Defect-based Lewis pairs on hydrophobic MnO mesocrystals for robust and efficient ozone decomposition

基于缺陷的路易斯酸碱对在疏水性MnO介晶上实现高效稳定的臭氧分解

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Abstract

Catalytic ozone decomposition is a promising technique for eliminating ozone from the environment. However, developing redox-active catalysts that efficiently decompose ozone while maintaining robust performance under high humidity remains challenging. Herein, we develop a hydrophobic carbon-coated mesocrystalline MnO (Meso-MnO@C) featuring a high density of manganese vacancies (V(Mn))-based Lewis pairs (LPs) for catalytic ozone decomposition. The presence of V(Mn) induces the electronic restructuring in MnO, leading to the formation of V(Mn)-Mn acidic sites and adjacent lattice oxygen atoms as basic sites. These LPs act as electron donors and acceptors, facilitating rapid electron transfer and lowering the energy barrier for O(3) conversion to O(2). The hydrophobic carbon layer protects against water accumulation on Meso-MnO@C in humid conditions. As a result, the Meso-MnO@C achieves nearly 100% O(3) decomposition at a high weight hourly space velocity of 1500 L⋅g(-1) h(-1), with rapid reaction kinetics and stable performance for 100 hours under 65% relative humidity.

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