Direct synthesis of organic carbonates from the reaction of CO2 with methanol and ethanol over CeO2 catalysts

Direct synthesis of organic carbonates from the reaction of CO2 with methanol and ethanol over CeO2 catalysts
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DOI:
10.1016/j.cattod.2006.02.027
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发表时间:
2006-06-30
期刊:
影响因子:
5.3
通讯作者:
Tomishige, Keiichi
Tomishige, Keiichi
中科院分区:
化学2区
文献类型:
--
作者:
Yoshida, Yuichi;Arai, Yoko;Tomishige, Keiichi

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研究了CeO2催化剂在甲醇和CO2直接合成碳酸二甲酯(DMC)反应中的催化性能。在873 K及以上焙烧的催化剂上,DMC的生成速率与催化剂的比表面积几乎成正比。然而,CeO2煅烧在673 K显示出较低的活性比预期的表面积。从催化剂表征的结果,CeO2在673 K焙烧含有相当数量的非晶相。相反,在873 K及以上焙烧的催化剂上,非晶相的比例降低。在CH_3OH + C_2H_5OH + CO_2低温反应中,生成了碳酸甲乙酯(EMC),其选择性与DMC相当。通过与酯交换反应的比较,探讨了其生成途径。(c)2006 Elsevier B.V.保留所有权利。
The catalytic properties of CeO2 catalysts in direct synthesis of dimethyl carbonate (DMC) from CH3OH and CO2 were investigated. The formation rate of DMC over the catalysts calcined at 873 K and above was almost proportional to the surface area of catalysts. However, CeO2 calcined at 673 K showed lower activity than expected from the surface area. From the results of catalyst characterization, CeO2 calcined at 673 K contained considerable amount of amorphous phase. In contrast, the ratio of amorphous phase decreased on the catalysts calcined at 873 K and above. This suggests that stable crystallite surface is active for the reaction.In the CH3OH + C2H5OH + CO2 reaction at low temperature, ethyl methyl carbonate (EMC) was formed, and selectivity of EMC formation was comparable to that of DMC. The formation route is discussed by the comparison with transesterification reaction. (c) 2006 Elsevier B.V. All rights reserved.