Methylation of 4-methylbiphenyl with methanol over metal oxide-modified HZSM-5 zeolite catalysts

• A series of HZSM-5 zeolite catalysts modifed with metal oxides (MgO, CaO, SrO, BaO, ZnO, La2O3 and CeO2) were prepared by impregnation method and characterized by XRD, TPD and N-2-adsorption. Methylation of 4-methylbiphenyl (4-MBP) with methanol to 4,4'-dimethylbiphenyl (4,4'-DMBP) was carried out over the prepared catalysts under fixed-bed down-flow conditions. The results showed that the MgO-modified HZSM-5 can significantly improve the selectivity for target product 4,4'-DMBP (up to 80 % vs only 13 % over the parent HZSM-5). The effects of metal oxides on 4,4'-DMBP selectivity are arranged in the following order: MgO>SrOapproximate toZnOapproximate toCaOapproximate toLa(2)O(3)>BaO>CeO2. The effects of MgO contents, precursor-salt types, and loading methods were further investigated, and the results revealed that during 4-MBP conversion, proper MgO loading (5.6 %) can be more effective, and the ion-exchange methed is much better than the impregnation method. However, it is difficult to get higher metal oxide loading by using the ion-exchange method. The high selectivity over HZSM-5 modified with MgO largely results from the depression of 4,4-DMBP second reactions such as isomerization, dealkylation and alkylation, as demonstrated by the reaction of 4,4'-DMBP as reactant over MgO/ZSM-5 catalyst and HZSM-5 zeolite.

Nyckelord

4-methylbiphenyl

methanol

methylation

4,4 '-dimethylbiphenyl

HZSM-5 zeolite

metal oxide

modification

shape-selective catalysis

shape-selective alkylation

naphthalene

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