Surface structure and catalytic performance of CuCl/SiO2-Al2O3 catalysts for methanol oxidative carbonylation

被引:30
作者
Li Zhong [1 ]
Meng Fanhui [1 ]
Ren Jun [1 ]
Zheng Huayan [1 ]
Xie Kechang [1 ]
机构
[1] Taiyuan Univ Technol, Minist Educ & Shanxi Prov, Key Lab Coal Sci & Technol, Taiyuan 030024, Shanxi, Peoples R China
基金
中国国家自然科学基金;
关键词
cuprous chloride; alumina-silica mixed oxide; methanol; oxidative carbonylation; dimethyl carbonate;
D O I
10.1016/S1872-2067(08)60063-7
中图分类号
O69 [应用化学];
学科分类号
081704 ;
摘要
Aluminum was doped into amorphous silica get to modify its surface structure. The obtained SiO2Al2O3 support was used to prepare the CuCl/SiO2-Al2O3 catalyst by solid-state ion exchange, and the catalyst activity for liquid-phase oxidative carbonylation of methanol to dimethyl carbonate was investigated. The results showed that the prepared SiO2-Al2O3 support kept the amorphous structure of the silica gel. The BET specific surface area of the silica gel was decreased to 200 m(2)/g, and the surface acid sites (including Bronsted acid sites) were increased. In the CuCl/SiO2-Al2O3 catalyst, CuCl was not only dispersed on surface but also was ion exchanged with surface Bronsted acid sites of the SiO2-Al2O3 support to form Cu+ species, which resulted in a decrease in BET specific surface area to 148 m(2)/g. These two kinds of Cu+ species on the catalyst surface were both active centers for the oxidative carbonylation of methanol to dimethyl carbonate. When the catalyst was prepared with Si/Al molar ratio of 5 and was calcined at 500 degrees C, the selectivity and space-time yield of dimethyl carbonate reached 74% and 1.27 g/(g(.)h), respectively.
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页码:643 / 648
页数:6
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