Steam Reforming of Hydrocarbons on Noble Metal Catalysts (Part 2)

E. Kikuchi, Y. Yamazaki, Y. Morita
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引用次数: 6

Abstract

Steam-reforming of n-heptane on rhodium catalysts was investigated under atmospheric pressure and in the temperature range from 550 to 800°C. The degree of dispersion of supported rhodium was determined from hydrogen chemisorption data measured at 25°C by a pulse technique.Rhodium supported on silica was found to sinter considerably on reduction in hydrogen flow, and its activity also decreased. On the other hand, γ-alumina support was found to keep the dispersion of rhodium unchanged on reduction in the temperature range from 550 to 800°C.The activity per weight of a catalyst increased with the concentration of rhodium supported on γ-alumina. The activity was correlated with the amount of hydrogen uptake when more than 0.2% of rhodium was supported.The product composition from reactions at 600°C was compared with the equilibrium composition determined by the following two reactions: i) CH4+H2O=CO+3H2, and ii) CO+H2O=CO2+H2. The composition was found to deviate considerably from the equilibrium at earlier stages of the reaction, but to approach it with increasing conversion of n-heptane. It was suggested that the rate of these equilibrating reactions, especially of the reaction ii), was smaller than that of the initial decomposition of the feed hydrocarbon.
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贵金属催化剂上烃类蒸汽重整(二)
在常压条件下,在550 ~ 800℃的温度范围内,研究了铑催化剂上正庚烷的蒸汽重整。负载铑的分散程度是通过脉冲技术在25°C下测量的氢化学吸附数据来确定的。结果表明,硅载铑在氢流减少时发生明显的烧结,其活性也随之下降。另一方面,在550 ~ 800℃的还原温度范围内,γ-氧化铝载体使铑的分散保持不变。催化剂的单位重量活性随负载在γ-氧化铝上的铑浓度的增加而增加。当铑含量大于0.2%时,活性与吸氢量呈正相关。将600℃下反应的产物组成与以下两个反应确定的平衡组成进行了比较:i) CH4+H2O=CO+3H2, ii) CO+H2O=CO2+H2。结果表明,在反应的早期阶段,其组成与平衡有很大的偏离,但随着正庚烷转化率的增加,其组成逐渐接近平衡。结果表明,这些平衡反应,特别是反应ii)的速率小于原料烃的初始分解速率。
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