Highly stable ceria-zirconia-yttria supported Ni catalysts for syngas production by CO2 reforming of methane

作者:Munoz M A; Calvino J J; Rodriguez Izquierdo J M; Blanco G; Arias D C; Perez Omil J A; Hernandez Garrido J C; Gonzalez Leal J M; Cauqui M A*; Yeste M P
来源:Applied Surface Science, 2017, 426: 864-873.
DOI:10.1016/j.apsusc.2017.07.210

摘要

Ni/CeO2/YSZ and Ni/Ce0.15Zr0.85O2 have been investigated as catalysts for the dry reforming of methane at 750 degrees C. Ni was incorporated by the impregnation method. The supports were previously activated by using a thermo-chemical protocol consisting on a severe reduction (H-2/Ar) at 950 degrees C follow ed by a mild oxidation (O-2/He) at 500 degrees C. According to TPR results, this protocol leads to the development of unique redox properties in the case of the CeO2/YSZ oxide. Two types of CO2 + CH4 (1 :1 ) mixtures (helium-diluted and undiluted) w ere used to feed the reactor. When using the Ni/Ce0.15Zr0.85O2 catalyst with undiluted feed, the reactor became plugged by coke. By contrast, Ni/CeO2/YSZ behaved as an active and stable catalyst even under the most severe operation conditions. The characterization of the spent Ni/CeO2/YSZ using TGA, TEM, Raman and XPS spectroscopy revealed that only a limited amount of graphitic carbon, in form of nanotubes, was formed. No evidences of deactivating carbonaceous forms were obtained. The singular redox properties of the activated CeO2/YSZ oxides are proposed as a key for designing Ni catalysts highly stable in reforming processes.

  • 出版日期2017-12-31