Ultra-Low-Temperature Ozone Abatement on α-MnO2(001) Facets with Down-Shifted Lowest Unoccupied Orbitals,Industrial & Engineering Chemistry Research

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Ultra-Low-Temperature Ozone Abatement on α-MnO2(001) Facets with Down-Shifted Lowest Unoccupied Orbitals
Industrial & Engineering Chemistry Research ( IF 3.8 ) Pub Date : 2018-09-04 , DOI: 10.1021/acs.iecr.8b03491
Yaxin Chen ₁ , Weiye Qu ₁ , Chao Li ₁ , Junxiao Chen ₁ , Zhen Ma _{1,

2} , Xingfu Tang _{1,

2}

Affiliation

Extraordinary 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.

中文翻译：

上的超低温臭氧消除α-MnO的₂（001）与下移最低未占小平面σ轨道

对于装备在商用客机上的臭氧转化器，在能量上极希望在超低温下具有非凡的催化性能，但要实现这一目标仍然是巨大的挑战。在这里，我们合成了片状α-MnO的₂暴露反应性的（001）面的大百分比，在其上的低化合价表面锰离子和丰富的表面氧空位作为催化位点。用α-MnO的相比_2个棒，α-MnO的₂片材，即使在-55℃下，由于丰富的催化位点表现出臭氧分解特殊催化活性。通过使用锰大号₃ _edge时吸收光谱和前沿轨道理论，我们发现，α-MnO的₂张纸下移最低未占据的Mn的3d轨道相对于β-MnO的₂，其更容易地使电子从过氧化物中间体转移到催化位点，从而加速即使在平流层中的非常低的温度下的反应速率。

更新日期：2018-09-05

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