concluded that O-, Si-, and P-doped graphene are suitable supports for Pt catalysts in a hydrogen atmosphere.