[1]黄凯,乔宏琴.SO2-4/ZrO2型固体超强酸催化剂的改性[J].东南大学学报(自然科学版),2010,40(5):1003-1008.[doi:10.3969/j.issn.1001-0505.2010.05.023]
 Huang Kai,Qiao Hongqin.Modification of SO2-4/ZrO2 solid superacid catalysts[J].Journal of Southeast University (Natural Science Edition),2010,40(5):1003-1008.[doi:10.3969/j.issn.1001-0505.2010.05.023]
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SO2-4/ZrO2型固体超强酸催化剂的改性()
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《东南大学学报(自然科学版)》[ISSN:1001-0505/CN:32-1178/N]

卷:
40
期数:
2010年第5期
页码:
1003-1008
栏目:
化学化工
出版日期:
2010-09-20

文章信息/Info

Title:
Modification of SO2-4/ZrO2 solid superacid catalysts
作者:
黄凯 乔宏琴
东南大学化学化工学院,南京 211189
Author(s):
Huang Kai Qiao Hongqin
School of Chemistry and Chemical Engineering, Southeast University, Nanjing 211189, China
关键词:
催化剂 SO2-4/ZrO2固体超强酸 α-Al2O3 表征
Keywords:
catalyst SO2-4/ZrO2 solid superacid α-Al2O3 characterization
分类号:
O643.3;TQ032.4
DOI:
10.3969/j.issn.1001-0505.2010.05.023
摘要:
针对传统SO2-4/ZrO2固体超强酸存在稳定性较差等缺点,通过添加α-Al2O3和偏钨酸铵对其进行改性,制备出复合氧化物固体超强酸SO2-4/ZrO2-WO3-Al2O3(SWZA).为了获得催化性能高的SZWA催化剂,采用流动指示剂法测定改性催化剂的酸度,同时利用XRD,FTIR,TGA-DSC,SEM等多种现代物理方法对SWZA催化剂进行表征,研究了陈化温度、焙烧温度等制备条件以及Al2O3,WO3等不同金属氧化物的引入对产物催化性能的影响.实验结果表明:较低的陈化温度使催化剂表面易形成结晶中心,降低了质点的迁移速率,抑制了晶粒生长,易于生成小且规则的晶粒,使得到的催化剂具有较大的比表面积; 在制备催化剂时, 500 ℃的焙烧温度有利于ZrO2向四方晶型转化,增大了超强酸的比表面积; Al2O3的引入增加了超强酸的Lewis酸位,提高了催化剂的催化活性; WO3的引入对催化剂晶型具有定向诱导作用,延迟了ZrO2晶化,稳定了亚稳态的四方晶型,缓和了SO2-4高温下分解流失的趋势.
Abstract:
To improve the stability of traditional SO2-4/ZrO2 solid superacid catalysts, a kind of solid superacid catalyst SO2-4/ZrO2-WO3-Al2O3(SWZA)modified with α-Al2O3 and ammonium tungstate is prepared. To obtain the high catalytic performance of the catalysts, the flow indictor method is used to measure the acidity of the catalysts. The X-ray diffraction(XRD), the Fourier transform infrared ray spectroscopy(FTIR), the thermal gravimetric analysis-differential scanning calorimetry(TGA-DSC)and the scanning electron microscope(SEM)are used for studying the catalytic mechanism. The effects of the preparation conditions, such as the precipitation temperature, the calcination temperature and the addition of α-Al2O3 and ammonium tungstate, on the catalytic performance of the catalysts are studied. The experimental results show that a low precipitation temperature can help form crystal centers on the surfaces of the catalysts, reduce the rate of particle migration, inhibit the grain growth and produce small but regular crystal particles, resulting in an increase of specific surface area of the obtained catalysts. During the preparation, the suitable calcination temperature 500 ℃ induces the crystal transformation from the monoclinic phase to the tetragonal phase and the specific surface area of the superacid is increased. The addition of α-Al2O3 can increase the Lewis acid sites on the catalyst surfaces, improving the catalytic activity of the catalysts. The addition of WO3 can orientally induce the crystal formation of the catalysts, delay the crystallization of ZrO2, stabilize the tetragonal phase and constrain the loss of SO2-4 at the high temperature.

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备注/Memo

备注/Memo:
作者简介: 黄凯(1973—),男,博士,副教授,huangk@seu.edu.cn.
基金项目: 东南大学自然科学基金预研项目(9207041400)、浙江工业大学绿色化学合成技术国家重点实验室开放基金资助项目(GCTKF 2010013).
引文格式: 黄凯,乔宏琴.SO2-4/ZrO2型固体超强酸催化剂的改性[J].东南大学学报:自然科学版,2010,40(5):1003-1008. [doi:10.3969/j.issn.1001-0505.2010.05.023]
更新日期/Last Update: 2010-09-20