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Novel mechanistic view of catalytic ozonation of gaseous toluene by dual-site kinetic modelling
Hu, Maocong; Yao, Zhenhua; Hui, K. N.; Hui, K. S.
2017-01-15
Source PublicationCHEMICAL ENGINEERING JOURNAL
ISSN1385-8947
Volume308Pages:710-718
AbstractThe catalytic ozonation of VOCs is a promising approach for degradation of indoor VOCs, such as gaseous toluene. However, the mechanism and relevant kinetic steps involved in this reaction remain unclear. In this study, the catalytic ozonation of toluene over MnO2/graphene was investigated using the empirical power law model and classic Langmuir-Hinshelwood single-site (denoted as L-H5) mechanism. The apparent activation energy determined using the power law model was 29.3 +/- 2.5 kJ mol(-1). This finding indicated that the catalytic ozonation of toluene over MnO2/graphene was a heterogeneous reaction, and the Langmuir-Hinshelwood mechanism was applicable. However, the L-H5 mechanism did not fit the experimental data, suggesting that the reaction was non-single-site governed. A novel Langmuir-Hinshelwood dual-site (denoted as L-H-d) mechanism was then proposed to explain the experimental observations of the catalytic ozonation of toluene over MnO2/graphene through a steady-state kinetic study. This mechanism was based on the hypothesis that MnO2 was responsible for ozone decomposition and toluene adsorption on graphene; these two types of adsorption were coupled by an adjacent attack. Furthermore, XPS results confirmed the presence of a strong connection between MnO2 and graphene sites on the surface of MnO2/graphene. This connection allowed the adjacent attack and validated the dual-site mechanism. The L-Hd model was consistent with the predicted reaction rate of toluene removal with a correlation coefficient near unity (r(2) = 0.9165). Moreover, the physical criterion was in accordance with both enthalpy and entropy of toluene adsorption constraints. Fulfillment of mathematical and physical criteria indicated the catalytic ozonation of toluene over MnO2/graphene can be well described by the L-Hd mechanism. This study helps understand the catalytic ozonation of toluene over MnO2/graphene in a closely mechanistic view. (C) 2016 Elsevier B.V. All rights reserved.
KeywordMnO2/graphene Toluene degradation Catalytic ozonation Langmuir-Hinshelwood dual-site mechanism Kinetic modelling
DOI10.1016/j.cej.2016.09.086
URLView the original
Indexed BySCI
Language英语
WOS Research AreaEngineering
WOS SubjectEngineering, Environmental ; Engineering, Chemical
WOS IDWOS:000389088000070
PublisherELSEVIER SCIENCE SA
The Source to ArticleWOS
Fulltext Access
Citation statistics
Cited Times [WOS]:15   [WOS Record]     [Related Records in WOS]
Document TypeJournal article
CollectionUniversity of Macau
Recommended Citation
GB/T 7714
Hu, Maocong,Yao, Zhenhua,Hui, K. N.,et al. Novel mechanistic view of catalytic ozonation of gaseous toluene by dual-site kinetic modelling[J]. CHEMICAL ENGINEERING JOURNAL,2017,308:710-718.
APA Hu, Maocong,Yao, Zhenhua,Hui, K. N.,&Hui, K. S..(2017).Novel mechanistic view of catalytic ozonation of gaseous toluene by dual-site kinetic modelling.CHEMICAL ENGINEERING JOURNAL,308,710-718.
MLA Hu, Maocong,et al."Novel mechanistic view of catalytic ozonation of gaseous toluene by dual-site kinetic modelling".CHEMICAL ENGINEERING JOURNAL 308(2017):710-718.
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