催化学报

催化学报 ›› 2007, Vol. 28 ›› Issue (12): 1101-1106.

• 研究论文 • 上一篇    下一篇

介孔载体嫁接的Schiff碱铬配合物催化氧化苯甲醇合成苯甲醛

王晓丽1,2,吴功德1,2,李军平1,肖福魁1,魏伟1,孙予罕1   

  1. 1 中国科学院山西煤炭化学研究所煤转化国家重点实验室, 山西太原 030001; 2 中国科学院研究生院, 北京 100049
  • 收稿日期:2007-12-25 出版日期:2007-12-25 发布日期:2007-12-25

Oxidation of Benzyl Alcohol to Benzaldehyde Catalyzed by Chromium Schiff Base Complexes Immobilized on Mesoporous Supports

WANG Xiaoli1,2, WU Gongde1,2, LI Junping1, XIAO Fukui1, WEI Wei1*, SUN Yuhan1   

  1. 1 State Key Laboratory of Coal Conversion, Institute of Coal Chemistry, The Chinese Academy of Sciences, Taiyuan 030001, Shanxi, China; 2 Graduate University of Chinese Academy of Sciences, Beijing 100049, China
  • Received:2007-12-25 Online:2007-12-25 Published:2007-12-25

PDF

1074

被引次数

33

摘要： 将Cr(salen)配合物分别嫁接于介孔SiO2, MCM-41和SBA-15上制备成非均相Schiff碱铬配合物,并用FT-IR, UV-Vis, XRD, N2吸附和元素分析等对非均相铬配合物进行了表征. 以30%的H2O2为氧化剂,以非均相铬配合物为催化剂,在无有机溶剂、相转移催化剂和添加剂的条件下,研究了选择性催化氧化苯甲醇合成苯甲醛的反应. 结果表明,非均相铬配合物都表现出较好的催化性能. 选择不同的介孔载体对非均相铬配合物的催化性能有较大的影响, Cr(salen)/MCM-41配合物显示有最好的催化性能; 在优化的反应条件下,苯甲醇转化率可达52.5%, 苯甲醛选择性为100%, 且该非均相铬配合物重复使用4次后仍保持较好的催化性能.

关键词: 铬, N, N-双水杨醛缩乙二胺配体, 介孔载体, 非均相配合物, 席夫碱, 苯甲醇, 选择性氧化, 苯甲醛

Abstract: In order to investigate the effect of different mesoporous supports on the catalytic performance of heterogeneous complexes, three representative siliceous mesoporous materials (SiO2, MCM-41, and SBA-15) were selected as supports to immobilize the same chromium salen Schiff base complex. The coordination structure and textural properties of the heterogeneous complexes were characterized by various physico-chemical measurements such as FT-IR, UV-Vis, XRD, N2 adsorption, and elemental analysis. The heterogeneous complexes were effective catalysts for the selective oxidation of benzyl alcohol to benzaldehyde using 30%H2O2 as the oxidant, and they all exhibited much better catalytic performance than their homogeneous analogues. Simultaneously, the catalytic performance of the heterogeneous complexes was also closely related to the used supports, and the complex Cr(salen)/MCM-41 exhibited the best catalytic performance. Under the optimal reaction conditions, the conversion of benzyl alcohol could reach 52.5% with 100% of selectivity for benzaldehyde. In addition, the catalytic performance was remained after being reused 4 times.

Key words: chromium, N, N-bis(salicylideneamino)ethane (salen) ligand, mesoporous support, heterogeneous complex, Schiff base, benzyl alcohol, selective oxidation, benzaldehyde