Влияние кислотности на свойства алюмосиликатов, синтезированных золь-гель методом

Abstract

In the present work amorphous silica-aluminas were synthesized by the coprecipitation method during the hydrolysis of an alcohol solution of tetraethoxysilane (with a tetraethoxysilane: alcohol mass ratio of 1: 1) and 6% aqueous solution of aluminum nitrate at pH values of 1, 3, and 10. The Si/Al molar ratio for all synthesized samples were 4.72 (± 0.29). The amorphous character of the investigated materials was confirmed by X-ray phase analysis. According to the results of scanning electron microscopy, it was found that the resulting powders have particles with a size of 1-20 μm. It was shown that the conditions of synthesis affected the specific surface area and porosity of the materials under study. By the method of low-temperature adsorption-thermodesorption of nitrogen it was established that silica-aluminas obtained under acidic conditions were microporous materials. For the sample obtained under alkaline conditions (pH = 10), the contribution of macropores is very significant. A decrease in surface area is observed as the pH of the synthesis increases. The Hammett indicator method was used to identify and quantify surface centers of different acidity. All studied silica-aluminas are characterized by the presence of both Brønsted basic (pKax from 7 to 12.8) and acidic (pKax from 0 to 7) centers, and Lewis basic (pKax from -4.4 to 0) with a pronounced maximum at pKax = 1.02. It was found that the synthesis conditions had a significant effect on the concentration of active centers. The values of the Hammett function are practically the same for the 3 studied silica-aluminas and describe the studied samples as materials of medium acidity. The variety of Lewis and Brønsted centers on the surface indicates the amphoteric properties of the materials under study. This gives the samples the properties of polyfunctional sorbents and catalysts.