An in-situ modified sol-gel process for monolith catalyst preparation used in the partial oxidation of methane

An in-situ modified sol-gel method for the preparation of a Ni-based monolith-supported catalyst is reported. With the presence of a proper amount of plasticizer and binder, and at an optimized pH value, the stable boehmite sol was modified with metal ions (Ni, Li, La) successfully without distinct growth of the particle size. Monolith-supported Ni-based/gamma-Al2O3 catalysts were obtained using the modified sol as the coating medium with several cycles of dip-coating and calcination. Combined BET, SEM-EDS, XRD and H-2-TPR investigations demonstrated that the derived monolith catalysts had a high specific surface area, a relatively homogeneous surface composition, and a high extent of interaction between the active component and the support. These catalysts showed relatively stable catalytic activities for partial oxidation of methane (POM) to syngas under atmospheric pressure. The monolith catalysts prepared by this sol-gel method also demonstrated an improved resistance to sintering and loss of the active component during the reaction process.

Structure and base properties of calcined hydrotalcites

Five hydrotalcites with Mg/Al molar ratio range of 3-15 were prepared. The structure and basicity of Mg-Al mixed oxides (Mg(Al)O) transformed from hydrotalcites were investigated by TPD, XPS, XRD, FT-IR and NMR techniques. The results of elemental analysis and XPS indicate that Al is enriched in the surface regions of Mg(Al)O, and its amount increases with the Mg/Al molar ratio and, the calcination temperature. Al-27-MAS-NMR results show that Al exists in two chemical environments: tetrahedral aluminium (Al(t)) and octahedral aluminium (Al(o)) in Mg(AI)O. The amount of Al(t) increases with the Mg/Al molar ratio and the calcination temperature. It is assumed that Al(t) may be mainly from the surface Al. Temperature-programmed desorption (TPD) of CO2 shows that the number of basic sites of Mg(Al)O samples increases with the Mg/Al molar ratio, and the maximum number of basic sites is obtained for hydrotalcite calcined at 773 K. Infrared spectra of adsorbed CO2 and B(OCH3)(3) reveal that there are two kinds of basic sites: weak basic OH- sites and strong basic O2- sites on the Mg(AI)O samples, the base strength depends on the Mg/Al molar ratio and calcination temperature.