In situ investigation of iron-based ammonia decomposition catalysts derived from crystalline precursors

• Applicants: Professor Dr. Malte Behrens, since 10/2021; Professorin Dr. Claudia Weidenthaler
• Subject Area: Physical Chemistry of Solids and Surfaces, Material Characterisation ; Technical Chemistry
• Term: from 2020 to 2024
• Project identifier: Deutsche Forschungsgemeinschaft (DFG) - Project number 442614184

• Final Report Year: 2025

Final Report Abstract

Ammonia is an attractive transport and storage medium for hydrogen. The release of hydrogen from ammonia can be achieved via a thermally catalysed reaction, the ammonia decomposition. Highly active, stable and cost-effective catalysts are required for this reaction. In this project, new catalyst materials were produced from the base metals iron, cobalt and nickel, their properties were comprehensively investigated and contributions were made to a fundamental understanding of the interactions of metal-support interactions, particle size effects and the microstructure of the resulting supported materials under activation and working conditions of the catalyst. By combining controlled synthesis, comprehensive (operando) analysis and catalytic measurements, it was possible to show in particular that precursors from homogeneous solid solutions of the metal and carrier components can provide highly active materials, but that these must be activated under special conditions and behave dynamically under reaction conditions. Furthermore, it was shown that, depending on the particle size, a change in the rate-determining step can occur at high reaction temperatures and that a new method for the production of catalysts for ammonia cleavage could be established with microemulsion-supported co-precipitation.

Publications

• In‐situ Investigations of Co@Al2O3 Ammonia Decomposition Catalysts: The Interaction between Support and Catalyst. ChemCatChem, 14(20).
  Weidenthaler, Claudia; Schmidt, Wolfgang; Leiting, Sebastian; Ternieden, Jan; Kostis, Alexander; Ulucan, Tolga Han & Budiyanto, Eko
  
• Hydrogen storage in liquid hydrogen carriers: recent activities and new trends. Progress in Energy, 5(1), 012004.
  Ulucan, Tolga Han; Akhade, Sneha A.; Ambalakatte, Ajith; Autrey, Tom; Cairns, Alasdair; Chen, Ping; Cho, Young Whan; Gallucci, Fausto; Gao, Wenbo; Grinderslev, Jakob B.; Grubel, Katarzyna; Jensen, Torben R.; de Jongh, Petra E.; Kothandaraman, Jotheeswari; Lamb, Krystina E.; Lee, Young-Su; Makhloufi, Camel; Ngene, Peter; Olivier, Pierre ... & Weidenthaler, Claudia
  
• Support effect on Ni-based mono- and bimetallic catalysts in CO2 hydrogenation. Nanoscale, 16(37), 17378-17392.
  Wang, Jihao; Chen, Shilong; Ticali, Pierfrancesco; Summa, Paulina; Mai, Simon; Skorupska, Katarzyna & Behrens, Malte
  
• Unveiling the Structure–Property Relationship of MgO-Supported Ni Ammonia Decomposition Catalysts from Bulk to Atomic Structure by In Situ/Operando Studies. ACS Catalysis, 14(5), 2828-2841.
  Ulucan, Tolga H.; Wang, Jihao; Onur, Ezgi; Chen, Shilong; Behrens, Malte & Weidenthaler, Claudia
  
• Hydrogen Release From Ammonia: Size and Support Effects in Heterogeneous Transition Metal Catalysis. ChemCatChem, 17(5).
  Wang, Jihao; Chen, Shilong & Behrens, Malte