TY - JOUR A1 - Winter, Franziska Luise A1 - Diehl, Patrick A1 - Telaar, Pascal A1 - Watermann, Clara Maria A1 - Kaluza, Stefan A1 - Muhler, Martin A1 - Apfel, Ulf-Peter A1 - Zeidler-Fandrich, Barbara T1 - Influence of the catalyst precursor for cobalt on activated carbon applied in ammonia decomposition JF - Catalysis Today N2 - Ammonia is a key compound for storing and transporting green hydrogen. However, the efficient release of stored hydrogen through thermocatalytic ammonia decomposition is achievable only at temperatures around 600 °C, particularly with non-noble metal-based catalysts, which prove to be both ecologically and economically more feasible. In this study, electrically conductive activated carbon was selected as the catalyst support, chosen specifically for its suitability in achieving more energy-efficient direct reactor heating through the ohmic resistance of the catalysts. Cobalt salts were wet impregnated on activated carbon investigating the influence of different precursors (cobalt nitrate and cobalt acetate) and pyrolysis temperatures (400 °C and 600 °C) under N2 flow on the cobalt particle size and the incorporation of cobalt into the carbon matrix. TEM imaging and CO-chemisorption revealed well dispersed cobalt particles with sizes below 10 nm for the catalysts synthesized from the cobalt nitrate precursor. On the other hand, cobalt acetate led to about nine times larger Co agglomerates, which were partially detached from the carbon matrix. Moreover, this substantial difference in the Co particle size results in a significantly higher ammonia conversion for cobalt nitrate-based catalysts, achieving 94 % of ammonia conversion at 600 °C. Furthermore, the long-term stability test of the cobalt nitrate-based catalyst resulted in a slight deactivation of only 2 % ammonia conversion at 500 °C. KW - Katalyse KW - Ammoniak KW - Grüner Wasserstoff KW - Ammonia decomposition KW - Carbon supported cobalt KW - Synthesis design KW - Cobalt acetate KW - Cobalt nitrate KW - Resistance heating Y1 - 2024 U6 - http://nbn-resolving.de/urn/resolver.pl?urn:nbn:de:hbz:due62-opus-46600 SN - 0920-5861 VL - 429 PB - Elsevier ER - TY - JOUR A1 - Greuel, Marc A1 - Watermann, Clara Maria A1 - Lohmann, Heiko A1 - Kaluza, Stefan A1 - Apfel, Ulf-Peter A1 - Zeidler-Fandrich, Barbara T1 - The conversion of ethanol over 3d-metal saponite-like smectites JF - Materials Advances N2 - The replacement of fossil fuel processes with renewable pathways is critical to circumvent climate change and environmental risks. A process of interest is the production of 1,3-butadiene (BD), which is primarily derived as a by-product of naphtha steam cracking. A sustainable alternative path involves converting renewable ethanol to BD via the Lebedev process, which requires a catalyst with balanced redox, acidic, and basic sites. Due to the necessity of a multifunctional catalyst, existing materials for this reaction are either comprised of catalyst mixtures or supported catalysts. In this study, we introduce a bulk material, saponite, containing M–O–Si sites, which combine required catalytic sites for the ethanol to BD (ETB) reaction in one material. The product composition in ethanol conversion were strongly dependent on the type of 3d-metal used, while no conclusive correlation between surface properties, conversion, and product composition was observed. Herein, using V-Sap*, we achieved an ethene productivity of 448 gethene kgcat−1 h−1 (74%) at 573.15 K. High acetaldehyde productivity was maintained with Cu-Sap* (466 gAcA kgcat−1 h−1, 49%) at 573.15 K and Zn-Sap (528 gAcA kgcat−1 h−1, 55%) at 723.15 K. Mg-Sap primarily produced ethene but also yielded 10 gBD kgcat−1 h−1 BD at 723.15 K. Higher BD outputs were observed with Ni-Sap (31 gBD kgcat−1 h−1 at 523.15 K) and Mn-Sap* (51 gBD kgcat−1 h−1 at 723.15 K). This underscores the potential of saponite-based materials for flexible product outputs in ethanol conversion, influenced by the choice of integrated 3d-metal. KW - Butadien KW - Katalyse KW - Material Y1 - 2025 U6 - http://nbn-resolving.de/urn/resolver.pl?urn:nbn:de:hbz:due62-opus-52973 SN - 2633-5409 IS - 6 SP - 2885 EP - 2898 PB - Royal Society of Chemistry ER -