Effect of Ce/Zr Composition on Structure and Properties of Ce1−xZrxO2 Oxides and Related Ni/Ce1−xZrxO2 Catalysts for CO2 Methanation

Abstract

Ce1−xZrxO2 oxides (x = 0.1, 0.25, 0.5) prepared via the Pechini route were investigated using XRD analysis, N2 physisorption, TEM, and TPR in combination with density functional theory calculations. The Ni/Ce1−xZrxO2 catalysts were characterized via XRD analysis, SEM-EDX, TEM-EDX, and CO chemisorption and tested in carbon dioxide methanation. The obtained Ce1−xZrxO2 materials were single-phase solid solutions. The increase in Zr content intensified crystal structure strains and favored the reducibility of the Ce1−xZrxO2 oxides but strongly affected their microstructure. The catalytic activity of the Ni/Ce1−xZrxO2 catalysts was found to depend on the composition of the Ce1−xZrxO2 supports. The detected negative effect of Zr content on the catalytic activity was attributed to the decrease in the dispersion of the Ni0 nanoparticles and the length of metal–support contacts due to the worsening microstructure of Ce1−xZrxO2 oxides. The improvement of the redox properties of the Ce1−xZrxO2 oxide supports through cation modification can be negated by changes in their microstructure and textural characteristics.