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alkanes (including dimethycyclohexane, methylcyclohexane, and pentane) selectivity sharply drops from 95.3% at 573 K to 5.7% at 723 K. With the increasing temperature from 573 K to 723 K, the benzene, toluene, p-/m-xylene, o-xylene, and polyalkylated benzene’s selectivities increase from 0.0%, 0.7%, 2.0%, 0.5%, and 0.2% to 2.7%, 22.5%, 40.0%, 12.2%, and 13.6%, respectively. The total selectivity of the oxygenated product is less than 5.0%. Obviously, it can be concluded that the deoxygenation of 2,4-xylenol could effectively generate p-/m-xylene under the experimental conditions. Temperature, K 2,4-Xylenol Conversion, % Selectivity, % p-/m-Xylene o-Xylene 2.0 0.5 3.2 0.9 8.4 2.2 29.8 8.6 13.1 39.2 11.8 13.6 22.5 40.0 12.2 13.6 Table 2. Product selectivity and conversion for 2,4-xylenol hydrodeoxygenation. Alkanes Benzene 95.3 0.0 93.0 0.0 84.7 0.2 42.3 0.5 16.4 1.1 5.7 2.7 Toluene a PAB Cresol Xylenols 0.7 0.5 0.9 0.5 0.8 0.3 0.7 3.1 0.7 3.3 0.5 1.7 b PAP 0.0 0.0 0.0 0.2 0.7 0.8 573 99.4 623 99.7 648 99.8 673 97.3 698 97.4 723 99.0 0.7 0.5 1.7 5.9 0.2 0.9 1.6 9.1 a PAB is polyalkylated benzenes; b PAP is polyalkylated phenols; Reaction conditions: catalyst = 1.0 wt. % Pt/Z-57, W/F = 75 gcat ̈ h/gm -cresol , reaction temperature = 573 K–723 K, carrier gas = H2, pressure = 2 MPa. To sum up, the MTA and MTH of methanol occur in the co-catalytic conversion m-cresol with methanol, but only a small part of p-/m-xylene is produced from the MTA process. Nevertheless, the methylation of toluene and deoxygenation of xylenols are indeed the important pathways of p-/m-xylene formation. 2.2.4. Catalyst Stability An experiment of co-conversion of m-cresol with methanol (C/M ratio of 1/4) as a function of time on stream was carried out to test the catalyst stability. The variation of the m-cresol conversion and product selectivities over Pt/Z-57 at 673 K are plotted in Figure 4. The catalyst shows deactivation during ca. 8 h of on-stream reaction on account of the decrease in the conversion from 91.8% to 76.6%. The main products are always p-/m-xylene and toluene, and their selectivities decrease from 28.0% and 32.4% to 21.0% and 18.5%. Nevertheless, the selectivities of xylenols, o-cresol, and polyalkylated phenols increase from 3.9%, 0.8%, and 1.7% to 16.5%, 7.8%, and 6.6%. Thus, it can be seen that the deactivation is attributed to the formation of oxygenated compounds which may lead to the formation of coke on catalysts. The variation of the alkanes, o-xylene, and polyalkylated benzene’s selectivities is insignificant. Benzene, phenol, methylanisole, and other products are in minor amounts and their selectivities change slightly with increasing the time on stream. 213PDF Image | Zeolite Catalysis
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