Synthesis of lanthanum-doped MCM-48 molecular sieves and its catalytic performance for the oxidation of styrene

被引:80
作者
Zhan, Wangcheng [1 ]
Guo, Yanglong [1 ]
Wang, Yanqin [1 ]
Liu, Xiaohui [1 ]
Guo, Yun [1 ]
Wang, Yunsong [1 ]
Zhang, Zhigang [1 ]
Lu, Guanzhong [1 ]
机构
[1] E China Univ Sci & Technol, Res Inst Ind Catalysis, Adv Mat Lab, Shanghai 200237, Peoples R China
关键词
D O I
10.1021/jp074521l
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Lanthanum-doped MCM-48 molecular sieves with different La contents were synthesized hydrothermally and characterized by X-ray diffraction (XRD), nitrogen sorption, transmission electron microscopy (TEM), UV-visible spectroscopy, and Fourier transform infrared (FT-IR) spectroscopy. The results show that the majority of La cations have been incorporated into the framework of MCM-48 molecular sieves. When the molar ratio of La/Si is > 0.039 in the sample, some of lanthanurn species exist in the extraframework. Compared with pure silicate MCM-48, lanthanum-doped MCM-48 samples show the medium strong acidity that is due to the incorporation of La in the framework of silica. In the oxidation of styrene with H2O2 as the oxidant over the lanthanum-doped MCM-48 catalysts, benzaldehyde is the main product with a small amount of styrene oxide. The La content in the catalysts, reaction temperature, reaction time, and solvent affect greatly the catalytic oxidation of styrene. The conversion of styrene and the selectivity to styrene oxide increase noticeably when a small amount of NaOH aqueous solution is added into the reaction mixture. Ln-doped MCM-48 catalysts with 14 kinds of rare earth elements were synthesized hydrothermally and evaluated for the oxidation of styrene. The results show that their catalytic performance is tremendously different and depends on the nature of rare earth elements doped in the MCM-48 mesoporous materials.
引用
收藏
页码:12103 / 12110
页数:8
相关论文
共 35 条
[1]   Structure of MCM-48 revealed by transmission electron microscopy [J].
Alfredsson, V ;
Anderson, MW .
CHEMISTRY OF MATERIALS, 1996, 8 (05) :1141-1146
[2]   EPOXIDATION OF LOWER OLEFINS WITH HYDROGEN-PEROXIDE AND TITANIUM SILICALITE [J].
CLERICI, MG ;
INGALLINA, P .
JOURNAL OF CATALYSIS, 1993, 140 (01) :71-83
[3]   Solvent effects during the oxidation of olefins and alcohols with hydrogen peroxide on Ti-beta catalyst: The influence of the hydrophilicity-hydrophobicity of the zeolite [J].
Corma, A ;
Esteve, P ;
Martinez, A .
JOURNAL OF CATALYSIS, 1996, 161 (01) :11-19
[4]   STRUCTURE ORGANIZATION OF SILICATE POLYANIONS WITH SURFACTANTS - A NEW APPROACH TO THE SYNTHESES, STRUCTURE TRANSFORMATIONS, AND FORMATION MECHANISMS OF MESOSTRUCTURAL MATERIALS [J].
FYFE, CA ;
FU, GY .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1995, 117 (38) :9709-9714
[5]   Synthesis, characterization and catalytic properties in oxidation of styrene over cobalt-substituted microporous nickel phosphate CoVSB-5 [J].
Gao, DM ;
Gao, QM .
MICROPOROUS AND MESOPOROUS MATERIALS, 2005, 85 (03) :365-373
[6]   Characterization of Cu/MCM-41 and Cu/MCM-48 mesoporous catalysts by FTIR spectroscopy of adsorbed CO [J].
Hadjiivanov, K ;
Tsoncheva, T ;
Dimitrov, M ;
Minchev, C ;
Knözinger, H .
APPLIED CATALYSIS A-GENERAL, 2003, 241 (1-2) :331-340
[7]   The solvent effect in the sulfoxidation of thioethers by hydrogen peroxide using Ti-containing zeolites as catalysts [J].
Hulea, V ;
Moreau, P .
JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL, 1996, 113 (03) :499-505
[8]  
ISABEL D, 2004, J MATER CHEM, V14, P48
[9]   Novel isomerization of omega-phenylalkanals to phenyl alkyl ketones over cesium (lanthanum) oxide supported on mesoporous aluminosilicate molecular sieves and related materials [J].
Kloetstra, KR ;
vandenBroek, J ;
vanBekkum, H .
CATALYSIS LETTERS, 1997, 47 (3-4) :235-242
[10]   Hydrothermal synthesis and characterization of uranium-containing MCM-48 samples [J].
Kumar, D ;
Pillai, KT ;
Sudersanan, V ;
Dey, GK ;
Gupta, NM .
CHEMISTRY OF MATERIALS, 2003, 15 (20) :3859-3865