第八族金属/ al2o3催化剂的活性、选择性和热稳定性研究

M. Saito, T. Sakabe
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引用次数: 0

摘要

在300°C和1atm条件下,采用脉冲法和循环流动反应器,研究了CO和H2混合物合成烃类时,在300°C ~ 800°C条件下,预处理温度对VIII族金属(除oium外)/Al2O3催化剂活性和选择性的影响。此外,还利用化学吸附技术测定了不同处理温度下催化剂表面金属原子数的变化。催化剂单位重量的活度;Pt、Ir、Pd和Rh催化剂的mS值在500℃处理时达到最大值,但由于金属烧结的原因,随着处理温度的升高,它们的mS值单调降低。随着处理温度的升高,Ru(A)催化剂的活性和mS值略有下降。Ru(B)的初始活性和mS值随处理温度的升高而升高,但稳态活性降低。Ni和Co的活度和mS值随处理温度的升高而升高。铁既不吸附氢,也没有表现出任何活性。比活度(每表面金属原子)的顺序为Ru(B)、Ru(A)>Ni>Co>Rh>Pd、Pt> ir,主要反应产物为甲烷,但产物的碳氢化合物分布在很大范围内的变化主要取决于金属而不是处理温度。产物烃平均分子量的变化顺序为Ru(B)>Ir>Rh>Ru(A), Ni、Co>Pt>Pd。
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The Activity, Selectivity and Thermal Stability of Group VIII Metal/Al2O3Catalysts for Synthesis of Hydrocarbons from CO and H2
For hydrocarbon synthesis from mixtures of CO and H2, variation in activity and selectivity of Group VIII metals (except osmium)/Al2O3 catalysts with pretreatment temperature in flpwing H2 at 300°C∼800°C, was investigated at 300°C and 1atm using a pulse method and a circulating flow reactor. In addition, variation in the number of surface metal atoms (mS) in those catalysts with varying treatment temperature was also determined using the chemisorption technique. The activities (per unit weight of catalyst; per metal atom in the catalyst) of Pt, Ir, Pd, and Rh catalysts were maximum when they were treated at 500°C, though their mS values monotonously decreased with increasing treatment temperature due to metal sintering. The activity and the mS value of Ru(A) catalyst decreased slightly with increasing treatment temperature. On the other hand, the initial activity and the mS value of Ru(B) increased with increasing treatment temperature, but the steady-state activity decreased. The activities and mS values of Ni and Co increased with increasing treatment temperature. Fe neither adsorbed hydrogen nor showed any activity. The sequence of specific activity (per surface metal atom) was determined as follows: Ru(B), Ru(A)>Ni>Co>Rh>Pd, Pt>IrThe main reaction product was methane, but the hydrocarbon distribution of products varied over a wide range depending more on metal than on treatment temperature. The average molecular weight of product hydrocarbons changed in the following sequence: Ru(B)>Ir>Rh>Ru(A), Ni, Co>Pt>Pd.
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