TY - JOUR
T1 - Synthesis of fructone over dealmuinated USY supported heteropoly acid and its salt catalysts
AU - Zhang, Fumin
AU - Yuan, Chaoshu
AU - Wang, Jun
AU - Kong, Yan
AU - Zhu, Haiyang
AU - Wang, Chunyan
PY - 2006/3/16
Y1 - 2006/3/16
N2 - 12-Phosphotungstic acid (PW) and cesium salt of PW supported on dealuminated ultra-stable Y zeolite (DUSY) with various loadings were prepared by impregnation method, and their physicochemical properties were characterized by X-ray powder diffraction (XRD), N2 adsorption, solid state 31P and 29Si MAS NMR, Hammett indicator and SEM techniques. Their catalytic performances were evaluated in the liquid-phase acetalization of ethyl acetoacetate with ethylene glycol to fructone. The catalytic stability was tested using water treatment, in which the concentration of heteropoly compound was measured by ultraviolet-visual spectrophotometer. A high catalytic activity was found over the supported heteropoly compound catalysts. However, for the supported PW catalysts, a severe leaching of heteropoly anions into water was observed, leading to their poor reusability. By contrast, the Cs salt of PW catalyst supported on DUSY exhibited very high catalytic activity with high water-tolerance and reusability. The conversion of ethyl acetoacetate of 98.7% with the selectivity of fructone above 97% could be obtained over the DUSY supported sample containing 30% of Cs2.5H 0.5PW12O40 by weight at the optimal reaction conditions, and a considerable catalytic activity still could be achieved after five times of reaction cycle.
AB - 12-Phosphotungstic acid (PW) and cesium salt of PW supported on dealuminated ultra-stable Y zeolite (DUSY) with various loadings were prepared by impregnation method, and their physicochemical properties were characterized by X-ray powder diffraction (XRD), N2 adsorption, solid state 31P and 29Si MAS NMR, Hammett indicator and SEM techniques. Their catalytic performances were evaluated in the liquid-phase acetalization of ethyl acetoacetate with ethylene glycol to fructone. The catalytic stability was tested using water treatment, in which the concentration of heteropoly compound was measured by ultraviolet-visual spectrophotometer. A high catalytic activity was found over the supported heteropoly compound catalysts. However, for the supported PW catalysts, a severe leaching of heteropoly anions into water was observed, leading to their poor reusability. By contrast, the Cs salt of PW catalyst supported on DUSY exhibited very high catalytic activity with high water-tolerance and reusability. The conversion of ethyl acetoacetate of 98.7% with the selectivity of fructone above 97% could be obtained over the DUSY supported sample containing 30% of Cs2.5H 0.5PW12O40 by weight at the optimal reaction conditions, and a considerable catalytic activity still could be achieved after five times of reaction cycle.
KW - 12-Phosphotungstic acid
KW - Acetalization
KW - Cs salt of PW
KW - Ethyl acetoacetate
KW - Fructone
KW - Heteropoly acid
UR - http://www.scopus.com/inward/record.url?scp=33644594358&partnerID=8YFLogxK
U2 - 10.1016/j.molcata.2005.11.036
DO - 10.1016/j.molcata.2005.11.036
M3 - 文章
AN - SCOPUS:33644594358
SN - 1381-1169
VL - 247
SP - 130
EP - 137
JO - Journal of Molecular Catalysis A: Chemical
JF - Journal of Molecular Catalysis A: Chemical
IS - 1-2
ER -