Design the PdCu/TaN C electrocatalyst with core-shell structure having high efficiency for methanol and formic acid oxidation reactions

Abstract For the first time, PdCu/TaN C catalyst with a special core-shell structure is assembled, which exhibits high catalytic performance for methanol oxidation reaction (MOR) in alkaline medium (1326.95 A gPd−1) and formic acid oxidation reaction (FAOR) in acidic medium (1052.63 A gPd−1), 6.3 and 4.9 times those of the commercial Pd/C, respectively. According to the results of Tafel, Electrochemical Impedance Spectroscopy (EIS), CO stripping and chronoamperometry (CA), it is revealed that the reaction kinetics, anti-CO poisoning ability and stability of PdCu/TaN C for MOR and FAOR are all enhanced significantly. Density Functional Theory (DFT) calculations also indicate that the adsorption intensity of CO is weakened and the binding intensity of OH is enhanced on the Pd3Cu1/TaN(001) surface, which are beneficial to the removal of adsorbed CO and enhancement of the anti-CO poisoning ability. Combined with the characterization analysis and theoretical calculations, the good catalytic performance of PdCu/TaN C for MOR and FAOR can be attributed to the unique electronic structure and morphology from the effective interface, geometric effects and proper d-band center.