Two-Dimensional Graphdiyne-Confined Platinum Catalyst for Hydrogen Evolution and Oxygen Reduction Reactions

Pt-based materials are the state-of-the-art catalysts for hydrogen evolution reaction (HER) and oxygen reduction reaction (ORR); however, there is still much room to improve the catalytic activity and enhance the stability of Pt-based catalysts. In this work, two-dimensional (2D) graphdiyne (GDY) with uniform distributed pores was applied to cover the Pt surface for catalyzing HER and ORR through density functional theory (DFT) calculations. The 2D confinement induced by GDY was found to improve the catalytic performance of the Pt catalyst from three aspects: (1) the 2D covering layer increases the stability of the Pt catalyst through forming the heterogeneous interface of GDY/Pt(111); (2) GDY/Pt(111) shows better catalytic activities of HER and ORR, with the smaller average overpotential values of 0.26 and 0.51 V, respectively, compared with those (0.29 V for HER, 0.62 V for ORR) on the Pt catalyst; (3) the confinement effect of GDY weakens the adsorption energy of CO to −1.81 eV (average value) from -2.14 eV on Pt(111), inhibiting CO poisoning. This work sheds new light on 2D confinement effects for HER and ORR, which opens up a new strategy for improving the catalytic performance of Pt-based catalysts.