C‒C Bond Cleavage Driven by Lattice Oxygen during Ethanol Oxidation Process

The capacity of C‒C bond cleavage determines the pathway selectivity during the ethanol oxidation process. Herein, ultra-thin monodisperse PdCo nanosheets with an average diameter of 33 nm are successfully synthesized and the interface of Pd-O-Co is further constructed due to the introduction of lattice oxygen. Due to their ultra-thin nanosheet structure, unique surface electronic structures driven by lattice oxygen, and alloying effect, the prepared PdCo/Pd-O-Co nanosheets (PdCo/Pd-O-Co NSs) show excellent ethanol oxidation reaction (EOR) activity and stability. The mass activity and specific activity of PdCo/Pd-O-Co NSs are 12.43 A mg −1 and 22.01 mA cm −2 for EOR, which exceeded PdCo nanosheets, Pd nanosheets and commercial Pd black. In situ FTIR spectroscopy and theoretical calculation identified that lattice oxygen introduced after square-wave potential treatment can promote the cleavage of the C‒C bond. Through the introduction of lattice oxygen combined with lattice strain engineering, the PdCo/Pd-O-Co NSs surface is optimized to promote the generation of strong p-d orbital hybridization, which led to the upward shift of the d-band center and the electron delocalization effect, effectively promoting the C‒C bond cleavage and improving the anti-poisoning ability.