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In this work, series of catalysts like bimetallic oxides and supported ZSM-5 (acid and/or metal), were applied for the synthesis of pyridine and 3-picoline from acrolein diethyl acetal, water and ammonia in a fixed-bed reactor. The results showed that bimetallic oxides and alkaline catalysts exhibited extremely low catalytic activities whereas HZSM-5 had significantly better than MCM-41 and SBA-15. Among kinds of catalysts, the total yield of pyridine and 3-picoline over Mg-ZSM-5 through ion-exchanged process reached the highest. [ABSTRACT FROM AUTHOR]