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Outstanding Stability and Enhanced Catalytic Activity for Toluene Oxidation by Si–O–Mn Interaction over MnOx/SiO2
Industrial & Engineering Chemistry Research ( IF 4.2 ) Pub Date : 2022-01-10 , DOI: 10.1021/acs.iecr.1c02504
Baojiang Zhang 1 , Lilong Zhou 1 , Miao Qi 2 , Zhengjie Li 1 , Jilong Han 1 , Kunjie Li 1 , Yunsong Zhang 1 , Fariba Dehghani 3 , Runjing Liu 1 , Jimmy Yun 1, 4
Affiliation  

Emissions of volatile organic compounds (VOCs) have caused serious damage to the environment and public health. Catalytic combustion is an efficient technology for VOC elimination. In this study, porous silica supported amorphous MnOx was constructed. It presented excellent stability and high activity for toluene combustion, even under the high humidity (T90 = 218 °C). Compared with bulk amorphous MnOx, the catalytic activity has been improved by more than 11 times. The various characterizations and quantum chemical calculation results suggested that the Si–O–Mn hybridization induced weakening of the Mn–O bond strength and electron transfer from the catalyst to surface oxygen species. A promoting effect of the Si–O–Mn interaction on the spillover of active O species was proposed which enhanced the catalytic activity. In-situ DRIFTS and XPS analytical results determined the reaction mechanism and revealed that both Olatt and Osurf participate in the catalytic oxidation of toluene. The problem of the poor thermal stability of amorphous MnOx has been solved in this work. This work provides a convenient and effective method to prepare efficient catalysts with high activity and good thermal stability for VOC catalytic combustion.

中文翻译:

MnOx/SiO2 上 Si-O-Mn 相互作用对甲苯氧化的出色稳定性和增强的催化活性

挥发性有机化合物 (VOC) 的排放对环境和公众健康造成了严重破坏。催化燃烧是消除 VOC 的有效技术。在这项研究中,构建了多孔二氧化硅负载的无定形 MnO x即使在高湿度( T 90 = 218 °C)下,它对甲苯燃烧也表现出优异的稳定性和高活性。与块状非晶MnO x相比,催化活性提高了11倍以上。各种表征和量子化学计算结果表明,Si-O-Mn 杂化导致 Mn-O 键强度和电子从催化剂到表面氧物质的转移减弱。提出了 Si-O-Mn 相互作用对活性 O 物种溢出的促进作用,从而提高了催化活性。原位DRIFTS 和 XPS 分析结果确定了反应机理,并揭示了 O latt和 O surf都参与了甲苯的催化氧化非晶MnO x热稳定性差的问题在这项工作中得到了解决。该工作为制备VOC催化燃烧的高活性和良好热稳定性的高效催化剂提供了一种方便有效的方法。
更新日期:2022-01-19
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