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负载杂多酸(盐)的表征及其在苹果酯合成反应中的催化性能
引用本文:张富民,袁超树,任晓乾,王军.负载杂多酸(盐)的表征及其在苹果酯合成反应中的催化性能[J].化工学报,2006,57(4):762-768.
作者姓名:张富民  袁超树  任晓乾  王军
作者单位:南京工业大学化学化工学院,省部共建材料化学工程教育部重点实验室,江苏 南京 210009
基金项目:中国科学院资助项目 , 高等学校博士学科点专项科研项目
摘    要:用浸渍法制备了一系列负载型磷钨酸及其铯盐催化剂,载体包括超稳Y沸石(USY)、脱铝超稳Y沸石(DUSY)、SiO2和SBA-15,测定了催化剂的比表面积和酸强度,并在乙酰乙酸乙酯与乙二醇液相缩合制取苹果酯反应中考察了催化剂的性能.结果表明,这些负载型杂多化合物催化剂都表现出较高的催化活性.然而,催化剂在水中的溶脱性能实验表明,负载型磷钨酸催化剂存在严重的活性组分流失现象,不能重复使用,而DUSY负载的磷钨酸铯盐催化剂不仅表现出较高的催化活性,而且显示出较好的重复使用性能.在优化的反应条件下30% (质量分数) Cs2.5H0.5PW/DUSY催化剂上乙酰乙酸乙酯的转化率可达98.7%,苹果酯的选择性大于97%.

关 键 词:杂多酸  磷钨酸  磷钨酸铯盐  乙酰乙酸乙酯  缩合反应
文章编号:0438-1157(2006)04-0762-07
收稿时间:07 20 2005 12:00AM
修稿时间:2005-07-202005-11-04

Characterization of supported heteropoly acid (salt) and its catalytic behavior in synthesis of fructone
ZHANG Fumin,YUAN Chaoshu,REN Xiaoqian,WANG Jun.Characterization of supported heteropoly acid (salt) and its catalytic behavior in synthesis of fructone[J].Journal of Chemical Industry and Engineering(China),2006,57(4):762-768.
Authors:ZHANG Fumin  YUAN Chaoshu  REN Xiaoqian  WANG Jun
Affiliation:Key Laboratory of Materials-Oriented Chemical Engineering of Ministry of Education, School of Chemistry and Chemical Engineering, Nanjing University of Technology, Nanjing 210009, Jiangsu, China
Abstract:A series of 12-phosphotungstic acid(PW)and its cesium salt catalysts immobilized on various supports such as ultra-stable Y zeolite (USY), dealuminated USY (DUSY), SiO_2 and SBA-15 were prepared. Their specific surface area and acid strength were measured, and their catalytic performance was evaluated in the synthesis of fructone by acetalization of ethyl acetoacetate with ethylene glycol. The high catalytic activity was found over the prepared supported heteropoly compound catalysts in this reaction. 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 30%Cs_ 2.5H_ 0.5PW/DUSY under the optimal reaction conditions.
Keywords:heteropoly acid  12-phosphotungstic acid  Cs-salts of 12-phosphotungstic acid  ethyl acetoacetate  acetalization
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