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在酸蚀的MgMnO中构建氧空位以高效催化苯燃烧:气态氧和表面晶格氧的协同活化

Engineering oxygen vacancies in acid-etched MgMnO for efficiently catalytic benzene combustion: Synergistic activation of gaseous oxygen and surface lattice oxygen.

作者信息

Wu Yu, Lei Dongjing, Wang Aijie, Zhang Qiuyan, Jian Hongwei, Yang Haojie, Han Chong

机构信息

School of Metallurgy, Northeastern University, Shenyang 110819, China.

School of Metallurgy, Northeastern University, Shenyang 110819, China.

出版信息

J Hazard Mater. 2025 Mar 15;486:136907. doi: 10.1016/j.jhazmat.2024.136907. Epub 2024 Dec 18.

Abstract

The synergistic activation of gaseous oxygen and surface lattice oxygen is essential for designing highly efficient catalysts to eliminate VOCs. Herein, an effective acid treatment was carried out to create more oxygen vacancies by modulating the electronic structure of MgMnO spinels and MgMnO mixed oxides. The acid-treated MgMnO exhibited outstanding catalytic performance, with the reaction rate of benzene rising by 8.55 times at 200 °C. After acid treatment, MgMnO partially retained its spinel structure, while MnO in situ grew on the surface due to the selective removal of Mg. The transformation of Mn-O-Mg into Mn-O weakened the strength of adjacent Mn-O bonds, thereby promoting the release of surface lattice oxygen and the regeneration of oxygen vacancies. In addition, acid-treated MgMnO facilitated the adsorption and activation of gaseous oxygen. In situ DRIFTS analysis proved that the synergistic activation of gaseous oxygen and surface lattice oxygen accelerated the conversion of intermediates, thus contributing to the efficient degradation of benzene.

摘要

气态氧和表面晶格氧的协同活化对于设计用于消除挥发性有机化合物(VOCs)的高效催化剂至关重要。在此,通过调节MgMnO尖晶石和MgMnO混合氧化物的电子结构,进行了有效的酸处理以产生更多的氧空位。经酸处理的MgMnO表现出优异的催化性能,在200°C时苯的反应速率提高了8.55倍。酸处理后,MgMnO部分保留了其尖晶石结构,而MnO由于Mg的选择性去除而在表面原位生长。Mn-O-Mg向Mn-O的转变削弱了相邻Mn-O键的强度,从而促进了表面晶格氧的释放和氧空位的再生。此外,酸处理的MgMnO促进了气态氧的吸附和活化。原位漫反射红外傅里叶变换光谱(DRIFTS)分析证明,气态氧和表面晶格氧的协同活化加速了中间体的转化,从而有助于苯的有效降解。

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