高等学校化学学报

高等学校化学学报 ›› 2000, Vol. 21 ›› Issue (1): 116.

• 论文 • 上一篇    下一篇

S2O82-/ZrO2固体超强酸的研究

张黎, 王琳, 陈建民   

  1. 复旦大学环境科学与工程系, 上海 200433
  • 收稿日期:1999-03-04 出版日期:2000-01-24 发布日期:2000-01-24
  • 通讯作者: 陈建民(1965年出生),男,副博士,副教授,从事固体酸催化剂研究.E2mail:jmchen@fudan.ac.cn E-mail:jmchen@fudan.ac.cn
  • 基金资助:

    国家教育部归国留学人员基金

Studies of Peroxodisulfated Zirconia Solid Superacid

ZHANG Li, WANG Lin, CHEN Jian-Min   

  1. Department of Environmental Science & Engineering, Fudan University, Shanghai 200433, China
  • Received:1999-03-04 Online:2000-01-24 Published:2000-01-24

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摘要： 以S2O82-浸渍无定形Zr(OH)4,制得较SO42-/ZrO2酸性更强的固体超强酸.用正丁烷异构化反应考察了S2O82-/ZrO2的酸性.结果表明,在对ZrO2有促进作用的非卤素阴离子中,S2O82-是最好的促进剂.最佳焙烧条件下S2O82-/ZrO2固体超强酸比SO42-/ZrO2的酸性更强.35℃下,S2O82-/ZrO2上正丁烷异构化反应速率较SO42-/ZrO2提高了1.2倍.反应20h后的正丁烷转化率提高了约1.5倍.用XRD、TEM和化学分析等手段分析了S2O82-/ZrO2体系的晶化过程、比表面和含硫量.结果表明,与SO42-/ZrO2体系形成的固体超强酸的过程类似,晶化温度、比表面和含硫量均明显影响S2O82-/ZrO2的酸性强弱.S2O82-/ZrO2的最佳焙烧温度比SO42-/ZrO2低50℃,在500～800℃焙烧的S2O82-/ZrO2可形成纳米级固体超强酸.

关键词: S2O82-/ZrO2, 固体超强酸, 正丁烷异构化

Abstract: The preparation of peroxodisulfated zirconia(PSZ) solid strong acid catalysts is introduced. It showed more active than sulfated zirconia (SZ) for n-butane isomerization at ambient temperature. Peroxodisulfate is the first type of nonhalide found to be more efficient than sulfate which so far has been found the best one promoted zirconia. The optimum calcination temperature is 600 ℃, which is 50 ℃ lower than that of SZ. The conversion of n-butane over PSZ was 50.4% during 20 h and at 35 ℃, and 36.7% over SZ under the same condition. According to X-Ray differential, TEM, BET and chemical analysis, it can be concluded that the formation of superacids over PSZ is similar to that over SZ. It is worth to point out the particle sizes of PSZ calcined between 500 ℃ and 800 ℃ are in the range of nanometers, and the optimum PSZ has both tetragonal and limited monoclinic zirconia.

Key words: S2O82-/ZrO2, Solid superacid, n-Butane isomerization

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