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Supported vanadium oxides are becoming the model catalysts for. numerous selective oxidation reactions. To exploit redox chemistry of well-known titania-supported vanadia is currently one of the most fascinating topics. Herein, by applying in situ electron energy-loss spectroscopy, we succeeded in stimulating a new redox reaction in a routine transmission electron microscope; the electron beam can boost further oxidation from an amorphous lower-oxidation-state vanadia to maximal V(2)O(5) with an expense of oxygen from its support of TiO(2) to be reduced. Our findings could be extended into a new strategy: through utilizing an electron beam, and probing the redox chemistry between catalysts and their support in a wide class of heterogeneous catalyst systems, such as various oxide/oxide, metal/oxide, and oxide/metal catalysts.