N, P-Codoped Graphene Dots Supported on N-Doped 3D Graphene as Metal-Free Catalysts for Oxygen Reduction

ACS Appl Mater Interfaces. 2021 Jul 7;13(26):30512-30523. doi: 10.1021/acsami.1c03141. Epub 2021 Jun 25.

Abstract

Nitrogen and phosphorus-codoped graphene dots supported on nitrogen-doped three-dimensional graphene (N, P-GDs/N-3DG) have been synthesized by a facile freeze-annealing process. On the surface of the 3D interconnected porous structure, the N, P-GDs are uniformly dispersed. The as-prepared N, P-GDs/N-3DG material served as a metal-free catalyst for oxygen reduction reaction (ORR) in an alkaline medium and evaluated by a rotating ring-disk electrode. The N, P-GDs/N-3DG catalyst exhibits excellent ORR activity, which is comparable to that of the commercial Pt/C catalyst. Furthermore, it exhibits a higher tolerance to methanol and better stability than the Pt/C. This enhanced electrochemical catalytic performance can be ascribed to the presence of abundant functional groups and edge defects. This study indicates that P-N bonded structures play a vital role as the active sites in ORR.

Keywords: 3D graphene; graphene dots; heteroatom doping; nitrogen-doped; oxygen reduction reaction (ORR); phosphorus-doped.