Insights into the surface-defect dependence of molecular oxygen activation over birnessite-type MnO <inf>2</inf>

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Journal Article
Applied Catalysis B: Environmental, 2018, 233 pp. 184 - 193
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© 2018 Elsevier B.V. In establishing the kinetics, energetics and mechanisms of phenolic degradation reactivity, active reactive oxygen species (ROS) on catalysts surface could exert a vital part. This paper attempts to account for different ROS at the atomic level using octahedral layered birnessite-type MnO 2 as a platform with different crystal planes which could induce the Jahn-Teller effect and further realize deep mineralization of phenolic pollutants at low temperature. The catalytic degradation phenol rate of (100) MnO 2 is 3 times as much as that of (001) MnO 2 , and the activation energy of the catalytic reaction is reduced by 11 KJ/mol. The degradation content of (100) MnO 2 surpasses 30% than that of (001) MnO 2 . Both spin-trapping EPR and DFT results show superoxide ([rad]O 2− ) species could exist on (001) MnO 2 through one electron transfer, while the peroxide (O 22− ) species exist on (100) MnO 2 via two electrons transfer. All the results illustrate that birnessite MnO 2 possesses surface-dependent molecular oxygen activation properties.
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