物理化学学报 >> 2010, Vol. 26 >> Issue (08): 2229-2234.doi: 10.3866/PKU.WHXB20100640

催化和表面结构 上一篇    下一篇

Al含量对Pt-SO2-4 /ZrO2-Al2O3固体超强酸催化

宋华1,2, 董鹏飞1, 张 旭1   

  1. 1. 大庆石油学院, 化学化工学院, 黑龙江 大庆 163318;
    2. 大庆石油学院, 石油与天然气化工省重点实验室, 黑龙江 大庆1 63318
  • 收稿日期:2009-12-23 修回日期:2010-03-09 发布日期:2010-07-23
  • 通讯作者: 宋华 E-mail:songhua@dqpi.edu.cn
  • 基金资助:

    中国石油天然气股份有限公司科技风险创新基金(07-06D-01-04-03-02)资助项目

Effect of Al Content on the n-Pentane Isomerization of the Solid Superacid Pt-SO2-4 /ZrO2-Al2O3

SONG Hua1,2, DONG Peng-Fei1, ZHANG Xu1   

  1. 1. College of Chemistry and Chemical Engineering, Daqing Petroleum Institute, Daqing 163318, Heilongjing Province, P. R. China;
    2. Heilongjiang Provincial Key Laboratory of Chemical Engineering of Oil and Gas, Daqing Petroleum Institute, Daqing 163318, Heilongjiang Province, P. R. China
  • Received:2009-12-23 Revised:2010-03-09 Published:2010-07-23
  • Contact: SONG Hua E-mail:songhua@dqpi.edu.cn
  • Supported by:

    The project was supported by the Science and Technological Innovation Foundation of PetroChina Company Limited (07-06D-01-04-03-02).

摘要:

通过向SO2-4 /ZrO2催化剂中同时引入适量的Pt和Al2O3, 制备出了具有较高催化性能和稳定性的Pt-SO2-4 /ZrO2-Al2O3型固体超强酸催化剂. 以正戊烷异构化反应为探针, 考察了Al含量对催化剂性能的影响; 并采用X射线衍射(XRD)、比表面积测定(BET)、红外(IR)光谱、程序升温还原(TPR)、热重-差热分析(TG-DTA)和氨-程序升温脱附(NH3-TPD)手段对催化剂进行了表征. 结果表明, Al能够提高ZrO2的晶化温度, 抑制硫的分解, 增加催化剂的比表面积, 增强硫氧键的结合, 提高催化剂的还原性能, 增加催化剂的酸强度和酸总量. 当Al2O3含量(质量分数, w)为5.0%时, Pt-SO2-4 /ZrO2-Al2O3固体超强酸催化剂的催化活性最好, 在100 h内异戊烷收率可稳定在52.0%以上, 选择性在98.2%以上.

关键词: 固体超强酸, 催化剂, SO2-4 /ZrO2, 异构化, Al2O3含量, Pt

Abstract:

Highly active and stable Pt-SO2-4 /ZrO2-Al2O3 solid superacid catalysts were prepared by simultaneously introducing appropriate amounts of Pt and Al2O3 into a SO2-4 /ZrO2 catalyst. The effect of Al content on the performance of the catalysts was studied using n-pentane isomerization as a probe reaction and the catalysts were characterized by X-ray diffraction (XRD), specific surface area measurements (BET), infrared (IR) spectroscopy, temperature-programmed reduction (TPR), thermogravimetry-differential thermal analysis (TG-DTA), and NH3 temperature-programmed desorption (NH3-TPD). The results show that Al can increase the crystallization temperature of ZrO2 and inhibit the decomposition of sulfur. Al can also increase the surface area of the catalyst, strengthen the combination between S and O, improve the redox performance of the catalyst and increase the acid strength and the acidity of the catalyst. The catalytic activity of the Pt-SO2-4 /ZrO2-Al2O3 solid superacid catalyst with a Al2O3 mass fraction of 5.0% was found to be the best. The isopentane yield was stable above 52.0% and the selectivity was higher than 98.2% within 100 h.

Key words: Solid superacid, Catalyst, SO2-4 /ZrO2, Isomerization, Al2O3 content, Pt

MSC2000: 

  • O643