4-Methylquinoline and 2-methylquinoline were synthesized from acetaldehyde and aniline in the gas phase over BEA* zeolite catalysts. High combined yields of 2- and 4-methyl-substituted quinolines were obtained with H-BEA* zeolite and with BEA*-F synthesized in fluoride medium, with 4-methylquinoline being the predominant isomer. Postsynthesis fluorination of the H-BEA* with ammonium fluoride leads to dealumination and formation of extra-framework aluminium fluoride compounds. Product selectivities changed with time over this catalyst, Such that 2-methylquinoline became the predominant product. New insight into the reaction mechanism is offered, and previous propositions can be rationalized based on these new results. (c) 2006 Elsevier Inc. All rights reserved.