催化学报 ›› 2008, Vol. 29 ›› Issue (6): 513-518.

• 研究论文 • 上一篇    下一篇

丝光沸石-氧化铝双组元负载钼催化剂上的1-丁烯歧化反应

刘会娟1,2,黄声骏1,张玲1,2,刘盛林1,王威3,辛文杰1,谢素娟1,徐龙伢1   

  1. 1 中国科学院大连化学物理研究所, 辽宁大连 116023; 2 中国科学院研究生院, 北京 100049; 3 中国石油锦州石化公司, 辽宁锦州 121001
  • 收稿日期:2008-06-25 出版日期:2008-06-25 发布日期:2012-04-28

1-Butene Metathesis over a MoO3/H-Mordenite-Alumina Catalyst

LIU Huijuan1,2, HUANG Shengjun1, ZHANG Ling1,2, LIU Shenglin1, WANG Wei3, XIN Wenjie1, XIE Sujuan1, XU Longya1*   

  1. 1 Dalian Institute of Chemical Physics, The Chinese Academy of Sciences, Dalian 116023, Liaoning, China; 2 Graduate University of Chinese Academy Sciences, Beijing 100049, China; 3 Jinzhou Petrochemical Company, PetroChina, Jinzhou 121001, Liaoning, China
  • Received:2008-06-25 Online:2008-06-25 Published:2012-04-28

摘要: 在固定床反应器上考察了氢型丝光沸石(HM)-氧化铝双组元负载MoO3催化剂上的1-丁烯歧化反应性能,通过氨程序升温脱附、X射线衍射和氢程序升温还原对样品进行了表征. 实验结果表明,在110 ℃, 0.1 MPa, WHSV=1.5 h-1及TOS=1 h的反应条件下, MoO3没有歧化反应活性. Al2O3, HM-Al2O3和HM载体上只生成异构产物,并且载体酸性越强,异构产物越多. MoO3/HM几乎没有歧化活性,而MoO3/Al2O3催化剂上生成了一定量的歧化产物,且各产物收率相近. MoO3/HM-Al2O3具有最高的歧化活性,1-丁烯转化率为84.9%, 丙烯和戊烯收率分别为28.5%和20.6%. 催化剂本身的酸性和载体表面Mo物种存在状态是影响1-丁烯歧化制丙烯反应性能的两个关键因素.

关键词: 丝光沸石, 氧化铝, 钼, 1-丁烯, 歧化

Abstract: Metathesis reactions of 1-butene over a MoO3/H-mordenite-alumina (MoO3/HM-Al2O3) catalyst were investigated in a fixed-bed reactor. The catalysts were characterized by NH3 temperature-programmed desorption,X-raydiffraction, and H2 temperature-programmed reduction. The results indicate that under the reaction conditions of 110 ℃, 0.1 MPa, WHSV=1.5 h-1, and TOS=1 h, MoO3 shows no isomerization and metathesis activities. Al2O3, HM-Al2O3, and HM supports only possess suitable isomerization activity controlled by the acidity of the samples, and the isomerization products increase with the acid strength. The yields of products are close to each other on the MoO3/Al2O3 catalyst with less metathesis activity. MoO3/HM-Al2O3 has the best reaction performance, on which 1-butene conversion, propene yield, and pentene yield are 84.9%, 28.5%, and 20.6%, respectively. The acidity of the catalyst and the oxidation state of Mo species are the two key factors for the catalyst performance for 1-butenemetathesis.

Key words: mordenite, alumina, molybdenum, 1-butene, metathesis