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在α-MnO催化剂上构建氧空位以改善甲苯催化氧化的简单策略。

Simple strategy for the construction of oxygen vacancies on α-MnO catalyst to improve toluene catalytic oxidation.

作者信息

Chen Lingzhu, Liu Yongjun, Fang Xue, Cheng Yan

机构信息

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.

出版信息

J Hazard Mater. 2021 May 5;409:125020. doi: 10.1016/j.jhazmat.2020.125020. Epub 2020 Dec 31.

Abstract

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.

摘要

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。

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