催化学报 ›› 2008, Vol. 29 ›› Issue (5): 482-488.

• 研究论文 • 上一篇    下一篇

CuO/SBA-15催化剂上巴豆醛选择性加氢

王月娟,王雪俐,谢冠群,鲁继青,金炜阳,刘西敬,罗孟飞   

  1. 浙江师范大学物理化学研究所浙江省固体表面反应化学重点实验室, 浙江金华 321004
  • 收稿日期:2008-05-25 出版日期:2008-05-25 发布日期:2012-05-02

Crotonaldehyde Hydrogenation over CuO/SBA-15 Catalyst

WANG Yuejuan, WANG Xueli, XIE Guanqun, LU Jiqing, JIN Weiyang, LIU Xijing, LUO Mengfei*   

  1. Zhejiang Key Laboratory for Reactive Chemistry on Solid Surfaces, Institute of Physical Chemistry, Zhejiang Normal University, Jinhua 321004, Zhejiang, China
  • Received:2008-05-25 Online:2008-05-25 Published:2012-05-02

摘要: 通过γ-氨丙基三甲氧基硅烷(APTS)偶联与Cu2+离子络合两步法将CuO负载到介孔分子筛SBA-15上,制得CuO/SBA-15催化剂,考察了催化剂的巴豆醛选择性加氢反应性能. 通过X射线粉末衍射、氮气吸脱附和程序升温还原(TPR)技术对催化剂进行了表征. 结果表明, SBA-15分子筛负载CuO后保持原有的介孔结构,但是孔容和比面表积随着CuO负载量的增大而下降. TPR结果表明CuO/SBA-15系列催化剂有三种CuO物种: 高分散CuO、晶相CuO和进入SBA-15分子筛骨架的Cu2+. 高分散CuO物种对巴豆醛加氢反应的催化活性最高,晶相CuO物种次之,而进入SBA-15分子筛骨架的Cu2+物种几乎没有活性.

关键词: 氧化铜, SBA-15分子筛, 巴豆醛, 加氢, γ-氨丙基三甲氧基硅烷

Abstract: CuO catalysts supported on SBA-15 were prepared by chelating Cu2+with γ-aminopropyltrimethoxysilane (APTS) on the SBA-15 support and were tested for selective hydrogenation of crotonaldehyde. The CuO/SBA-15 catalysts with different CuO loadings were characterized byX-raydiffraction, N2 sorption, and hydrogen temperature-programmed reduction (H2-TPR). N2 sorption results showed that the samples maintained a fine 2D-hexagonal structure after the CuO was loaded, whereas the BET surface area and pore volume decreased with increasing Cu content. H2-TPR results revealed that there were three Cu species: finely dispersed CuO, bulk CuO, and Cu2+ions incorporated into the framework of SBA-15. Catalytic activity of each species was evaluated. The finely dispersed CuO had the highest activity, and the bulk CuO had medium activity, while the Cu2+in the SBA-15 framework was inactive in the reaction. These indicated that the finely dispersed Cu species were the active phase for the reaction. Furthermore, the catalyst calcined under N2 instead of air could increase the content of the finely dispersed CuO, which could consequently enhance the catalytic activity.

Key words: copper oxide, SBA-15 molecular sieve, crotonaldehyde, hydrogenation, γ-aminopropyltrimethoxysilane