TY - JOUR
T1 - Cesium salt of a heteropolyacid in nanotubular channels and on the external surface of SBA-15 crystals
T2 - Preparation and performance as acidic catalysts
AU - Rao, P. Madhusudhan
AU - Landau, M. V.
AU - Wolfson, A.
AU - Shapira-Tchelet, A. M.
AU - Herskowitz, M.
N1 - Funding Information:
This paper has been presented at the International Mesostructured Materials Symposium (IMMS 2004) in May 2004 in Cape Town, South Africa. This study was supported by the Israel Science Foundation, Center of Excellence (Grant no. 8003). The authors gratefully acknowledge Mr. V. Ezersky, Mrs. L. Burlaka for HRTEM, HRSEM, and Dr. A.I. Erenburg for conducting WAXS and SAXS characterizations, respectively.
PY - 2005/5/30
Y1 - 2005/5/30
N2 - The Cs-salt of heteropolyacid with stoichiometry Cs2.5H 0.5PW12O40 (CsHPW) was deposited selectively at the external surface of the SBA-15 silica microcrystals, inside its mesoporous channels and simultaneously at both location modes. The structure, texture and performance of these CsHPW/SBA-15 composites were compared with that of a reference bulk salt of the same composition. Location of CsHPW salt on the external surface of SBA-15 microcrystals leads to disintegration of its agglomerates increasing acidity of the catalytic phase. A novel preparation strategy consisting of grafting the basic Cs-species at the internal pores surface of SBA-15 stabilized the CsHPW phase inside the channels in form of 5-8 nm nanocrystals at 30-70 wt.% loadings. The catalytic tests demonstrated that insertion of the CsHPW catalytic phase inside the nanotubular channels of SBA-15 in combination with location of an additional amount of this phase at the external surface of SBA-15 microcrystals allows to increase the specific activity of this phase in MTBE synthesis, propionylation of anisole and alkylation of catechol with t-butanol by a factor of 1.5-3. This level of specific activity in combination with high total loading of catalytic phase >60 wt.% permit to get composite catalytic materials with catalytic activity higher by a factor of 1.2-1.5 with respect to the bulk CsHPW catalyst and stabilizing the catalytic phase against colloidization in polar media.
AB - The Cs-salt of heteropolyacid with stoichiometry Cs2.5H 0.5PW12O40 (CsHPW) was deposited selectively at the external surface of the SBA-15 silica microcrystals, inside its mesoporous channels and simultaneously at both location modes. The structure, texture and performance of these CsHPW/SBA-15 composites were compared with that of a reference bulk salt of the same composition. Location of CsHPW salt on the external surface of SBA-15 microcrystals leads to disintegration of its agglomerates increasing acidity of the catalytic phase. A novel preparation strategy consisting of grafting the basic Cs-species at the internal pores surface of SBA-15 stabilized the CsHPW phase inside the channels in form of 5-8 nm nanocrystals at 30-70 wt.% loadings. The catalytic tests demonstrated that insertion of the CsHPW catalytic phase inside the nanotubular channels of SBA-15 in combination with location of an additional amount of this phase at the external surface of SBA-15 microcrystals allows to increase the specific activity of this phase in MTBE synthesis, propionylation of anisole and alkylation of catechol with t-butanol by a factor of 1.5-3. This level of specific activity in combination with high total loading of catalytic phase >60 wt.% permit to get composite catalytic materials with catalytic activity higher by a factor of 1.2-1.5 with respect to the bulk CsHPW catalyst and stabilizing the catalytic phase against colloidization in polar media.
KW - Acidic catalysis
KW - Cesium salt
KW - Heteropolyacid
KW - Mesostructured silica
UR - http://www.scopus.com/inward/record.url?scp=17544382817&partnerID=8YFLogxK
U2 - 10.1016/j.micromeso.2004.11.021
DO - 10.1016/j.micromeso.2004.11.021
M3 - Article
AN - SCOPUS:17544382817
VL - 80
SP - 43
EP - 55
JO - Microporous and Mesoporous Materials
JF - Microporous and Mesoporous Materials
SN - 1387-1811
IS - 1-3
ER -