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低镍催化剂上CO和CO2加氢反应的对比研究
COMPARATIVE STUDY ON THE HYDROGENATION OF CO AND CO2 OVER LOW NICKEL LOADING Ni/Al2O3 CATALYST
【摘要】 采用CO和CO_2对比加氢活性测试,XRD及TPR方法研究了两个不同Na助剂含量的低镍Ni/Al_2O_3体系的性能。实验发现,在低镍催化剂上CO_2在较低温度下就可加氢生成甲烷,而CO则需要更高的温度,CO_2无需先经逆变换生成CO,然后再加氢,它可直接加氢生成CH_4。在同一催化剂上,CO_2加氢生成CH_4的表现活化能要低于CO加氢生成CH_4反应的表现活化能。晶相NiO还原后形成的活性相对CO_2加氢反应的活性明显高于它对CO的加氢活性,非晶相镍氧化物还原后形成的活性相对CO的加氢反应特别有利。Na助剂的含量不同会造成Ni氧化物物种的分配不同,从而导致CO、CO_2的加氢活性及其随温度的变化也不相同,催化剂对CO、CO_2加氢反应作用的本质是不相同的。
【Abstract】 Two low nickel loading Ni/Al2O3 catalysts containing different amount of Na promoter havebeen characterized by comparative CO and CO2 hydrogenation activity measurement, XRD and tem-perature-programmed reduction (TPR)techniques.It was found that CO2 could be converted toCH4 at lower temperature than that for CO.CO2 could be converted to CH4 directly without reverseshift reaction to form CO at first. when CO and CO2 coexisted in a reaction system,CO inhibitedthe hydrogenation of CO2 while CO2 did not have significant effect on CO.The nickel species formedafter the reduction of crystalline NiO exhibited favorite hydrogenation activity for CO2 which was higher than that for CO whithin the temperature range tested.While the nickel species formed afterthe reduction of noncrystalline nickel oxides which could be reduced at low temperature exhibitedhigh CO hydrogenation activity,and at above 540K thase species exhibited higher hydrogenation ac-tivity for CO than for CO2 .The aparent activation energy for CO@ hydrogenation was much lowerthan that for CO.The fact that Ni/Al2O3 catalyze both CO and CO2 hydrogenation to form CH4might be due to the inhomogeneity fo Ni/Al2O3.The active phase for CO hydrogenation and that for CO2,and the interaction of CO with the active phase and that of CO2 would be fifferent.
【Key words】 Low nickel loading catalyst.Comparative hydrogenation of CO and CO2 XRD; TPR;
- 【文献出处】 化学研究与应用 ,CHEMICAL RESEARCH AND APPLICATION , 编辑部邮箱 ,1994年03期
- 【分类号】O643.38
- 【被引频次】6
- 【下载频次】141