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活化条件对正己烷在Pt/SO42-/ZrO2-Al2O3上的异构化活性影响

田 静,宋月芹,冯敏超,金亚清,周晓龙   

  1. 华东理工大学化工学院石油加工研究所,上海 200237
  • 出版日期:2012-12-05 发布日期:2012-12-05

Effect of activation condition on n-hexane isomerization performance of Pt/SO42?/ZrO2-Al2O3 catalyst

TIAN Jing, SONG Yueqin, FENG Minchao, JIN Yaqing, ZHOU Xiaolong   

  1. Petroleum Processing Research Center, East China University of Science and Technology, Shanghai 200237, China
  • Online:2012-12-05 Published:2012-12-05

摘要: 采用浸渍法制备了Pt改性的Pt/SO42?/ZrO2-Al2O3(PSZA)催化剂,考察了活化条件对PSZA催化剂正己烷异构化活性的影响,采用程序升温氧化(TPO-MS)、氮气-程序升温处理(TPN-MS)、程序升温还原(TPR-MS)对催化剂进行表征。异构化反应在连续流动的固定床微型反应器中进行。结果表明,200 ℃以上的高温氮气中活化预处理后的PSZA几乎没有异构化活性;空气气氛中、200~500 ℃高温条件下活化预处理的PSZA表现出了较高的异构化活性,正己烷初始转化率均在85%以上。在高于300 ℃的氢气中活化预处理,PSZA表现出较低的异构化活性。空气气氛中预处理除脱水之外,由于氧气的存在对催化剂的表面起到再氧化作用,导致高的异构化活性。氢气气氛中高温活化预处理导致了PSZA上硫物种的损失,进而引起异构化活性的下降。PSZA适宜的预处理条件为:空气气氛、300~500 ℃活化,250 ℃氢气中还原。

关键词: 活化条件, 铂, SO42?/ZrO2-Al2O3, 正己烷, 异构化

Abstract: Pt/SO42?/ZrO2-Al2O3 (PSZA) catalyst was prepared by impregnating SO42?/ZrO2-Al2O3 with H2PtCl6. The effect of activation condition on n-hexane isomerization activity of PSZA catalyst was investigated. The catalyst was characterized by temperature-programmed oxidation (TPO-MS), temperature-programmed nitrogen treatment (TPN-MS) and temperature-programmed reduction (TPR-MS). The n-hexane isomerization activity of the catalyst was evaluated in a continuous flow fixed bed reactor. The experiment results showed that the conversion of n-hexane over PSZA was about 85% when it was activated in air at the temperature ranging from 200 ℃ to 500 ℃. However, the catalyst hardly possessed the isomerization activity when PSZA was activated in nitrogen at above 300 ℃. The reduction pretreatment at a high temperature above 300 ℃ led to the great decrease in catalytic activity. It was proposed that the role of activation in air at a high temperature was not only removal of water on the catalyst, but also re-oxidation of catalyst surface, which led to high catalytic activity. However, the pre-treatment in hydrogen gas at a high temperature led to the loss of sulfur species over PSZA, resulting in significant decrease in catalytic activity. The suitable activation condition was as follows:pretreatment in air at the temperature ranging from 300 ℃ to 500 ℃ and reduction in hydrogen gas at 250 ℃.

Key words: activation condition, Pt, SO42?/ZrO2-Al2O3, n-hexane, isomerization

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