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Effect of support composition on the structural and catalytic properties of Ru/AlOOH–SiO2 catalysts for benzene selective hydrogenation†
Catalysis Science & Technology ( IF 4.4 ) Pub Date : 2018-02-01 00:00:00 , DOI: 10.1039/c8cy00059j
Gongbing Zhou 1, 2, 3, 4, 5 , Yanlu Dong 1, 2, 3, 4, 5 , Lan Jiang 1, 2, 3, 4, 5 , Daiping He 1, 2, 3, 4, 5 , Ya Yang 1, 2, 3, 4, 5 , Xin Zhou 1, 2, 3, 4, 5
Affiliation  

Benzene selective hydrogenation to cyclohexene, which has been attracting attention in terms of atomic economy, feedstock accessibility, and operational facilitation, has been investigated on Ru catalysts supported on AlOOH–SiO2 composites with varying Al/Si ratios aiming at unveiling the effect of support acidity. Various techniques such as Fourier transform infrared spectroscopy of adsorbed pyridine, transmission electron microscopy, and extended X-ray absorption fine structure spectroscopy were employed to comprehensively characterize the catalysts. It is confirmed that the amount of Lewis acid sites increased steadily with the increase in the Al/Si molar ratio. In benzene selective hydrogenation, the turnover frequency of benzene linearly correlated with the amount of acid sites, while the cyclohexene selectivity showed a volcano-type trend, achieving a maximum of 81%. Kinetic investigation revealed that the Lewis acid sites promoted the rate constants of both the benzene hydrogenation and cyclohexene hydrogenation steps to inequable extents. The resulting ratios of the rate constants evolved parallel to the variation in the cyclohexene selectivity, which elucidated the volcano-type relationship between the cyclohexene selectivity and the amount of Lewis acid sites.

中文翻译:

载体组成对Ru / AlOOH-SiO 2苯选择性加氢催化剂的结构和催化性能的影响

在AlOOH-SiO 2负载的Ru催化剂上,研究了苯选择性加氢成环己烯的问题,这在原子经济,原料可及性和操作便利性方面引起了人们的关注。Al / Si比不同的复合材料旨在揭示载体酸性的影响。各种技术,例如吸附吡啶的傅里叶变换红外光谱,透射电子显微镜和扩展的X射线吸收精细结构光谱被用来全面表征催化剂。证实了路易斯酸位点的数量随着Al / Si摩尔比的增加而稳定地增加。在苯的选择性加氢中,苯的周转频率与酸性部位的数量成线性关系,而环己烯的选择性则呈现出火山型的趋势,最高达到81%。动力学研究表明,路易斯酸位点在不等程度上促进了苯加氢和环己烯加氢步骤的速率常数。
更新日期:2018-02-01
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