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XGa2O3-CeO2-ZrO2 (X=0, 1, 3, 5, 7, and 9) catalysts were prepared by a single-step sol-gel method with a variation of Ga2O3 content (X, wt%). Based on our previous work, the ratio of cerium oxide : zirconium oxide in the XGa2O3-CeO2-ZrO2 catalyst was fixed to be Ce0.6Zr0.4O2. The prepared catalysts were applied to the direct synthesis of DMC from methanol and carbon dioxide. XGa2O3-CeO2- ZrO2 (X=1, 3, 5, 7, and 9) showed a better catalytic performance than 0Ga2O3-CeO2-ZrO2 (Ce0.6Zr0.4O2) in the reaction due to the enhanced acidity and basicity provided by Ga2O3. Among the catalysts tested, 3Ga2O3-CeO2-ZrO2 catalyst showed the best catalytic performance in the direct synthesis of DMC from methanol and carbon dioxide. Furthermore, the amount of DMC produced over 3Ga2O3-CeO2-ZrO2 catalyst prepared by a single-step sol-gel method was larger than that over 5Ga2O3/Ce0.6Zr0.4O2 catalyst (the best catalyst in our previous work) prepared by an incipient wetness impregnation method. This indicates that a single-step sol-gel method was more efficient than an incipient wetness impregnation method in the preparation of Ga2O3-CeO2-ZrO2 mixed metal oxide catalyst for the reaction. NH3-TPD and CO2-TPD experiments were conducted to investigate the effect of acidity and basicity of the catalyst on the catalytic performance in the direct synthesis of DMC from methanol and carbon dioxide. Experimental results revealed that the catalytic performance of XGa2O3-CeO2-ZrO2 was closely related to both acidity and basicity of the catalyst in this reaction. The amount of DMC increased with increasing both acidity and basicity of the catalyst. It is concluded that both acidity and basicity of the catalyst played important roles in determining the catalytic performance in the direct synthesis of DMC from methanol and carbon dioxide. |
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4楼2013-03-18 15:52:21
sunliuqian
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vigor_smile
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5楼2013-03-19 12:55:47
