4.7 Article

Revelation of Mm4+-Osur-Mn3+ active site and combined Langmuir-Hinshelwood mechanism in propane total oxidation at low temperature over MnO2

Journal

CHEMICAL ENGINEERING JOURNAL
Volume 451, Issue -, Pages -

Publisher

ELSEVIER SCIENCE SA
DOI: 10.1016/j.cej.2022.138868

Keywords

alpha-MnO2; Propane oxidation; Active sites; Kinetic studies; Reaction mechanism

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This study conducted systematic experimental and computational research using OMS-2 as a model compound, revealing Mn4+-O-sur-Mn3+ as the active site at low temperature and proving the condensation mechanism as the catalytic oxidation pathway of propane on MnO2 surface. These research results provide important theoretical support for propane combustion on manganese oxides.
Mn-based oxides exhibit attractive catalytic activity for VOCs oxidation, but the catalytic mechanism and kinetics are still significant challenges and rarely mentioned. Therefore, we prepared OMS-2 manganese oxide octahedral molecular sieve with alpha-MnO2 crystal phase as model compound. By analyzing the properties of the surface chemical states of the catalysts in different reaction stages, combined with the control experiments, the coordination of Mn4+-O-sur-Mn3+ was confirmed as the active site at low temperature. Meanwhile, the reaction path of propane catalytic oxidation on MnO2 surface based on condensation mechanism was proved by in-situ spectroscopy and density functional theory calculation. And kinetic studies revealed that the catalytic combustion of propane processed through Langmuir-Hinshelwood mechanism at low temperature. All these systematic study results supplied a well-defined understanding for the propane combustion over manganese oxide.

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