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化学学报
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化学学报 ›› 2008, Vol. 66 ›› Issue (11): 1287-1292.    下一篇

研究论文

Cr-Cu/SiO2催化剂上顺酐和1,4-丁二醇的耦合反应

沈伟，潘超，杨新艳，徐华龙*   

  1. (复旦大学化学系 上海市分子催化与功能材料重点实验室 上海 200433)
  • 投稿日期:2007-10-26 修回日期:2007-12-24 发布日期:2008-06-14
  • 通讯作者: 徐华龙

Coupling Reaction of 1,4-Butanediol with Maleic Anhydride over Cr-Cu/SiO2 Catalysts

SHEN, Wei; PAN, Chao; YANG, Xin-Yan; XU, Hua-Long*   

  1. (Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Department of Chemistry, Fudan University, Shanghai 200433)
  • Received:2007-10-26 Revised:2007-12-24 Published:2008-06-14
  • Contact: XU, Hua-Long

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研究了Cr-Cu/SiO2催化剂上顺酐加氢反应和1,4-丁二醇脱氢反应耦合制备重要的精细化学品γ-丁内酯. 耦合反应显著提高了顺酐转化率和γ-丁内酯选择性. Cr修饰提高了催化剂的脱氢活性, 抑止了催化剂的过度加氢活性, 使1,4-丁二醇的转化率和γ-丁内酯选择性显著提高. Cr修饰量为w＝5%的Cr-Cu/SiO2催化剂上耦合反应的原料转化率为100%, γ-丁内酯选择性达98.8%. XRD, XPS等研究表明, Cr修饰促进了催化剂上铜元素的分散, 氧化铬对氧化铜有给电子作用, Cr修饰的Cr-Cu/SiO2催化剂还原后比Cu/SiO2具有更多的Cu＋, 这有利于催化剂脱氢活性和γ-丁内酯选择性的提高.

关键词: 顺丁烯二酸酐, 1,4-丁二醇, γ-丁内酯, 耦合反应, Cr-Cu/SiO2

The coupling process of dehydrogenation of 1,4-butanediol with hydrogenation of maleic anhydride over Cr-Cu/SiO2 catalysts to produce one important fine chemical γ-butyrolactone was studied, which shows advantages over the conventional processes. Cr improved the selectivity to γ-butyrolactone and conversion of 1,4-butanediol. The conversion of 1,4-butanediol and maleic anhydride reached 100%, and the selectivity to γ-butyrolactone was 98.8% over w＝5% Cr2O3 modified Cr-Cu/SiO2. The results of XRD, XPS and TPR revealed that Cr improved the dispersion of Cu and had the electron donating effect on Cu. There are more Cu＋ species on reduced Cr-Cu/SiO2 than Cu/SiO2. Cu＋ is beneficial for dehydrogenation of 1,4-butanediol and the coupling process.

Key words: maleic anhydride, 1,4-butanediol, γ-butyrolactone, coupling process, Cr-Cu/SiO2