物理化学学报 >> 2004, Vol. 20 >> Issue (02): 149-153.doi: 10.3866/PKU.WHXB20040208

研究论文 上一篇    下一篇

杂化MCM-41固载催化剂的合成、表征及催化研究

聂春发;索继栓   

  1. 中国科学院兰州化学物理研究所,羰基合成与选择氧化国家重点实验室,兰州　730000; 解放军第一医院,兰州　730030
  • 收稿日期:2003-08-04 修回日期:2003-09-29 发布日期:2004-02-15
  • 通讯作者: 索继栓 E-mail:jssuo@ns.lzb.ac.cn

Synthesis,Characterization and Catalytic Applications of Asymmetric Hydrogenation Catalyst Immobilized on Hybrid MCM-41

Nie Chun-Fa;Suo Ji-Shuan   

  1. State Key Laboratory for Oxo Synthesis and Selective Oxidation, Lanzhou Institute of Chemical Physics, Chinese Academy of Sciences, Lanzhou　730000;The First Hospital of People’s Liberation Army, Lanzhou　730030
  • Received:2003-08-04 Revised:2003-09-29 Published:2004-02-15
  • Contact: Suo Ji-Shuan E-mail:jssuo@ns.lzb.ac.cn

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摘要： 用γ-氯丙基三乙氧基硅烷和正硅酸乙酯混合在模板剂引导下共水解合成了有机-无机杂化的介孔分子筛MCM-41,通过与(1R,2R)-1,2-环己二胺和[RuCl2(p-cymene)]2反应,制成了固载化的不对称氢转移反应催化剂,并进行了FT-IR、XRD和N2吸附脱附的表征.不对称氢转移催化反应结果表明,在催化还原苯乙酮成α-苯乙醇的反应中,平均转化率为6.42％,产物平均ee（对映体过量）值为12.64％,固载化催化剂与其匀相体系的催化性能相比(转化率为3.56％,ee值为33.04％),转化率更高,ee值有一定程度的降低.

关键词: 有机-无机杂化, 介孔分子筛MCM-41, 不对称氢转移反应, 固载催化剂

Abstract: Organic-inorganic hybrid mesoporous molecular sieve MCM-41 was synthesized by co-condensation of tetraethoxysilane (TEOS) and 3-chlorpropyl-triethoxysilane, then reacted with (1R,2R)-1,2-diaminocyclohexane and dichloro(p-cymene)-ruthenium dimer successively to afford immobilized asymmetric hydrogen transfer catalyst. The prepared catalyst was characterized by means of FT-IR, PXRD and N2 adsorption-desorption isotherms,and was applied in asymmetric hydrogen transfer reactions of reduction of acetophenone to α-phenyl ethanol. It showed an average conversion of 6.42％ and ee (enantiomeric excess) value of 12.64％ in all 3 performances. The conversion was a little higher than its corresponding homogenous counterpart (conversion of 3.56％ and ee value of 33.04％), while the ee values were somewhat lower.

Key words: Organic-inorganic hybrid, Mesoporous molecular sieve MCM-41, 　Asymmetric hydrogen transfer, Immobilized catalyst