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A detailed study on the synergetic effect of TeMo5O16 and MoO3 phases in the MoTeOx catalysts for the partial oxidation of propylene to acrolein has been reported in this work. It was found that both propylene conversion and acrolein selectivity increased with the addition of MoO3 to TeMo5O16. Based on the results of N2 adsorption-desorption, XRD, XPS, in-situ XRD, O2-TPO, and 2-propanol decomposition reaction, the higher catalytic performance and synergetic effect could be attributed to the enhancement of acidity and the oxygen transfer from TeMo5O16 to MoO3 phase.