The synthesis of pyridine bases from acetaldehyde, formaldehyde and ammonia through aminocyclization continues to provide the best prospect for meeting growing demand. A proper selection of catalyst and standardization of process parameters are vital to achieve a market friendly product distribution and reactor operation. In this work, the major responsible factors for enhancing the activity and selectivity of HZS-5 catalysts have been identified and their individual and combined effects on aldehyde conversion, coke formation and selectivity to pyridine formation have been assessed. A priori assessment of catalyst time on stream behavior has been achieved by modeling the catalyst deactivation process.