CO加氢合成低碳醇的研究
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摘要
本文使用固定床反应器进行了CO加氢催化合成低碳醇的研究。首先通过共沉淀法和浸渍法制备了Cu-Co基催化剂和Cu-Co/SiO2催化剂,研究了添加K、Ce和Zr助剂对催化剂性能的影响。通过分析H2和CO转化率、CH4和CO2及总醇的选择性、醇的时空产率和单醇的分布,得出优化反应温度、压力和助剂添加量等反应参数。进一步应用BET、XRD和TPR等分析手段进行了催化剂表征。催化剂表征结果表明：添加助剂对催化剂的物理结构、表面物相都产生了一定的影响,尤其是对催化剂的比表面积、分散度以及还原性能影响较为显著。实验结果表明：在催化剂中添加适量助剂后,醇的时空产率和选择性将得到提升,而CH4的选择性下降。通过实验确定了催化合成低碳醇的最佳反应温度为300℃,适宜的反应压力为5Mpa；对于浸渍法制备的Cu-Co/SiO2催化剂,助剂K2O、CeO2和zrO2的最佳添加量分别为0.2%、0.2%、4%。
This paper conducted a study on synthesis of higher alcohols by catalytic hydrogenation of CO in a fixed bed reactor. Two kinds of methods for preparation of Cu-Co-based catalyst has been dealt with in this paper, one was by co-precipitation way, the other was by impregnation way. The impact of different additive amounts of K, Ce and Zr on catalytic properties of Cu-Co/SiO2catalyst was discussed. The optimum reaction temperature, reaction pressure and amount of catalyst addition has been determined by conversion ratio of hydrogen and carbon monoxide, selectivity of methane, carbon dioxide and total alcohol, space-time yield of alcohol and distribution of alcohol. Deep research and analysis on catalytic properties has been carried out by the BET, XRD and TPR, in which the physical structure and surface phase has been affected by different catalyst additives, especially the specific surface area and the dispersion, and the reducibility of the catalyst have been significantly affected. The results showed that:the space time yield-and the selectivity of alcohol increased, and the selectivity of CH4was reduced The optimal reaction temperature of producing higher alcohols reaction was300℃; The suitable reaction pressure was5Mpa The optimal addition dosage of K2O, CeO2and ZrO2on catalytic properties of Cu-Co/SiO2catalyst was0.2%,0.2%and4%.
This paper conducted a study on synthesis of higher alcohols by catalytic hydrogenation of CO in a fixed bed reactor. Two kinds of methods for preparation of Cu-Co-based catalyst has been dealt with in this paper, one was by co-precipitation way, the other was by impregnation way. The impact of different additive amounts of K, Ce and Zr on catalytic properties of Cu-Co/SiO2catalyst was discussed. The optimum reaction temperature, reaction pressure and amount of catalyst addition has been determined by conversion ratio of hydrogen and carbon monoxide, selectivity of methane, carbon dioxide and total alcohol, space-time yield of alcohol and distribution of alcohol. Deep research and analysis on catalytic properties has been carried out by the BET, XRD and TPR, in which the physical structure and surface phase has been affected by different catalyst additives, especially the specific surface area and the dispersion, and the reducibility of the catalyst have been significantly affected. The results showed that:the space time yield-and the selectivity of alcohol increased, and the selectivity of CH4was reduced The optimal reaction temperature of producing higher alcohols reaction was300℃; The suitable reaction pressure was5Mpa The optimal addition dosage of K2O, CeO2and ZrO2on catalytic properties of Cu-Co/SiO2catalyst was0.2%,0.2%and4%.
引文
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