【作者】 邸立辉；

【导师】 王亚权；

【作者基本信息】 天津大学 ， 化学工艺， 2004， 硕士

【摘要】 近年来,天然气部分氧化成为天然气转化制合成气领域研究的热点。目前研究最多的是负载型催化剂,但是都不适合于工业应用。本论文对纯金属镍整体型催化剂进行研究发现,此整体型催化剂有着很好的活性和稳定性,适合于工业应用。由粒度不同的纯金属镍小球制成两种规格整体型催化剂,分别在单管和套管反应器中进行甲烷催化部分氧化反应,考察了不同原料气配比n(CH4)/n(O2)、不同空速下产物的选择性、两种催化剂的活性和稳定性,考察了不同的反应器对反应结果的影响。实验结果表明,两种催化剂具有较好的催化活性、选择性和稳定性。在两种催化剂上,随着原料气n(CH4)/n(O2)比的增加,甲烷转化率降低,一氧化碳和氢气的选择性升高;随着空速增加,甲烷转化率、一氧化碳和氢气的选择性都升高。减小镍小球的粒径有利于增加催化剂的活性和选择性,反应温度低。催化剂的高径比对催化剂的活性影响很大。炉温的升高有利于提高催化剂的活性。镍整体型催化剂对原料气中的硫有很好的抵抗性能,中毒后的催化剂能迅速的恢复活性。在此催化剂上镀加5wt%的贵金属铑同纯镍催化剂相比,催化剂的活性变化不大。更多还原

【Abstract】 In the utilization of natural gas, research on the partial oxidation of natural gasinto syngas has been paid more and more attention. Recent experimental reportsconcentrated on the study of catalysts, especially supported catalysts, which are notsuitable for the industrial application as expected. In this work, pure metal nickelmonolithic catalysts were found suitable for industrial application due to their highactivity and good stability in the reaction.Partial oxidation of methane reaction, catalyzed by two kinds of monolithiccatalysts made of pure metal nickel spheres of different diameter, has been studied inboth a tubular and a double-tube reactor. Activity, selectivity and stability of the twokinds of catalysts have been observed at different feed ratios of CH4 to O2 anddifferent gas hourly space velocities. Also, the effect of different reactor configurationon the reaction has been studied in the experiment.It has been demonstrated that two kinds of catalysts have considerable activity,selectivity and stability. Over the two catalysts, with the increase of n(CH4)/n(O2)ratio CH4 conversion decreases, and CO and H2 selectivity increase. With the increaseof gas hourly space velocities, CH4 conversion, CO and H2 selectivity all increase。Reduction of diameter of nickel sphere can improve the activity and selectivityof catalyst.The activity of the catalyst is greatly influenced by the ratio of length anddiameter. Higher temperature of furnace increases the activity of the catalyst.The activity of the Nickel monolithic catalyst can be recovered rapidly afterpoisoning by sulfur.The activity of nickel monolithic catalyst coated with 5wt% Rh is not apparentlyhigher than pure nickel monolithic catalyst.更多还原