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and ca. 2.0 times as high as that without methanol. The remarkable improvement in the p-/m-xylene selectivity may be a result of enhanced methylation reaction rate, as well as the other reactions brought by the methanol, such as methanol to aromatics (MTA) process. Of course, an enhanced methylation reaction rate should be taken as one of the most important pathways as discussed below. 100 80 60 40 20 0 Figure 3. Effect of the m-cresol/methanol molar ratio on the product distribution. Figure 3. Effect of the m-cresol/methanol molar ratio on the product distribution. a: m-cresol a: m-cresol conversion, b: alkanes, c: benzene, d: toluene, e: p-/m-xylene, conversion, b: alkanes, c: benzene, d: toluene, e: p-/m-xylene, f: o-xylene, g: polyalkylated f: o-xylene, g: polyalkylated aromatics, h: others, i: phenol, j: o-cresol; k: xylenols, aromatics, h: others, i: phenol, j: o-cresol; k: xylenols, l: polyalkylated phenols. l: polyalkylated phenols. (Reaction conditions: T = 698 K, p = 2 MPa, W/F = 75 (Reaction conditions: T = 698 K, p = 2 MPa, W/F = 75 gcat·h/molcresol, H2/ reagent = 5, gcat ̈ h/molcresol, H2/ reagent = 5, catalyst = 1.0 wt. % Pt/Z-57). catalyst = 1.0 wt. % Pt/Z-57). At 698AKt,6th9e8pKh,enthoel spelheecntioviltyseilsescmtiavlilt(yleissstmhaanll1%(le)sisntheanin1v%est)iginattehdeCi/nMverastiogaratnegdeC. W/Mith the increrasteiofrathnegme.etWhaintohl tahmeouinctrineathseroefactthaentm, theethoa-cnroesloalmanoduxnytleinotlshfeirrsetlaycitnacnret,astehefrom-cr1e.2so%l and 2.0%an(tdhexyCl/eMnorlastifiorosftl1y/1in)ctore5a.s4e%fraonmd 61..12%(athnedC2/.M0%ra(ttihoeoCf 1//M2),rantdiothoefn1/de1c)retoas5e.4to%0a.8n%dand 3.9%6.(1t%he(Cth/Me Cra/tMio orfat1i/o4)o,fa1n/d2l)a,stalnydintchreansedetocr1e.a8%se atond0.68.%4%an(tdhe3C.9/%M (rtahtieoCof/M1/8r),atiniodiocafting that1/th4e)r,eanisdlasctloymipnlcerxeaisnetetroac1t.i8o%n abnetdw6e.e4n%t(htehemCe/thManroaltiaonodf1o/-c8r)e,sionldaicnadtinxgyltehnaotlsthneereding furthiesraincvoemstipgaletixoni.nteraction between the methanol and o-cresol and xylenols needing further investigation. Therefore, increasing the methanol/m-cresol molar ratio would further improve the selectivity of p-/m-xylene, but also introduce additional reactions, such as the conversion of methanol to hydrocarbons or aromatics [40]. Obviously, those reactions, to a certain degree, contribute to the considerable improvement of p-/m-xylene selectivity, which needs further investigation and clarification. 2.2.3. Co-Catalytic Conversion under N2 and the Intermediate Conversion To identify the other reactions (MTA, MTH, etc.) of methanol other than methylation, co-catalytic conversion of m-cresol with methanol at the C/M ratio of 1/4 was carried out under N2. Under these conditions, HDO reactions of m-cresol and xylenols to form toluene and xylenes do not take place [41]. Thus, the observed alkanes, and aromatics (benzene, toluene, p-/m-xylene, o-xylene, and polyalkylated benzenes) under N2 (see Table 1), may be products from MTA and MTH processes. It should be noted in the temperature range of 573 K to 723 K, the m-cresol conversion under N2 is less than 51%, while the m-cresol conversion under H2 is more than 91%, a b c d e f g h i j k l 1:1 1:2 1:4 1:8 m-Cresol/methanol molar ratio 211 Selectivity (%)PDF Image | Zeolite Catalysis
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