Comparative study of Mn oxides catalysts on toluene oxidation: the effect of Mn valence electronic structures
发布时间：2024-11-29
点击次数：
- 影响因子：
- 7.7
- DOI码：
- 10.1016/j.jece.2024.112780
- 所属单位：
- 环境与资源学院
- 教研室：
- 化学工程系
- 发表刊物：
- Journal of Environmental Chemical Engineering
- 项目来源：
- 重庆市科技局
- 关键字：
- Mn-based oxides；d-band center；Orbital interaction；Toluene oxidation；O2 activation
- 摘要：
- Understanding the structure-activity relationship of Mn-based oxide catalysts is of great importance for the rational development of highly performance catalysts for VOCs catalytic oxidation. However, the knowledge of the electronic structure-catalytic oxidation activity relationship over Mn-based oxide catalysts is still limited. Herein, we investigated the typical MnxOy (Mn3O4, MnO2, and Mn2O3) with different valence electronic structures by using various characterizations and DFT calculations. The MnO2 exhibits superior intrinsic activities (RS, 1.14×10−9 mol·m−2·s−1) when compared with Mn3O4 (0.54×10−9 mol·m−2·s−1) and Mn2O3 (0.45×10−9 mol·m−2·s−1) for toluene catalytic oxidation. The solid experimental and DFT calculation results show that the d-band center of Mn determines the intrinsic activity. The superior catalytic oxidation activity of MnO2 can be attributed to its higher d-band center (-1.03 eV) in comparison with that of Mn3O4 (-1.25 eV) and Mn2O3 (-1.59 eV). The higher d-band center can weaken the surface Mn-O bonds strength (k = 290.9 N/m) and strengthen the gaseous O2 adsorption simultaneously, then enhancing the mobility of surface lattice oxygen and the amount of adsorbed oxygen species. This work firstly reveals the intrinsic relationship between catalytic oxidation activity and d electronic structure over Mn-based oxide catalysts and provides knowledge that will advance the design of high-performance catalysts for catalytic oxidation.
- 第一作者：
- Jia Zeng
- 合写作者：
- Sijia Song,Shuang Chen,Guizhi Zhang,Hongmei Xie
- 论文类型：
- 源刊论文
- 通讯作者：
- Guilin Zhou
- 学科门类：
- 工学
- 文献类型：
- Journal Article
- 卷号：
- 12
- 期号：
- 3
- 页面范围：
- 112780
- 是否译文：
- 否
- 发表时间：
- 2024-06-03
- 收录刊物：
- SCI