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and the p-/m-xylene selectivity (2.6% at 698 K) under N2 is ca. 1/11 as much as that with H2 (28.6% at 723 K), implying that the MTA process, as a minor pathway, only gives a small amount of p-/m-xylene in presence of H2. That is to say, the increased selectivity of p-/m-xylene as the increasing C/M ratio is mainly from the toluene methylation and deoxygenation of xylenols. As far as the MTA is concerned, toluene also plays an important role in remarkably enhancing the selectivity of the xylenes (ca. 8.4 times) as reported by Ilias and Bhan [42], which may also attribute to high selectivity of p-/m-xylene. Similarly, the alkane’s selectivity decreases from 26.8% (with H2 ) to 1.0% at 648 K (without H2), confirming that the MTH process indeed produces partial alkanes in the co-catalytic conversion of m-cresol in spite of further hydrogenation of toluene in the presence of H2. Table 1. Effect of carrier gas on the product distribution from converting m-cresol with methanol. Reaction Conditions m-Cresol conversion, % H2 N2 573K 623K 648K 673K 698K 723K 573K 623K 648K 673K 698K 723K 97.1 91.7 93.1 92.8 91.8 92.2 6.2 9.3 0.0 0.0 0.0 0.0 0.0 0.8 1.4 0.9 0.0 0.0 0.0 2.8 0.0 0.0 5.6 0.9 64.2 58.0 6.3 8.8 22.5 27.1 19.4 39.5 1.0 1.9 0.2 0.1 1.0 0.8 2.1 2.4 0.4 0.5 8.2 10.5 0.0 0.0 0.5 0.7 52.3 52.6 11.8 13.5 22.0 16.6 44.3 51.0 2.0 1.6 0.2 0.2 0.7 0.7 2.6 2.3 0.5 0.5 9.9 8.3 0.0 0.0 1.0 1.2 52.8 54.3 15.7 16.9 14.0 13.5 Selectivity, % Alkanes 85.4 44.8 26.8 18.1 9.6 7.1 Benzene Toluene p-/m-Xylene o-Xylene a PAB Phenol o-Cresol Xylenols b PAP c MA 0.0 0.6 1.2 2.1 4.0 5.2 8.5 21.7 27.9 29.8 32.4 32.1 2.1 17.0 24.2 27.3 28.0 28.6 1.0 5.1 1.0 7.5 0.0 0.1 0.2 0.1 0.9 1.9 0.1 0.2 0.8 0.7 7.2 8.3 9.0 9.2 0.1 0.1 0.3 0.4 1.9 2.5 0.4 0.8 0.7 0.8 8.5 8.9 8.6 9.2 0.3 0.3 0.8 0.7 3.9 3.5 1.7 1.8 0.5 0.5 a PAB is polyalkylated benzenes; b PAP is polyalkylated phenols; c MA is methylanisole; Reaction conditions: m-cresol/methanol molar ratio = 1/4, catalyst = 1.0 wt. % Pt/Z-57, W/F = 75 gcat ̈h/gm-cresol, reaction temperature = 573–723 K, carrier gas = H2 or N2, pressure = 2 MPa. On the other side, the xylenol’s selectivity under N2 (54.3% at 723 K) is around 15.5 times compared to that with H2 (3.5% at 723 K), indicating that the increased p-/m-xylene under H2 may be partially formed from the deoxygenation of xylenols [32]. Without H2, the polyalkylated phenols and methylanisole selectivities (16.9% at 723 K and 27.1% at 623 K) raise sharply compared with those with H2 (1.8% at 723 K and 0.7% at 623 K), illustrating that the reaction rate of xylenols methylation and cresol methylation is much faster in the absence of H2. In order to confirm the deoxygenation of xylenols to p-/m-xylene, the conversion of 2,4-xylenol was performed under H2. Table 2 reports the conversion of 2,4-xylenol and product distribution with the reaction temperature over Pt/Z-57 catalyst. In the investigated temperature range, the 2,4-xylenol conversion is above 97% and the 212PDF Image | Zeolite Catalysis
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