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Catalysts 2018, 8(2), 42; https://doi.org/10.3390/catal8020042

Structural Changes of Highly Active Pd/MeOx (Me = Fe, Co, Ni) during Catalytic Methane Combustion

1
Leibniz Institute for Catalysis at the University of Rostock, Albert-Einstein-Str. 29a, D-18059 Rostock, Germany
2
School of Energy and Power Engineering, Jiangsu University, Xuefu Str. 301, Zhenjiang 212013, China
3
Federal Institute of Materials Testing and Research (BAM), Unter den Eichen 44-46, D-12203 Berlin, Germany
*
Author to whom correspondence should be addressed.
Received: 15 December 2017 / Revised: 13 January 2018 / Accepted: 19 January 2018 / Published: 23 January 2018
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Abstract

Fe2O3, Co3O4 and NiO nanoparticles were prepared via a citrate method and further functionalized with Pd by impregnation. The pure oxides as well as Pd/Fe2O3, Pd/Co3O4, and Pd/NiO (1, 5 and 10 wt % Pd) were employed for catalytic methane combustion under methane lean (1 vol %)/oxygen rich (18 vol %, balanced with nitrogen) conditions. Already, the pure metal oxides showed a high catalytic activity leading to complete conversion temperature of T100 ≤ 500 °C. H2-TPR (Temperature-programmed reduction) experiments revealed that Pd-functionalized metal oxides exhibited enhanced redox activity compared to the pure oxides leading to improved catalytic combustion activity at lower temperatures. At a loading of 1 wt % Pd, 1Pd/Co3O4 (T100 = 360 °C) outperforms 1Pd/Fe2O3 (T100 = 410 °C) as well as 1Pd/NiO (T100 = 380 °C). At a loading of 10 wt % Pd, T100 could only be slightly reduced in all cases. 1Pd/Co3O4 and 1Pd/NiO show reasonable stability over 70 h on stream at T100. XPS (X-ray photoelectron spectroscopy) and STEM (Scanning transmission electron microscopy) investigations revealed strong interactions between Pd and NiO as well as Co3O4, respectively, leading to dynamic transformations and reoxidation of Pd due to solid state reactions, which leads to the high long-term stability. View Full-Text
Keywords: methane total oxidation; methane slip; methane removal; carbon dioxide; combustion methane total oxidation; methane slip; methane removal; carbon dioxide; combustion
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This is an open access article distributed under the Creative Commons Attribution License which permits unrestricted use, distribution, and reproduction in any medium, provided the original work is properly cited (CC BY 4.0).

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Seeburg, D.; Liu, D.; Radnik, J.; Atia, H.; Pohl, M.-M.; Schneider, M.; Martin, A.; Wohlrab, S. Structural Changes of Highly Active Pd/MeOx (Me = Fe, Co, Ni) during Catalytic Methane Combustion. Catalysts 2018, 8, 42.

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