RESUMO
A series of Ni-La/Al2O3 catalysts for the syngas methanation reaction were prepared by a mechanochemical method and characterized by thermogravimetric analysis (TG-DTA), X-ray fluorescence (XRF), X-ray diffraction (XRD), N2 adsorption-desorption, H2 temperature-programmed reduction (H2-TPR), and X-ray photoelectron spectroscopy (XPS). The calcination temperatures (350-700 °C) had significant impacts on the crystallite sizes and interactions between NiO and Al2O3. The catalyst calcined at 400 °C (cat-400) showed a 12.1% Ni dispersion degree and the maximum bound state of NiO (54%) through the Gaussian fitting of H2-TPR. Cat-400 also achieved the highest CO conversion, CH4 selectivity and yield. Cat-400 exhibited good stability and catalytic activity in a lifetime testing of 200 h. The deactivation of cat-400 was mainly caused by carbon deposition according to the data from XRD, TG-DTG and XPS.
RESUMO
In this study, the pyrolysis behavior and kinetics of raw biomasses and their pellets were studied by Coats Redfern and DAEM methods. The results demonstrated that the similar activation energies obtained by both methods confirmed accuracy of the kinetics calculation. The activation energy of the pellets was 132.49-232.44â¯kJâ¯mol-1, slightly higher than those of raw biomasses, which was 120.58-210.55â¯kJâ¯mol-1. The results from Coats Redfern method showed that the pyrolysis of all the samples were controlled by mass and heat diffusion. DAEM revealed that the activation energies of the pellets were higher than those of raw biomasses during hemicellulose and cellulose decomposition stages, and was opposite for the lignin decomposition stage. Physical structure characterization indicated that the pellets had smaller surface area and more compact surface than those of their raw biomasses. Hence, the mass and heat diffusion were suppressed and more cross-linking reactions occurred during pellets pyrolysis.