Accelerating hydrogen-species migration induced by fullerene to attain promoting ethanol oxidation

Abstract

Accelerating the migration of hydrogen species during ethanol oxidation is crucial for regenerating active sites on catalyst surfaces. Herein, we report a composite catalyst (Pd/EDAC 60 @CNTs) comprising ethylenediamine-modified fullerene supported on carbon nanotubes with anchored Pd nanoparticles. For the ethanol oxidation reaction, this catalyst delivers a high mass activity of 2183.7 mA mg −1 , approximately three times that of commercial Pd/C (712.6 mA mg −1 ), alongside significantly enhanced CO tolerance (onset potential shifted negatively by 48 mV) and excellent long-term stability (64.4% retention after 500 cycles). The superior performance arises from synergistic effects: the high-curvature C 60 promotes hydrogen spillover via π-electron localization and sp 3 hybridization, regenerating Pd active sites; the interfacial electronic interaction downshifts the Pd d-band center, weakening intermediate adsorption; and the nitrogen-containing anchors effectively suppress Ostwald ripening of Pd NPs. This work provides a promising strategy for designing high-performance electrocatalysts through hydrogen spillover and support engineering.