| 杨光,李臣芝,陈彤.制备条件对Cu-MnOx低温液相甲醇合成性能影响[J].分子催化,2015,(2):143-151 |
| 制备条件对Cu-MnOx低温液相甲醇合成性能影响 |
| Effect of Preparation Conditions on Catalystic Performance of Cu-MnOx for Low-temperature Methanol Synthesis |
| 投稿时间：2015-02-12 修订日期：2015-04-03 |
| DOI： |
| 中文关键词: CO/CO2/H2 低温液相 甲醇 Cu-MnOx K2CO3 |
| 英文关键词:CO/CO2/H2 low-temperature methanol Cu-MnOx K2CO3 |
| 基金项目: |
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| 摘要点击次数: 1310 |
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| 中文摘要: |
| 采用并流共沉淀法制备Cu-MnOx催化剂，用于合成气CO/CO2/H2为原料的低温液相甲醇合成。研究了制备条件对Cu-MnOx结构及催化性能的影响，XRD、H2-TPR、CO-TPD表征显示，制备过程中的沉淀pH、煅烧温度等影响Cu-MnOx中CuO的分散性、还原性能和对CO的吸附能力。沉淀pH为7、煅烧温度450℃制备的铜锰摩尔比为1:1的Cu-MnOx铜锰相互作用强，CuO分散好，形成的Cu1.5Mn1.5O4晶相利于中间产物甲酸酯的生成，并且其对CO的吸附能力强，H2还原温度适中，利于在预还原条件下生成较多Cu+，因此，表现出最好的催化性能。在170℃、5MPa反应条件下，以K2CO3为助剂、乙醇为溶剂，碳转率为71.8%，甲醇选择性55.9%，同时生成了较多的碳链增长产物，说明CO在该催化剂上可发生解离吸附，为乙醇等C2+低碳醇的合成提供参考。 |
| 英文摘要: |
| Cu-MnOx catalyst was prepared by co-precipitation method and was used for low-temperature methanol synthesis from syngas(CO/CO2/H2). The effect of preparing conditions of Cu-MnOx catalyst on the structure and catalytic performance were studied by XRD, H2-TPR and CO-TPD. The results showed that the Cu/Mn molar ratio, the precipitation pH and the calcination temperature affected the CuO dispersion, the reducibility and the adsorption capacity of CO of Cu-MnOx. Using ethanol as solvent and K2CO3 as additive at 170℃ and 5MPa, the highest carbon conversion of 71.8% along with a methanol selectivity of 55.9% was obtained over the Cu-MnOx with Cu/Mn molar ratio of 1 prepared at the pH value of 7 and the calcination temperature of 450℃. For the Cu-MnOx prepared under the optimum preparation conditions, a strong intereaction between Cu and Mn, highly dispersed CuO, a strong adsorption capacity of CO and a suitable reduction temperature were obtained. Therefore, more Cu+ would be attained on the catalyst reduced by H2, and Cu+ was favourable for the low-temperature methanol synthesis. In addition, ethyl acetate was obtained over Cu-MnOx, which indicated that CO was dissociated on the catalyst and would provide a reference for higher alcohols synthesis. |
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