Ammoxidation of methylpyrazine (MP) to cyanopyrazine (CP) was performed at 633-693 K over iron phosphate catalysts having a P/Fe ratio of 1.2, obtained by adopting different methods of catalyst preparation. The catalysts were characterized by XRD, FTIR, UV-DRS, laser-Raman spectroscopy, TPR, TEM, XPS, acidity by Potentiometric titration and TPD of NH3. XRD and Raman data suggested predominant formation of quartz phase of iron phosphate. The structure and texture of the catalysts varied with the nature of starting material as well as the preparation method. The catalytic activity depended on the extent of quartz phase formation. Precipitation in the basic medium improved quartz phase formation and enhanced the activity. However, the decreased acid strength caused reduction in nitrile selectivity. A judicious combination of the redox and acid strength properties is required for obtaining maximum yield of CP. (C) 2008 Published by Elsevier B.V.