期刊
APPLIED CATALYSIS A-GENERAL
卷 482, 期 -, 页码 16-23出版社
ELSEVIER
DOI: 10.1016/j.apcata.2014.05.011
关键词
Silica-doped alumina; Bronsted and Lewis acid sites; Thermal stability; Acid site concentration
资金
- U.S. Department of Energy's National Nuclear Security Administration [DE-AC04-94AL85000]
- DOE [DE-FG02-05ER15666]
- National Science Foundation [CHE-0959862]
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. (C) 2014 Elsevier B.V. All rights reserved.
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