期刊
MICROPOROUS AND MESOPOROUS MATERIALS
卷 210, 期 -, 页码 69-76出版社
ELSEVIER SCIENCE BV
DOI: 10.1016/j.micromeso.2015.02.012
关键词
Sn-BEA; Lewis-acid; FTIR; TGA; Silanol
类别
资金
- Catalysis Center for Energy Innovation, an Energy Frontier Research Center - U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-SC0001004]
The correlation of the similar to 960 cm(-1) IR absorption band, frequently observed in Sn-BEA zeolite, to the incorporation of Sn in the zeolite framework has been investigated. IR and NMR spectra of freshly calcined and water treated zeolites combined with first principle calculations indicate that the 960 cm(-1) band is not a vibration involving Sn but rather a result of isolated internal silanol groups. Thermogravimetric analysis and temperature-programmed desorption showed the silanol groups condense to form water at temperatures between 400 and 700 degrees C. These silanol groups form slowly at mild relative humidity (similar to 30-40%) and 25 degrees C, but in less than an hour at 98 degrees C in liquid water: they are expected to form in the course of an aqueous phase reaction. The water uptake observed following a one-hour liquid water treatment is 1.2 wt% in Sn-BEA with Si/Sn = 125, equal to 4-5 water molecules per Sn or 1 water molecule per 40 Si, too high for all of it to be directly linked to interaction with Sn atoms. Instead this water uptake can be explained by a site that can be hydroxylated at relatively low temperatures and dehydrated at temperatures typically used for zeolite calcination. (c) 2015 Elsevier Inc. All rights reserved.
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