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Frontiers of Chemical Science and Engineering

ISSN 2095-0179

ISSN 2095-0187(Online)

CN 11-5981/TQ

邮发代号 80-969

2019 Impact Factor: 3.552

Frontiers of Chemical Science and Engineering  2012, Vol. 6 Issue (4): 415-422   https://doi.org/10.1007/s11705-012-1214-4
  RESEARCH ARTICLE 本期目录
Influence of crystalline phase of Li-Al-O oxides on the activity of Wacker-type catalysts in dimethyl carbonate synthesis
Influence of crystalline phase of Li-Al-O oxides on the activity of Wacker-type catalysts in dimethyl carbonate synthesis
Yadong GE, Yuanyuan DONG, Shengping WANG, Yujun ZHAO, Jing LV, Xinbin MA()
Key Laboratory for Green Chemical Technology (Ministry of Education), School of Chemical Engineering and Technology, Tianjin University, Tianjin 300072, China
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Abstract

The catalysts supported on LiAl5O8 (spinel) for vapor phase synthesis of dimethyl carbonate (DMC) from methyl nitrite (MN) have been studied. Their catalytic activities on supports prepared by different methods were evaluated in a continuous reactor. The samples were characterized by powder X-ray diffraction, N2 adsorption-desorption isotherms, fourier transform infrared spectroscopy and temperature-programmed reduction of H2. Li/Al molar ratio and calcination temperature greatly influence the structure of crystalline phase of Li-Al-O oxides. Desirable LiAl5O8 (spinel) was formed at 800°C, while LiAl5O8 (primitive cube) formed at 900°C is undesirable for the reaction. A high Li/Al molar ratio, which was related with LiAlO2, also slowed the reaction rate. The electron transfer ability and the interaction with active component are the important properties of the spinel-based supports. The CuCl2-PdCl2/LiAl5O8 (spinel) with better electron transfer ability and low Pd2+ reduction temperature exhibited a better catalytic ability.

Key wordsWacker-type catalyst    dimethyl carbonate    methyl nitrite    spinel
收稿日期: 2012-04-26      出版日期: 2012-12-05
Corresponding Author(s): MA Xinbin,Email:xbma@tju.edu.cn   
 引用本文:   
. Influence of crystalline phase of Li-Al-O oxides on the activity of Wacker-type catalysts in dimethyl carbonate synthesis[J]. Frontiers of Chemical Science and Engineering, 2012, 6(4): 415-422.
Yadong GE, Yuanyuan DONG, Shengping WANG, Yujun ZHAO, Jing LV, Xinbin MA. Influence of crystalline phase of Li-Al-O oxides on the activity of Wacker-type catalysts in dimethyl carbonate synthesis. Front Chem Sci Eng, 2012, 6(4): 415-422.
 链接本文:  
https://academic.hep.com.cn/fcse/CN/10.1007/s11705-012-1214-4
https://academic.hep.com.cn/fcse/CN/Y2012/V6/I4/415
Calcination temperature /°CSpecific surface area /(m2·g–1)Pore volume /(cm3·g–1)Pore diameter /nm
700128.80.338.8
800103.20.309.5
90080.10.2811.7
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SupportsLi/Al (molar) ratioCalcination at 800°C
LiAl-0.050.05γ-Al2O3 + LiAl5O8
LiAl-0.100.10γ-Al2O3 + LiAl5O8
LiAl-0.150.15γ-Al2O3 + LiAl5O8
LiAl-0.200.20LiAl5O8 + LiAlO2
LiAl-0.250.25LiAl5O8 + LiAlO2
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SupportsSpecific surface area /(m2·g–1)Pore volume /(cm3·g–1)Pore diameter /nm
γ-Al2O3178.40.335.9
LiAl-0.05134.30.337.8
LiAl-0.10126.00.338.3
LiAl-0.15103.20.309.5
LiAl-0.20?97.60.309.9
LiAl-0.25?70.00.2512.3?
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