摘要
To clarify the key role of oxygen vacancy defects on enhancing the oxidative activity of the catalysts, metal–organic frameworks (MOFs) derived MnO X catalysts with different morphologies and oxygen vacancy defects were successfully prepared using a facile in-situ self-assembly strategy with different alkali moderators. The obtained morphologies included three-dimensional (3D) triangular cone stacked MnO X hollow sphere (MnO X -H) and 3D nanoparticle stacked MnO X nanosphere (MnO X -N). Compared to MnO X -N, MnO X -H exhibited higher activity for the oxidation of toluene (T 90 = 226 °C). This was mainly due to the large number of oxygen vacancy defects and Mn 4+ species in the MnO X -H catalyst. In addition, the hollow structure of MnO X -H not only facilitated toluene adsorption and activation of toluene and also provided more active sites for toluene oxidation. Reaction mechanism studies showed that the conversion of toluene to benzoate could be realized over MnO X -H catalyst during toluene adsorption at room temperature. In addition, abundant oxygen vacancy defects can accelerate the activated oxidation of toluene and the formation of oxidation products during toluene oxidation.
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