Structural effect and reaction mechanism of MnO2 catalysts in the catalytic oxidation of chlorinated aromatics

doi:10.1016/S1872-2067(19)63322-X

Abstract

Abstract:

Various MnO₂ structures have been extensively applied in catalysis. In this study, γ-MnO₂, α-MnO_2, and δ-MnO₂ with corresponding rod, tube, and hierarchical architecture morphologies were prepared and applied for the catalytic oxidation of chlorobenzene (CB). The redox ability, H₂O activation behavior, and acidity of MnO₂ were analyzed using a range of techniques, including TPR, H₂O-TPD, XPS, and pyridine-IR. The catalytic activities in CB oxidation were assessed; this revealed that γ-MnO₂ exhibited the highest activity and best stability, owing to its enriched surface oxygen vacancies that functioned to activate O₂ and H₂O, and capture labile chlorine, which reacted with dissociated H₂O to form HCl. All the MnO₂ phases generated toxic polychlorinated by-products, including CHCl₃, CCl₄, C₂HCl₃, and C₂Cl₄, indicating the occurrence of electrophilic chlorination during CB oxidation. In particular, the dichlorobenzene detected in the effluents of α-MnO₂ might generate unintended dioxins via a nucleophilic substitution reaction.

Key words: MnO₂, Chlorobenzene, Catalytic oxidation, Polychlorinated byproducts, Environmental risk

Xiaole Weng, Yu Long, Wanglong Wang, Min Shao, Zhongbiao Wu. Structural effect and reaction mechanism of MnO₂ catalysts in the catalytic oxidation of chlorinated aromatics[J]. Chinese Journal of Catalysis, 2019, 40(5): 638-646.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(19)63322-X

https://www.cjcatal.com/EN/Y2019/V40/I5/638

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Structural effect and reaction mechanism of MnO₂ catalysts in the catalytic oxidation of chlorinated aromatics

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