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Zeolite Catalysis

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Zeolite Catalysis ( zeolite-catalysis )

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nature of the supporter and metal on the product distribution. Table 3 shows the conversion of m-cresol and product distribution at 698 K over seven kinds of catalysts. At 698 K, the abundant compounds are toluene and p-/m-xylene on the catalysts except 1.0 wt. % Pt/B-25. For the Pt/HZSM-5 catalysts with parent supporter loading same metal content, the toluene and p-/m-xylene selectivities are, respectively, in the range of 32.4% to 36.9% and 27.8% to 28.7%, and the conversion of m-cresol and product distribution does not exhibit a distinct relation to the SiO2/Al2O3 ratio (acid amount). Nevertheless, for Pt/Z-57 with lower Pt content, the conversion of m-cresol declines from 91.8% to 83.4%, the alkanes selectivity decreases (from 9.6% to 8.1%), and the total oxygenated compounds (phenol, o-cresol, xylenols, and polyalkylated phenols) selectivity increases (from 6.7% to 10.0%) with lower Pt loading. This is probably associated with the reducing hydrogenation capacity of the catalyst with low metal loading. The lower selectivities of benzene and toluene, and the higher selectivities of p-/m-xylene and polyalkylated benzenes, are also observed over 0.6 wt. % Pt/Z-57 compared to 1.0 wt. % Pt/Z-57. This could be explained that the deoxygenation activity of oxygenated compounds decreases because of the deactivation, and the aromatics’ methylation rate enhances over 0.6 wt. % Pt/Z-57. Over 10.0 wt. % Ni/Z-107, the decrease in the m-cresol conversion (from 93.7% over 1.0 wt. % Pt/Z-107 to 85.1%), and the selectivities of p-/m-xylene and polyalkylated benzenes (from 28.7% and 9.3% over 1.0 wt. % Pt/Z-107 to 22.7% and 6.2%) may be attributed to the coverage of the active sites by high metal loading, while the increase of the alkane’s selectivity (from 8.0% over 1.0 wt. % Pt/Z-107 to 11.4%) is possible relative to the high hydrogenation selectivity over Ni/Z-107. Otherwise, the total oxygenated compounds selectivity on 10.0 wt. % Ni/Z-107 is ca. two times as much as that on 1.0 wt. % Pt/Z-107, which may result from the catalyst deactivation. After introducing mesopores by desilication, the m-cresol conversion and the alkane’s selectivity increases from 91.8% and 9.6% to 96.7% and 10.4%, while the total oxygenated compounds selectivity is just 56.7% of that over 1.0 wt. % Pt/Z-57, demonstrating that the generation of mesopores and the improved Pt dispersion by desilication are conducive to the m-cresol transformation, aromatics’ hydrogenation, and deoxygenation of oxygenated compounds. It should be noted that the p-/m-xylene selectivity (34.3%) over Pt/Z-57D is the highest among the seven catalysts, and the benzene and toluene selectivities clearly reduce (from 4.0% and 32.4% over Pt/Z-57 to 1.3% and 23.3% over Pt/Z-57D). The reason for this may be correlated with the increase of the aromatics methylation rate in the generated mesopores thanks to appropriate aperture size and the decrease in the effective diffusion length by desilication [44]. For Pt/B-25, the m-cresol conversion (97.2%) is the largest among the seven catalysts. Meanwhile, the selectivities of larger molecules (such as polyalkylated benzenes, xylenols, and polyalkylated phenols) are also the maximal. This is related to the 12-membered ring channels’ convenience to further 216

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