高等学校化学学报

高等学校化学学报 ›› 2003, Vol. 24 ›› Issue (1): 130.

• 论文 • 上一篇    下一篇

S2O82-和SO42-促进ZrO2固体超强酸正戊烷反应性能差异的研究

宋国新, 王琳, 薛华欣, 张黎, 陈建民   

  1. 复旦大学环境科学与工程系, 上海 200433
  • 收稿日期:2002-03-20 出版日期:2003-01-24 发布日期:2003-01-24
  • 通讯作者: 陈建民(1964年出生),男,博士,教授,博士生导师,主要从事环境催化和环境化学研究.E-mail:jmchen@fudan.ac.cn E-mail:jmchen@fudan.ac.cn
  • 基金资助:

    国家教育部留学归国人员基金资助

A Study on n-Pentane Reactions over Peroxodisulfated Zirconia and Sulfated Zirconia Solid Superacid

SONG Guo-Xin, WANG Lin, XUE Hua-Xin, ZHANG Li, CHEN Jian-Min   

  1. Department of Environmental Science & Engineering, Fudan University, Shanghai 200433, China
  • Received:2002-03-20 Online:2003-01-24 Published:2003-01-24

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摘要： 考察了常温下S2O2-8促进ZrO2(PSZ)固体超强酸催化剂上正戊烷的反应性能,并与SO2-4促进ZrO2(SZ)反应相比较,观察到PSZ和SZ对正戊烷都具有异构化和裂解的双重作用,主要产物分别为异戊烷和异丁烷.正戊烷的异构化转化率和表观反应速率常数主要取决于样品的焙烧温度.但对于正戊烷异构化反应,PSZ的最佳焙烧温度为550℃,比SZ的低50℃.在各自的最佳焙烧温度下反应1h后,前者的异戊烷生成率为后者的1.3倍.通过S含量和比表面积测定以及用XRD和FTIR等手段分析了PSZ的物理化学特性.从原位FTIR谱图发现,PSZ(550℃)表面S-O键的红外吸收明显比SZ(600℃)的强;通过吡啶红外手段发现PSZ(550℃)吡啶离子吸收峰的红移大于SZ(600℃),表明前者的Lewis酸强于后者.

关键词: 固体超强酸, S2O2-8促进ZrO2, SO2-4促进ZrO2, 正戊烷, 异构化, 裂解

Abstract: n-Pentane reaction over S22-82(PSZ) at an ambient temperature in the steady state system has been introduced in relation with the same reaction occurring over SO2-4/ZrO2(SZ). It can be concluded that both PSZ and SZ have two functions on n-pentane: isomerization and cracking. The products of the two reactions are i-pentane and i-butane respectively. The conversion of n-pentane isomerization and apparent reactive velocity constant lie mainly on the calcining temperature of each sample. The catalysis activity of PSZ is higher than that of SZ: the molar ratio of i-pentane over the former to that over the latter is 1.3/1 after 1 h reaction. The optimum calcining temperature of PSZ is 550 ℃, which is 50 ℃ lower than that of SZ. By means of S-content measurement, BET, XRD, FTIR and chemical analysis, the physical and chemical characteristics of S22-82 can be attained. We draw a conclusion that PSZ has stronger Lewis acidic sites and more acid quantity than SZ from the results of the in situ FTIR and Pyridine-FTIR experiment.

Key words: Solid superacid, S22-82, SO2-4/ ZrO2, n-Pentane, Isomerization, Cracking

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