Oxygen-Bridged Long-Range Dual Sites Boost Ethanol Electrooxidation by Facilitating C–C Bond Cleavage

Abstract

Optimizing the interatomic distance of dual sites to realize C–C bond breaking of ethanol is critical for the commercialization of direct ethanol fuel cells. Herein, the concept of holding long-range dual sites is proposed to weaken the reaction barrier of C–C cleavage during the ethanol oxidation reaction (EOR). The obtained long-range Rh–O–Pt dual sites achieve a high current density of 7.43 mA/cm 2 toward EOR, which is 13.3 times that of Pt/C, as well as remarkable stability. Electrochemical in situ Fourier transform infrared spectroscopy indicates that long-range Rh–O–Pt dual sites can increase the selectivity of C1 products and suppress the generation of a CO intermediate. Theoretical calculations further disclose that redistribution of the surface-localized electron around Rh–O–Pt can promote direct oxidation of −OH, accelerating C–C bond cleavage. This work provides a promising strategy for designing oxygen-bridged long-range dual sites to tune the activity and selectivity of complicated catalytic reactions.