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In Situ ATR-FTIR Analysis Of The CO-tolerance Mechanism On Pt2Ru3/C Catalysts Prepared By The Nanocapsule Method
Published 2011 · Chemistry
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The CO-tolerance mechanism of monodisperse Pt2Ru3 (d = 3.6 nm) nanoparticles supported on high surface area carbon black prepared by the nanocapsule method (n-Pt2Ru3/C) was investigated by in situ attenuated total reflection Fourier-transform infrared (ATR-FTIR) spectroscopy in 1% CO (H2-balance)-saturated 0.1 M HClO4 at 25 and 60 °C. For the n-Pt2Ru3/C catalyst, the band intensity ratio of bridged CO to linear CO, I[COB]/I[COL] was smaller and the band intensity of CO on the Ru site I[CO-Ru] was larger than those of a commercial catalyst, c-Pt2Ru3/C, at nearly identical CO coverage θCO. This suggests that the Pt and Ru atoms were exposed on the n-Pt2Ru3 surface more uniformly (well-alloyed) than those of c-Pt2Ru3. The initial CO adsorption rate on n-Pt2Ru3/C was lower than that on c-Pt2Ru3/C. At high θCO, the hydrogen oxidation reaction (HOR) current on n-Pt2Ru3/C decreased significantly with increasing I[CO-Ru], while the c-Pt2Ru3/C exhibited a higher HOR current with a lower I[CO-Ru]. It was found that the CO-tolerance on n-Pt2Ru3/C was greatly improved by treatment in H2 at 200 °C and was superior to c-Pt2Ru3/C at an apparent θCO of 0.95. Because the hydrogen adsorption sites were found to be increased and I[CO-Ru] was suppressed markedly, the formation of a Pt-rich surface with an underlying Pt–Ru alloy was found to be essential to maintain the electronic modification effect of Ru, which helps to preserve HOR active sites by weakening the bond strength of Pt-CO.