Chinese Journal of Catalysis ›› 2017, Vol. 38 ›› Issue (3): 475-488.DOI: 10.1016/S1872-2067(17)62749-9

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Pt-CeO2/SiO2 catalyst for CO oxidation in humid air at ambient temperature

Shirish S. Punde, Bruce J. Tatarchuk   

  1. Department of Chemical Engineering, Auburn University, Auburn, AL, USA
  • Received:2016-08-05 Revised:2016-08-29 Online:2017-03-18 Published:2017-03-22
  • Supported by:

    This work was supported by US Army contract (W56HZV-05-C0686) at Auburn University administered through TARDEC.

Abstract:

CO self-poisoning and slow surface kinetics pose major challenges to a CO oxidation catalyst that should work at ambient temperature. Furthermore, the presence of moisture would cause passivation of the catalyst. A highly active ceria promoted Pt catalyst (4%Pt-12%CeO2/SiO2; conversion ≥ 99% at low (< 500 ppm) and high (> 2500 ppm) CO concentrations was developed for CO oxidation at ambient temperature in humid air. Catalyst preparation variables such as Pt and CeO2 loading, ceria deposition method, drying and calcination conditions for the ceria and Pt precursors were optimized experimentally. The activity was correlated with surface properties using CO/H2 chemisorption, O2-H2 titration, X-ray diffraction and BET surface area analysis. The method of CeO2 deposition had a significant impact on the catalytic activity. CeO2 deposition by impregnation resulted in a catalyst that was three times more active than that prepared by deposition precipitation or CeO2 grafting. O2-H2 titration results revealed that the close association of ceria and Pt in the case of CeO2 deposition by impregnation resulted in higher activity. The catalyst support used was also crucial as a silica supported catalyst was five times more active than an alumina supported catalyst. The particle size and pore structure of the catalyst support were also crucial as the reaction was diffusion controlled. The drying and calcination conditions of the ceria and Pt precursors also played a crucial role in determining the catalytic activity. The Pt-CeO2/SiO2 catalysts with Pt > 2.5 wt% and CeO2 > 15 wt% were highly active (TOF > 0.02 s-1) and stable (conversion ≥ 99% after 15 h) at ambient conditions.

Key words: Carbon monoxide oxidation, Catalyst, Platium, Ceria, Silica, Precursor, O2-H2 titration, Chemisorption, Temperature-programmed reduction