Engineering oxygen vacancies in acid-etched MgMn2O4 for efficiently catalytic benzene combustion: Synergistic activation of gaseous oxygen and surface lattice oxygen

IF 12.2 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Journal of Hazardous Materials Pub Date : 2024-12-18 DOI:10.1016/j.jhazmat.2024.136907
Yu Wu, Dongjing Lei, Aijie Wang, Qiuyan Zhang, Hongwei Jian, Haojie Yang, Chong Han
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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 MgMn2O4 spinels and MgMnOx mixed oxides. The acid-treated MgMn2O4 exhibited outstanding catalytic performance, with the reaction rate of benzene rising by 8.55 times at 200 °C. After acid treatment, MgMn2O4 partially retained its spinel structure, while Mn2O3 in situ grew on the surface due to the selective removal of Mg2+. 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 MgMn2O4 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.

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气态氧和表面晶格氧的协同活化对于设计消除挥发性有机化合物的高效催化剂至关重要。在此,通过调节 MgMn2O4 尖晶石和 MgMnOx 混合氧化物的电子结构,对其进行了有效的酸处理,以产生更多的氧空位。酸处理后的 MgMn2O4 表现出了优异的催化性能,在 200 °C 时苯的反应速率提高了 8.55 倍。酸处理后,MgMn2O4 部分保留了尖晶石结构,而由于 Mg2+ 的选择性去除,Mn2O3 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,经酸处理的 MgMn2O4 还能促进气态氧的吸附和活化。原位 DRIFTS 分析证明,气态氧和表面晶格氧的协同活化加速了中间产物的转化,从而促进了苯的高效降解。
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来源期刊
Journal of Hazardous Materials
Journal of Hazardous Materials 工程技术-工程:环境
CiteScore
25.40
自引率
5.90%
发文量
3059
审稿时长
58 days
期刊介绍: The Journal of Hazardous Materials serves as a global platform for promoting cutting-edge research in the field of Environmental Science and Engineering. Our publication features a wide range of articles, including full-length research papers, review articles, and perspectives, with the aim of enhancing our understanding of the dangers and risks associated with various materials concerning public health and the environment. It is important to note that the term "environmental contaminants" refers specifically to substances that pose hazardous effects through contamination, while excluding those that do not have such impacts on the environment or human health. Moreover, we emphasize the distinction between wastes and hazardous materials in order to provide further clarity on the scope of the journal. We have a keen interest in exploring specific compounds and microbial agents that have adverse effects on the environment.
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