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The gas phase methylation of biphenyl with MeOH over HZSM-5 and HZSM-5 modified with Si(OEt)4 was investigated at atm. pressure in the presence of water. The modification of the outer surface of the catalyst pellets by silicate gives increased selectivity to 4,4'-dimethylbiphenyl. Modified HZSM-5 gave 75% selectivity to 4-methylbiphenyl. [on SciFinder (R)]