ie8b03491_si_001.pdf (2.09 MB)
Ultra-Low-Temperature Ozone Abatement on α‑MnO2(001) Facets with Down-Shifted Lowest Unoccupied Orbitals
journal contribution
posted on 2018-08-20, 00:00 authored by Yaxin Chen, Weiye Qu, Chao Li, Junxiao Chen, Zhen Ma, Xingfu TangExtraordinary catalytic performance
at ultralow temperatures is
energetically desirable for ozone converters equipped on commercial
passenger aircrafts, but it remains a great challenge to achieve it.
Here we synthesized sheet-shaped α-MnO2 exposing
a large percentage of reactive (001) facets, on which low-valence
surface manganese ions and abundant surface oxygen vacancies act as
catalytic sites. Compared with α-MnO2 rods, α-MnO2 sheets exhibited exceptional catalytic activity in ozone
decomposition even at −55 °C due to the abundant catalytic
sites. By using Mn L3-edge absorption spectroscopy and
the frontier orbital theory, we found that α-MnO2 sheets have down-shifted lowest unoccupied Mn 3d orbitals with respect
to β-MnO2, which enables electrons to transfer from
peroxide intermediates to catalytic sites more easily, thus accelerating
the reaction rate even at very low temperatures in the stratosphere.
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β- MnO 2α- MnO 2 sheetssiteα- MnO 2 rodsozone decompositionozone converterspassenger aircraftssurface oxygen vacancies actlow-valence surface manganese ionsedge absorption spectroscopyMn 3peroxide intermediatesDown-Shifted LowestMn L 3sheet-shaped α- MnO 2ultralow temperaturesreaction rateUltra-Low-Temperature Ozone Abatement
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