Manganese oxides have emerged as promising catalysts for the low-temperature activation of molecular oxygen (O₂), crucial for the catalytic oxidation and removal of gaseous pollutants. However, the undesired Jahn–Teller (J-T) effects associated with the Mn^iv/Mnⁱⁱⁱ redox couple, particularly under SO₂ poisoning, led to the effectiveness of Mn oxides in applications. Herein, we construct a highly covalent Se^iv-O-Mnⁱⁱⁱ structure via the introduction of selenium into α-MnO₂. Such a structure features high-valence Se^iv anchored on the oxygen-terminated (110) plane of α-MnO₂, facilitates the generation of more active oxygen species, and maintains the continuous cycling of oxygen-linked Mn^iv/Mnⁱⁱⁱ. Such dynamics are pivotal for stabilizing manganese activation and mitigating the J-T effect. Through a combination of experimental investigations and theoretical calculations, we demonstrate that the Se^iv-O-Mnⁱⁱⁱ configuration, characterized by a high degree of Mn–O hybridization, significantly enhances CO oxidation, NH₃ oxidation, and elemental mercury (Hg⁰) removal performances, and exhibits resistance to SO₂. This study paves the way for the development of efficient low-temperature O₂ activation processes for the removal of gaseous pollutants in real-world applications.

中文翻译：

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揭示了 Jahn-Teller 降低 Se 锚定 Mn 氧化物的复杂性，在气态分子氧活化中实现卓越的 SO2 抵抗力


锰氧化物已成为一种很有前途的分子氧 （O₂） 低温活化催化剂，对于催化氧化和去除气态污染物至关重要。然而，与 Mn^iv/Mnⁱⁱⁱ 氧化还原对相关的不良 Jahn-Telr （J-T） 效应，特别是在 SO₂ 中毒下，导致 Mn 氧化物在应用中的有效性。在此，我们通过将硒引入 α-MnO₂ 中构建了高度共价的 Se iv-O-Mnⁱⁱⁱ 结构。这种结构的特点是高价 Se^iv 锚定在 α-MnO₂ 的氧终止 （110） 平面上，促进更多活性氧的产生，并维持氧连接的 Mn^iv/Mnⁱⁱⁱ 的连续循环。这种动力学对于稳定锰活化和减轻 J-T 效应至关重要。通过实验研究和理论计算的结合，我们证明了以高度 Mn-O 杂化为特征的 Se iv-O-Mnⁱⁱⁱ 构型显着增强了 CO 氧化、NH₃ 氧化和元素汞 （Hg⁰） 去除性能，并表现出对 SO₂ 的抵抗力。这项研究为开发高效的低温 O₂ 活化工艺铺平了道路，以便在实际应用中去除气态污染物。