Acta Phys. -Chim. Sin. ›› 2016, Vol. 32 ›› Issue (2): 510-518.doi: 10.3866/PKU.WHXB201511134

• ARTICLE • Previous Articles     Next Articles

Highly Stable CsNO3/SiO2 Catalysts for the Synthesis of Vinylidene Chloride Using a Gaseous Phase Method

Yan-Xia JIN1,Cen TANG1,Xiu-Qing MENG1,Xiao-Xia WANG1,Guan-Qun XIE1,2,*(),Meng-Fei LUO1,*(),Xiao-Nian LI2   

  1. 1 Key Laboratory of the Ministry of Education for Advanced Catalysis Materials, Institute of Physical Chemistry, Zhejiang Normal University, Jinhua 321004, Zhejiang Province, P. R. China
    2 State Key Laboratory Breeding Base of Green Chemistry Synthesis Technology, Industrial Catalysis Institute, Zhejiang University of Technology, Hangzhou 310032, P. R. China
  • Received:2015-09-14 Published:2016-01-30
  • Contact: Guan-Qun XIE,Meng-Fei LUO E-mail:gqxie@zjnu.edu.cn;mengfeiluo@zjnu.cn
  • Supported by:
    the National Natural Science Foundation of China(21476207);Open Research Fund of Top Key Discipline ofChemistry in Zhejiang Provincial Colleges, China, and Key Laboratory of the Ministry of Education for Advanced Catalysis Materials, China(ZJHX201413)

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Abstract:

CsNO3/SiO2 catalysts were prepared using an impregnation method, and were applied in the vapor phase catalytic synthesis of vinylidene chloride (VDC) from 1, 1, 2-trichloroethane (TCE). The influence of reaction temperature on the deactivation of CsNO3/SiO2 catalysts was investigated in detail. It was found that low reaction temperatures ( < 350 ℃) lead to a rapid deactivation, while high reaction temperatures (> 400 ℃) result in a high and stable catalytic activity. During the dehydrochlorination process, CsNO3 species were transformed into CsCl, and coke was formed and deposited on the catalyst surface. However, the chemical change of the Cs species and deposited coke were not the main reason for the deactivation of CsNO3/SiO2 catalyst. Some chlorine-containing species (organic products or HCl) were formed during the reaction and were difficult to desorb from the catalyst surface, which accounts for the deactivation of CsNO3/SiO2 catalysts at low reaction temperatures. High temperature treatment (550 ℃) in a non-oxidizing atmosphere could remove the contaminants and regenerate the catalysts completely. The life test of CsNO3/SiO2 catalyst was carried out at 400 ℃ for 100 h. The TCE conversion and the selectivity to VDC remained stable at 98% and 78%, respectively, showing good prospect for industrial applications.

Key words: Vinylidenechloride, 1, 1, 2-Trichloroethane, CsNO3, Dehydrochlorination, Heterogeneous reaction