Abstract
We prepared monodisperse Pt2Ru3 nanoparticles supported on carbon black and Sb-doped SnO2 (denoted as Pt2Ru3/CB and Pt2Ru3/Sb-SnO2) with identical alloy composition and particle size distribution by the nanocapsule method. The activities for the hydrogen oxidation reaction (HOR) of these anode catalysts were examined in H2-saturated 0.1 M HClO4 solution in both the presence and absence of carbon monoxide by use of a channel flow electrode at 70 °C. It was found that the CO-tolerant HOR mass activity at 0.02 V versus a reversible hydrogen electrode (RHE) on the Pt2Ru3/Sb-SnO2 electrode was higher than that at the Pt2Ru3/CB electrode in 0.1 M HClO4 solution saturated with 1000 ppm CO (H2-balance). The CO tolerance mechanism of these catalysts was investigated by in situ attenuated total reflection Fourier transform infrared reflection-adsorption spectroscopy (ATR-FTIRAS) in 1% CO/H2-saturated 0.1 M HClO4 solution at 60 °C. It was found, for the Pt2Ru3/Sb-SnO2 catalyst, that the band intensity of CO linearly adsorbed (COL) at step/edge sites was suppressed, together with a blueshift of the COL peak at terrace sites. On this surface, the HOR active sites were concluded to be more available than those on the CB-supported catalyst surface. The observed changes in the adsorption states of CO can be ascribed to an electronic modification effect by the Sb-SnO2 support.
Highlights
Polymer electrolyte fuel cells (PEFCs) have been intensively developed for the applications of residential cogeneration systems and fuel cell vehicles
The diffraction peaks assigned to the Pt-Ru alloy for Pt2 Ru3 /CB were clearly shifted to higher angles than those of pure Pt with the face-centered cubic structure
The peak of 2θ = 39.8◦ observed for Pt/CB was assigned to Pt(111), whereas the corresponding peak for the Pt2 Ru3 /CB catalyst was observed at 40.5◦
Summary
Polymer electrolyte fuel cells (PEFCs) have been intensively developed for the applications of residential cogeneration systems and fuel cell vehicles. The CO concentration in the reformate must be reduced further, down to ≤10 ppm, by the preferential oxidation (PROX) of CO This is because the CO-tolerance of the state-of-the-art commercial anode catalyst, Pt2 Ru3 nanoparticles supported on high-surface-area carbon black (c-Pt2 Ru3 /CB), is insufficient. We focus on the effect of Sb-doped SnO2 (electronic conductive oxide support) on the CO-tolerant HOR activity of Pt2 Ru3. For this purpose, we have prepared Pt2 Ru3 nanoparticles supported on both Sb-SnO2 and conventional carbon black with the identical alloy composition, as well as the identical size distribution.
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