Characterization of Pd catalysts supported on USY zeolites with different SiO2/Al2O3 ratios for the hydrogenation of naphthalene in the presence of benzothiophene

Jian Zheng; Ming Guo; Chunshan Song

doi:10.1016/j.fuproc.2007.11.025

Characterization of Pd catalysts supported on USY zeolites with different SiO₂/Al₂O₃ ratios for the hydrogenation of naphthalene in the presence of benzothiophene

Jian Zheng, Ming Guo, Chunshan Song

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Abstract

A series of ultra-stable Y-type (USY) zeolites with different SiO₂/Al₂O₃ ratios in the range of 10-80 were used as supports for preparing Pd/USY at 2 wt% Pd loading. The FT-IR of hydroxyl groups of USY zeolites, the n-butylamine chemisorption and the temperature-programmed desorption were used in combination to characterize the zeolite acidity. TPR, H₂-TPD and chemisorption using H₂ were used to characterize the Pd reduction and dispersion. The hydrogenation of naphthalene was conducted at 200 °C in the presence of benzothiophene at different sulfur/metal ratios. The hydrogenation activity, selectivity, and the sulfur tolerance strongly depended on the SiO₂/Al₂O₃ ratio (thus the acidity) of the zeolites. The activity decreased with increasing SiO₂/Al₂O₃ in this range. The IR and n-butylamine TPD showed that both the amount and strength of Brönsted acidity decreased with the increase of the SiO₂/Al₂O₃ ratio. The good relationship between the acidity modification and catalytic performance suggests that the sulfur tolerance of Pd/USY zeolite might be due to the desired metal-support interaction, which resulted in larger amount of electron-deficient Pd. However, as shown in TGA and TPO-IR studies, the higher hydrogenation performance on more acidic zeolite also caused higher amount of carbonaceous species on the catalyst.

Original language	English (US)
Pages (from-to)	467-474
Number of pages	8
Journal	Fuel processing technology
Volume	89
Issue number	4
DOIs	https://doi.org/10.1016/j.fuproc.2007.11.025
State	Published - Apr 2008

All Science Journal Classification (ASJC) codes

General Chemical Engineering
Fuel Technology
Energy Engineering and Power Technology

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10.1016/j.fuproc.2007.11.025

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title = "Characterization of Pd catalysts supported on USY zeolites with different SiO2/Al2O3 ratios for the hydrogenation of naphthalene in the presence of benzothiophene",

abstract = "A series of ultra-stable Y-type (USY) zeolites with different SiO2/Al2O3 ratios in the range of 10-80 were used as supports for preparing Pd/USY at 2 wt\% Pd loading. The FT-IR of hydroxyl groups of USY zeolites, the n-butylamine chemisorption and the temperature-programmed desorption were used in combination to characterize the zeolite acidity. TPR, H2-TPD and chemisorption using H2 were used to characterize the Pd reduction and dispersion. The hydrogenation of naphthalene was conducted at 200 °C in the presence of benzothiophene at different sulfur/metal ratios. The hydrogenation activity, selectivity, and the sulfur tolerance strongly depended on the SiO2/Al2O3 ratio (thus the acidity) of the zeolites. The activity decreased with increasing SiO2/Al2O3 in this range. The IR and n-butylamine TPD showed that both the amount and strength of Br{\"o}nsted acidity decreased with the increase of the SiO2/Al2O3 ratio. The good relationship between the acidity modification and catalytic performance suggests that the sulfur tolerance of Pd/USY zeolite might be due to the desired metal-support interaction, which resulted in larger amount of electron-deficient Pd. However, as shown in TGA and TPO-IR studies, the higher hydrogenation performance on more acidic zeolite also caused higher amount of carbonaceous species on the catalyst.",

author = "Jian Zheng and Ming Guo and Chunshan Song",

year = "2008",

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doi = "10.1016/j.fuproc.2007.11.025",

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PY - 2008/4

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AB - A series of ultra-stable Y-type (USY) zeolites with different SiO2/Al2O3 ratios in the range of 10-80 were used as supports for preparing Pd/USY at 2 wt% Pd loading. The FT-IR of hydroxyl groups of USY zeolites, the n-butylamine chemisorption and the temperature-programmed desorption were used in combination to characterize the zeolite acidity. TPR, H2-TPD and chemisorption using H2 were used to characterize the Pd reduction and dispersion. The hydrogenation of naphthalene was conducted at 200 °C in the presence of benzothiophene at different sulfur/metal ratios. The hydrogenation activity, selectivity, and the sulfur tolerance strongly depended on the SiO2/Al2O3 ratio (thus the acidity) of the zeolites. The activity decreased with increasing SiO2/Al2O3 in this range. The IR and n-butylamine TPD showed that both the amount and strength of Brönsted acidity decreased with the increase of the SiO2/Al2O3 ratio. The good relationship between the acidity modification and catalytic performance suggests that the sulfur tolerance of Pd/USY zeolite might be due to the desired metal-support interaction, which resulted in larger amount of electron-deficient Pd. However, as shown in TGA and TPO-IR studies, the higher hydrogenation performance on more acidic zeolite also caused higher amount of carbonaceous species on the catalyst.

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Characterization of Pd catalysts supported on USY zeolites with different SiO₂/Al₂O₃ ratios for the hydrogenation of naphthalene in the presence of benzothiophene

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