TY - JOUR A1 - Seeburg, Dominik A1 - Liu, Dongjing A1 - Radnik, Jörg A1 - Atia, Hanan A1 - Pohl, Marga-Martina A1 - Schneider, Matthias A1 - Martin, Andreas A1 - Wohlrab, Sebastian T1 - Structural changes of highly active Pd/MeOx (Me = Fe, Co, Ni) during catalytic methane combustion N2 - 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. KW - Methane total oxidation KW - Methane removal KW - Carbon dioxide KW - X-ray photoelectron spectroscopy PY - 2018 U6 - http://nbn-resolving.de/urn/resolver.pl?urn:nbn:de:kobv:b43-439412 SN - 2073-4344 VL - 8 IS - 2 SP - Article 42, 1 EP - 13 PB - MDPI AN - OPUS4-43941 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Ha, Q. L. M. A1 - Armbruster, U. A1 - Atia, Hanan A1 - Lund, H. A1 - Agostini, G. A1 - Radnik, Jörg A1 - Vuong, H. T. A1 - Martin, A. T1 - Development of active and stable low nickel content catalysts for dry reforming of methane N2 - Methane dry reforming (DRM) was investigated over highly active Ni catalysts with low metal content (2.5wt%) supported on Mg-Al mixed oxide. The aim was to minimize carbon Deposition and metal sites agglomeration on the working catalyst which are known to cause catalyst deactivation. The solids were characterized using N2 adsorption, X-ray diffraction, temperature-programmed reduction, X-ray photoelectron spectroscopy, and UV-Vis diffuse reflectance spectroscopy. The results showed that MgO-Al2O3 solid solution phases are obtained when calcining Mg-Al hydrotalcite precursor in the temperature range of 550–800 °C. Such phases contribute to the high activity of catalysts with low Ni content even at low temperature (500 °C). Modifying the catalyst preparation with citric acid significantly slows the coking rate and reduces the size of large octahedrally coordinated NiO-like domains, which may easily agglomerate on the surface during DRM. The most effective Ni catalyst shows a stable DRM course over 60 h at high weight hourly space velocity with very low coke deposition. This is a promising result for considering such catalyst systems for further development of an industrial DRM technology. KW - Dry reforming of methane KW - Carbon dioxide KW - Ni PY - 2017 U6 - http://nbn-resolving.de/urn/resolver.pl?urn:nbn:de:kobv:b43-402904 SN - 2073-4344 VL - 7 IS - 5 SP - 157, 1 EP - 157, 17 PB - MDPI AN - OPUS4-40290 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Dang, Thi Thuy Hanh A1 - Seeburg, Dominik A1 - Radnik, Jörg A1 - Kreyenschulte, Carsten A1 - Atia, Hanan A1 - Vu, Thi Thu Ha A1 - Wohlrab, Sebastian T1 - Influence of V-sources on the catalytic performance of VMCM-41 in the selective oxidation of methane to formaldehyde N2 - VMCM-41 catalysts from two different tetravalent Vanadium sources, hydrothermally synthesized after a mild gelation step at room temperature, were used as catalysts for the selective oxidation of methane to formaldehyde. Vanadyl acetylacetonate as VMCM-41 precursor, facilitates highest VOx density with predominance of monomeric and a small portion of low-oligomeric VOx species. It produces CH2O in high yield and the highest space time yield (STYCH2O) reaches 5.3 kgCH2O·kgcat −1·h−1 at 600 °C (rate of formation, rCH2O of 363 h−1). VMCM-41 synthesized from vanadyl sulfate hydrate precursor contains a more significant portion of low-oligomeric species. With a lower V loading, these VOx species are significantly less active resulting in a Maximum STYCH2O of 2.7 kgCH2O·kgcat −1·h−1 at 625 °C (rCH2O of 243 h−1). KW - VOx catalyst KW - Methane KW - Formaldehyde PY - 2018 U6 - https://doi.org/10.1016/j.catcom.2017.09.004 SN - 1566-7367 VL - 103 SP - 56 EP - 59 PB - Elsevier Science AN - OPUS4-42820 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER -