The catalytic activities of FexPt100-x alloy nanoparticles at different compositions (x=10, 15, 42, 54, 58, and 63) in the electro-oxidation of formic acid have been investigated by using cyclic voltammetry (CV), chronoamperometry, and electrochemical impedance spectroscopy (EIS). It was observed that the electrocatalytic performance was strongly dependent on the FePt particle composition. In chronoamperometric measurements, the alloy particles at x approximately 50 showed the highest steady-state current density among the catalysts under study and maintained the best long-term stability. In addition, on the basis of the anodic peak current density, onset potentials, and the ratios of the anodic peak current density to the cathodic peak current density in CV studies, the catalytic activity for HCOOH oxidation was found to decrease in the order of Fe42Pt58>Fe54Pt46 approximately Fe58Pt42>Fe15Pt85>Fe10Pt90>Fe63Pt37. That is, within the present experimental context, the alloy nanoparticles at x approximately 50 appeared to exhibit the maximum electrocatalytic activity and stability with optimal tolerance to CO poisoning. Consistent responses were also observed in electrochemical impedance spectroscopic measurements. For the alloy nanoparticles that showed excellent tolerance to CO poisoning, the impedance in the Nyquist plots was found to change sign from positive to negative with increasing electrode potential, suggesting that the electron-transfer kinetics evolved from resistive to pseudoinductive and then to inductive characters. However, for the nanoparticles that were heavily poisoned by adsorbed CO species during formic acid oxidation, the impedance was found to be confined to the first quadrant at all electrode potentials. The present work highlights the influence of the molecular composition of Pt-based alloy electrocatalysts on the performance of formic acid electro-oxidation, an important aspect in the design of bimetal electrocatalysts in fuel cell applications.
Conversion of carbon dioxide (CO ) into fuels and chemicals by electroreduction has attracted significant interest, although it suffers from a large overpotential and low selectivity. A Pd-Sn alloy electrocatalyst was developed for the exclusive conversion of CO into formic acid in an aqueous solution. This catalyst showed a nearly perfect faradaic efficiency toward formic acid formation at the very low overpotential of -0.26 V, where both CO formation and hydrogen evolution were completely suppressed. Density functional theory (DFT) calculations suggested that the formation of the key reaction intermediate HCOO* as well as the product formic acid was the most favorable over the Pd-Sn alloy catalyst surface with an atomic composition of PdSnO , consistent with experiments.
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