Synthesis of dimethyl carbonate by vapor phase oxidative carbonylation of methanol over Cu-based catalysts

Synthesis of dimethyl carbonate by vapor phase oxidative carbonylation of methanol over Cu-based catalysts
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DOI:
10.1016/s1381-1169(01)00073-5
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发表时间:
2001-05-14
影响因子:
--
通讯作者:
Hong, SI
Hong, SI
中科院分区:
化学2区
文献类型:
--
作者:
Han, MS;Lee, BG;Hong, SI

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采用气相流反应系统,在铜基催化剂存在下,研究了甲醇氧化羰基化合成碳酸二甲酯(DMC)的反应。以活性炭(AC)为载体,采用常规浸渍法制备了一系列铜基催化剂。从甲醇转化率和DMC选择性方面深入评估了各种促进剂和反应条件对催化反应活性的影响。还通过 X 射线衍射和 SEM 进行形态分析,以表征所使用的催化剂。无论催化剂组成如何,甲醇氧化羰基化的最佳反应温度被发现为120-130℃左右。在100℃以下反应速率太慢,而在150℃以上则产生过多副产物。在所使用的各种催化剂中,OH/Cu摩尔比= 0.5-1.0的CuCl2/NaOH/AC催化剂表现出最好的催化性能,这似乎与中间物质Cu-2(OH)(3)Cl的形成有很强的关系。 (C) 2001 Elsevier Science B.V. 保留所有权利。
Dimethyl carbonate (DMC) synthesis reaction by oxidative carbonylation of methanol has been studied using vapor phase flow reaction system in the presence of Cu-based catalysts. A series of Cu-based catalysts were prepared by the conventional impregnation method using activated carbon (AC) as support. The effect of various promoters and reaction conditions on the catalytic reactivities were intensively evaluated in terms of methanol conversion and DMC selectivity. The morphological analysis by X-ray diffraction and SEM was also conducted in order to characterize the emloyed catalysts. Regardless of catalyst compositions, the optimal reaction temperature for oxidative carbonylation of methanol was found to be around 120-130 degreesC. The reaction rate was too slow below 100 degreesC, while too much by-products was produced above 150 degreesC. Among the various catalysts employed, CuCl2/NaOH/AC catalyst with the molar ratio of OH/Cu = 0.5-1.0, has shown the best catalytic performance, which appears to have a strong relationship with the formation of intermediate species, Cu-2(OH)(3)Cl. (C) 2001 Elsevier Science B.V. All rights reserved.