Precise control of platinum coordination environment on fullerene-derived catalysts for oxygen reduction reaction

The interaction between catalysts and supports is recognized as a crucial factor influencing catalytic activity and stability. However, the carbon materials, which have been widely employed as the support at present, encounter challenges including intricate composition and the difficulty of precise control. In this study, the fullerene-derived carbon materials serve as support to electrocatalysts with low platinum. Fullerene-based materials, as the only carbon material with a well-defined molecular structure, have a controllable active site structure, which can provide a reaction model for studying metal-support interactions. Four kinds of fullerene-derived catalysts such as Pt/fullerene, Pt/nitrogen-doped fullerene, Pt/sulfur-doped fullerene, and Pt/phosphorus-doped fullerene, were synthesized. Once the coordination environment of the Pt particles was controlled, thus their catalytic performance was modulated. Despite a platinum loading of only 4.2%, Pt/N-fullerene demonstrates superior oxygen reduction activity and stability compared to commercial Pt/C (20%). Density functional theory calculations show that the introduction of heteroatoms can change the surface charge distribution of fullerenes, in which N-fullerene has a more negative electrostatic potential and can effectively anchor Pt. This research establishes a foundation for understanding the catalysts-support interaction and further precise control of the coordination environment of Pt. This provides new insights for designing efficient ORR catalysts