Acid site properties of thermally stable, silica-doped alumina as a function of silica/alumina ratio and calcination temperature

作者:Mardkhe Maryam Khosravi; Keyvanloo Kamyar; Bartholomew Calvin H; Hecker William C; Alam Todd M; Woodfield Brian F*
来源:Applied Catalysis A: General , 2014, 482: 16-23.
DOI:10.1016/j.apcata.2014.05.011

摘要

Acid site properties of silica-doped aluminas prepared by a simple solvent deficient hydrolysis of the alkoxides was investigated. The total acid concentration (Bronsted and Lewis sites) of silica-doped aluminas (SDAs) calcined in the range of 700-1200 degrees C with Si/AI ratios of 5, 15, 27 wt% was determined using temperature-programmed desorption of ammonia (ammonia-TPD). Al-27 solid state MAS NMR (Al SS MAS NMR) was used to measure the intrinsic Lewis acid site concentration, and FTIR was also used as a separate measure of the Bronsted and Lewis acid site concentration. Results indicate that removing hydroxyl groups in the form of water molecules through calcination result in a lower concentration of Bronsted acid sites. Calcination at higher temperature also results in the transformation of unsaturated 5-coordinated aluminum (a strong Lewis acid) to higher concentrations of 6 and 4-coordinated aluminum in 5, 15 and 27% silica-doped alumina samples. Therefore, the total acid site concentration (Bronsted and Lewis sites) decreases by increasing the calcination temperature. In addition, the data show that increasing the silica/alumina ratio increases both the Bronsted and Lewis acid site concentrations. Based on these results, the acid site concentrations can be controlled by altering the Si/Al ratio and calcination temperature while maintaining high surface areas, large pore volumes, and large pore diameters.

  • 出版日期2014-7-22