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Insights into the Reactive and Deactivation Mechanisms of Manganese Oxides for Ozone Elimination: The Roles of Surface Oxygen Species

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journal contribution
posted on 25.01.2021, 14:42 by Lei Zhang, Sheng Wang, Lirong Lv, Ya Ding, Dongxu Tian, Shudong Wang
Manganese oxides with varied Mn valance states but identical morphologies were synthesized via a facile thermal treatment of γ-MnOOH. Also, their catalytic performance on ozone decomposition was investigated following the order of Mn3O4 < Mn2O3 < MnO2 < MnO2-H-200. In combination with X-ray diffraction (XRD), scanning electron microscopy (SEM), Brunauer–Emmett–Teller (BET), transmission electron microscopy (TEM), H2-temperature-programmed reduction (TPR), O2-temperature-programmed desorption (TPD), and X-ray photoelectron spectroscopy (XPS) characterization, it was deduced that the superior O3 decomposition capacity for MnO2-H-200 was strongly associated with abundant oxygen vacancies on its surface. Among Mn3O4, Mn2O3, and MnO2, the difference in O3 decomposition efficiency was dependent on the divergent nature of oxygen vacancy. Density functional theory (DFT) calculation revealed that Mn3O4 and MnO2 possessed lower formation energy of oxygen vacancy, while MnO2 had the minimum desorption energy of peroxide species (O2*). It was deduced that the promotion of the O3 decomposition capability was attributed to the easier O2* desorption. Insights into the deactivation mechanism for MnO2-H-200 further validated the assumptions. As the reaction proceeded, adsorbed oxygen species accumulated on the catalyst surface, and a portion of them were transformed to lattice oxygen. The consumption of oxygen vacancy led to the deactivation of the catalyst.