Effect of synthesis parameters on the chromium content and catalytic activities of mesoporous Cr-MSU-x prepared under acidic conditions

被引:23
作者
Liu, Licheng
Li, Huiquan
Zhang, Yi
机构
[1] Chinese Acad Sci, Inst Proc Engn, Beijing 100080, Peoples R China
[2] Grad Univ, Chinese Acad Sci, Beijing 100049, Peoples R China
关键词
MCM-41; MOLECULAR-SIEVES; OXIDATIVE DEHYDROGENATION; OXIDE CATALYSTS; CARBON-DIOXIDE; PORE-SIZE; SILICA; ETHANE; PERFORMANCES; SURFACTANTS; ETHYLENE;
D O I
10.1021/jp061875o
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
A series of chromium-incorporated MSU-x mesoporous molecular sieves were synthesized under different templates, initial Si/Cr molar ratios, aging times, and temperatures in acid solution. The synthesis was performed by using sodium silicate, chromium nitrate, and nonionic poly(ethylene oxide) surfactant as the source of silicone, metal, and the template, respectively. The Cr-MSU-x products were analyzed by inductively couple plasma-optical emission spectrometry to determine the actual Cr content and were characterized by X-ray diffraction, N-2 adsorption-desorption, scanning electron microscopy, high-resolution transmission electron microscopy, diffuse reflectance UV-visible, X-ray adsorption near-edge spectroscopy, and temperature-programmed reduction techniques. The Cr species were mostly formed as Cr(VI) in tetrahedral coordination. Two kinds of Cr(VI) species with different reduction abilities were distinguished. The catalytic activities of Cr-MSU-x in the dehydrogenation of ethane to ethylene with CO2 were investigated at the same time. The synthesis parameters explored strongly influence the chromium content in Cr-MSU-x and, subsequently, the catalytic activities. The Cr-MSU-x synthesized with Si/Cr = 20, aging at 25 degrees C for 22 h, and templating by fatty alcohol polyoxyethylene ether gave the best activities, resulting in 58.0% ethane conversion and 92.1% ethylene selectivity. The Cr species in Cr-MSU-x are more efficient in activating and converting ethane molecules than are conventional catalysts.
引用
收藏
页码:15478 / 15485
页数:8
相关论文
共 32 条
[21]   Synthesis of mesoporous silica with tunable pore size from sodium silicate solutions and a polyethylene oxide surfactant [J].
Sierra, L ;
Guth, JL .
MICROPOROUS AND MESOPOROUS MATERIALS, 1999, 27 (2-3) :243-253
[22]  
STEPHEN AB, 1998, MICROPOR MESOPOR MAT, V22, P419
[23]   Behavior of active sites on Cr-MCM-41 catalysts during the dehydrogenation of propane with CO2 [J].
Takehira, K ;
Ohishi, Y ;
Shishido, T ;
Kawabata, T ;
Takaki, K ;
Zhang, QH ;
Wang, Y .
JOURNAL OF CATALYSIS, 2004, 224 (02) :404-416
[24]   Preparation and catalytic performances of ultralarge-pore TiSBA-15 mesoporous molecular sieves with very high Ti content [J].
Vinu, A ;
Srinivasu, P ;
Miyahara, M ;
Ariga, K .
JOURNAL OF PHYSICAL CHEMISTRY B, 2006, 110 (02) :801-806
[25]  
Wang SB, 2000, APPL CATAL A-GEN, V196, P1, DOI 10.1016/S0926-860X(99)00450-0
[26]   Characterizations and catalytic properties of Cr-MCM-41 prepared by direct hydrothermal synthesis and template-ion exchange [J].
Wang, Y ;
Ohishi, Y ;
Shishido, T ;
Zhang, QH ;
Yang, W ;
Guo, Q ;
Wan, HL ;
Takehira, K .
JOURNAL OF CATALYSIS, 2003, 220 (02) :347-357
[27]   Alkane dehydrogenation over supported chromium oxide catalysts [J].
Weckhuysen, BM ;
Schoonheydt, RA .
CATALYSIS TODAY, 1999, 51 (02) :223-232
[28]   XANES study of Cr sorbed by a kitchen waste compost from water [J].
Wei, YL ;
Lee, YC ;
Hsieh, HF .
CHEMOSPHERE, 2005, 61 (07) :1051-1060
[29]   Characteristics of chromium oxides supported on TiO2 and Al2O3 for the decomposition of perchloroethylene [J].
Yim, SD ;
Nam, IS .
JOURNAL OF CATALYSIS, 2004, 221 (02) :601-611
[30]  
Yu JQ, 2001, CHINESE J CATAL+, V22, P331