Chen Lingzhu, Liu Yongjun, Fang Xue, Cheng Yan
School of Architecture and Environment, Sichuan University, Chengdu 610065, China.
School of Architecture and Environment, Sichuan University, Chengdu 610065, China; National Engineering Research Center for Flue Gas Desulfurization, Chengdu 610065, China.
J Hazard Mater. 2021 May 5;409:125020. doi: 10.1016/j.jhazmat.2020.125020. Epub 2020 Dec 31.
A strategy simple, safe and suitable for large scale production of α-MnO catalyst with high activity in VOCs oxidation is crucial for its application. The catalytic reactivity of α-MnO catalyst is largely related with its oxygen vacancy. Herein, we report effective construction of oxygen vacancies on α-MnO through simply adjusting precipitation temperature of a redox precipitation process. The key role of surface oxygen vacancies in toluene oxidation and the formation of different amount and distribution of the oxygen vacancies over the α-MnO catalysts were revealed by characterizations together with DFT calculations. The best catalyst (α-MnO-60) exhibited significantly improved catalytic activity of α-MnO catalyst in toluene oxidation (T = 203 ℃) and excellent water resistance. The richest surface oxygen vacancies of α-MnO-60 contributed to its best catalytic activity, despite of its relatively lower specific surface area. This work may provide a new perspective for the rational design of high efficient VOCs catalysts.
一种简单、安全且适用于大规模生产在挥发性有机化合物(VOCs)氧化中具有高活性的α-MnO催化剂的策略对其应用至关重要。α-MnO催化剂的催化活性在很大程度上与其氧空位有关。在此,我们报道了通过简单调节氧化还原沉淀过程的沉淀温度在α-MnO上有效构建氧空位。通过表征和密度泛函理论(DFT)计算揭示了表面氧空位在甲苯氧化中的关键作用以及在α-MnO催化剂上形成的不同数量和分布的氧空位。最佳催化剂(α-MnO-60)在甲苯氧化中(T = 203℃)表现出α-MnO催化剂显著提高的催化活性和优异的耐水性。尽管α-MnO-60的比表面积相对较低,但其最丰富的表面氧空位促成了其最佳催化活性。这项工作可能为高效VOCs催化剂的合理设计提供新的视角。