(513eu) Impact of Structural Changes from Metal Deposition Method on the Catalytic Performance of Pt/Ceria Zirconia-Based Catalysts | AIChE

(513eu) Impact of Structural Changes from Metal Deposition Method on the Catalytic Performance of Pt/Ceria Zirconia-Based Catalysts

Authors 

Sokefun, Y. O. - Presenter, University of South Florida
Su Khin Zaw, K., University of South Florida
Yung, M. M., National Renewable Energy Laboratory
Joseph, B., University of South Florida
Kuhn, J., University of South Florida
The catalyst synthesis method could impact its performance due to differences in metal particle size, metal dispersion, and metal-support interaction that may arise. Our current work is on the influence of the metal impregnation strategy method on catalyst performance. A set of reforming catalysts containing Pt (0.16 wt%),Ni (2.7wt%) and/or Mg (0.50wt%) supported on ceria-zirconia (CZO) was synthesized. The metal composition was selected based on a previous study on impact of metal loadings on catalyst performance. The metals were co-impregnated unto the support or impregnated sequentially to form Pt-Ni-CZO and Pt-Mg-CZO samples. Powder X-ray diffraction presented peaks for cubic-fluorite structure of ceria and this was corroborated by the Raman spectra, which presented a band for the F2g vibration of the fluorite lattice of ceria. The temperature-programmed reduction results indicated a difference in reduction temperature of the metal oxides arising from different degrees of metal-support interaction. For the Pt-Ni samples, the degree of reducibility followed the trend 0.16Pt-2.7Ni-CZO-seq<2.7Ni-0.16Pt-CZO-seq<0.16Pt-2.7Ni-CZO-co and those of the Pt-Mg sample was 0.16Pt-0.50Mg-CZO-seq<0.16Pt-0.50Mg-CZO-co<0.50Mg-0.16Pt-CZO-seq.The impregnation effect on the nature of CO2 dissociation on the catalyst surface was investigated using FTIR studies. The FTIR spectra presented bands of different intensities belonging to carbonates and formates. CH4 decomposition experiments showed differences in the amounts of products formed. Temperature-programmed oxidation also showed differences in the amounts of CO2 produced and their formation temperatures. Steady-state dry reforming tests indicated differences in catalyst activities with the CH4 conversion rate at 470 ℃ being between 10.2-10.9 µmol/gcat/s for the Pt-Ni samples and between 0.9 - 1.6 µmol/gcat/s for the Pt-Mg samples. The CH4 apparent activation energies of the Pt-Mg were ranged between 30.7-38.4 kcal/mol, and that of the Pt-Ni samples ranged from 29.1-37.7 kcal/mol. This work provides information on how the metal-metal interactions and metal deposition method could impact the catalyst performance.