N2 Hydrogenation with Molecular Catalysis in a Palladium Membrane Reactor

• Applicant: Professor Nikolay Kornienko, Ph.D.
• Subject Area: Physical Chemistry of Solids and Surfaces, Material Characterisation ; Inorganic Molecular Chemistry - Synthesis and Characterisation ; Technical Chemistry
• Term: since 2024
• Project identifier: Deutsche Forschungsgemeinschaft (DFG) - Project number 548295720

This project aims to understand and develop a sustainable route for N2 hydrogenation for the production of green ammonia as a fertilizer and value added chemical. This will be accomplished through the integration of a molecular catalyst with a Pd membrane reactor. Pd-membrane reactors enable the hydrogenation of reactants using H atoms abstracted from water but in reaction environments that are incompatible with water. This is enabled by the ability of Pd to transfer H (derived from water) to organic solvents with unsaturated reactants. With a view towards sustainability, the entire system can be driven by renewable electricity and uses water as the sole hydrogen source. A limit of such systems is that they are hindered by the lack of catalytic capacity of Pd to carry out challenging hydrogenation steps. To this end, this project combines a Pd membrane reactor with a molecular Ni Terpyridine (Ni-Tpy) catalyst to carry out the hydrogenation of N2 to ammonia. Building on a proof-of-concept data set that ammonia can be selectively generated in this system, the proposal aims to investigate the precise reaction mechanism of how this occurs (e.g. reaction process, intermediates, rate limiting steps, …). We then aim to improve the system through rational ligand design and reactor engineering. Catalytic measurements will be combined with state-of-the-art spectroscopic techniques that strive to provide a comprehensive understanding of how molecular design influences catalytic performance. In all, the project stands to advance the community’s understanding of how to integrate heterogeneous H-transfer membranes and effectively carry out molecularly-driven N2 activation in the overarching direction of sustainability.

• DFG Programme: Research Grants