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Plasma-Catalytic Oxidation of Toluene on MnxOy at Atmospheric Pressure and Room Temperature

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Abstract

MnxOy/SBA-15 catalysts were prepared via the impregnation method and utilized for toluene removal in dielectric barrier discharge plasma at atmospheric pressure and room temperature. The catalysts were characterized by X-ray diffraction, N2 adsorption–desorption, Raman spectroscopy, X-ray photoelectron spectroscopy, H2 temperature-programmed reduction, and O2 temperature-programmed desorption methods. The characterization results indicated that manganese loading did not influence the 2D-hexagonal mesoporous structure of SBA-15. The catalyst had various oxidation states of manganese (Mn2+, Mn3+, and Mn4+), with Mn3+ being the dominant oxidation state. Toluene removal was investigated in the environment of pure N2 and 80 % N2 + 20 % O2 plasma, showing that the toluene removal efficiency and CO2 selectivity were noticeably increased by MnxOy/SBA-15, especially in the presence of 5 % Mn/SBA-15. This activity was closely related to the high dispersion of 5 % Mn on SBA-15 and the lowest reduction temperature exhibited by this catalyst. Mn loading increased the yield of CO2 in the N2 plasma and promoted the deep oxidation of toluene. During toluene oxidation, oxygen exchange might follow a pathway, wherein bulk oxygen was released from the MnxOy/SBA-15 surface; gas-phase O2 subsequently filled up the vacancies created on the oxide. Each of the manganese oxidation states played an important role; Mn2O3 was considered as a bridge for oxygen exchange between the gas phase and the catalyst, and Mn3O4 mediated transfer of oxygen between the catalyst and toluene.

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Acknowledgments

We would like thanks Hangao Liu very much for assistance in experimental setup. This work was carried out with the support of “the National Natural Science Foundation of China” (No. 50978103, No. U1201231).

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Authors and Affiliations

  1. College of Environment and Energy, South China University of Technology, Guangzhou Higher Education Mega Centre, Panyu District, Guangzhou, 510006, People’s Republic of China

    Meijuan Lu, Rong Huang, Peitao Wang, Limin Chen, Junliang Wu, Mingli Fu, Bichun Huang & Daiqi Ye

  2. Guangdong Provincial Key Laboratory of Atmospheric Environment and Pollution Control, Guangzhou, 510006, People’s Republic of China

    Meijuan Lu, Rong Huang, Peitao Wang, Limin Chen, Junliang Wu, Mingli Fu, Bichun Huang & Daiqi Ye

  3. Centre for Clean Environment and Energy, Environmental Futures Centre, and Griffith School of Environment, Griffith University, Gold Coast, QLD, 4222, Australia

    William Wen

  4. The Key Laboratory of Pollution Control and Ecosystem Restoration in Industry Clusters (South China University of Technology), Ministry of Education, Guangzhou, 510006, People’s Republic of China

    Daiqi Ye

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  1. Meijuan Lu
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  2. Rong Huang
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Correspondence to Daiqi Ye.

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Lu, M., Huang, R., Wang, P. et al. Plasma-Catalytic Oxidation of Toluene on MnxOy at Atmospheric Pressure and Room Temperature. Plasma Chem Plasma Process 34, 1141–1156 (2014). https://doi.org/10.1007/s11090-014-9556-y

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  • DOI: https://doi.org/10.1007/s11090-014-9556-y

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