Photochemical Solid-Phase Synthesis of Platinum Single Atoms on Nitrogen-Doped Carbon with High Loading as Bifunctional Catalysts for Hydrogen Evolution and Oxygen Reduction Reactions

Currently, Pt single atoms as promising electrocatalysts have been applied to electrocatalysis aiming to significantly improve performance and remarkably lower usage of the noble metal. Herein, we propose a photochemical solid-phase reduction method to fabricate well-defined isolated Pt atoms on a nitrogen-doped porous carbon (Pt1/NPC). Using this simple and fast synthesis strategy, the formed Pt atoms are well-dispersed on the carbon without clusters or nanoparticles. The loading of the Pt is up to 3.8 wt % relative to the carbon. The Pt1/NPC catalyst displays an ultrahigh electrocatalytic activity for hydrogen evolution reaction with an overpotential of 25 mV at the current density of 10 mA cm–2 and mass activity of 2.86 A mg–1 Pt (24-times higher than a commercial Pt/C). Moreover, the catalyst also presents efficient catalytic activity for the oxygen reduction reaction. Its mass activity is 4.3-times that obtained by a commercial Pt (20 wt %). The improved electrocatalytic activities of the Pt1/NPC catalyst are ascribed to the favorable chemical and electronic structure of the Pt–N4 coordination raised by strong electron transfer from the isolated Pt atoms to the coordinated N atoms in this catalyst. The Pt1/NPC can be employed as a bifunctional catalyst for fuel cells and hydrogen production.