RuCatDAH: Rational design of Ruthenium Catalysts towards efficient Decomposition of Ammonia for Hydrogen production

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Efficient decomposition of ammonia (NH3) to generate hydrogen (H2) is an ideal approach to solving the H2 storage and transportation problem. Ru-based catalyst, the state-of-art catalyst toward NH3 decomposition, still fails to meet the requirements for large-scale applications due to the unaffordable cost and vague understanding of the catalyst structure-performance relationship.Designing catalysts with identical active centers on the atomic level is highly desired to mitigate this challenge. This project will precisely design and synthesize supported Ru catalysts with accurate sizes ranging from atomic and sub-nanometric clusters to nanoparticles. The multi-scale Ru entities will change the NH3 adsorption, N-N formation, and the Ru-N dissociation on the catalyst surface, which can be probed via a series of operando/in-situ X-ray or Infrared spectroscopic techniques. The possible intermediates and reaction mechanisms (Dissociative and Associative pathways) will be explored with those operando methods in combination with density-functional theory calculations. On this basis, the simultaneous high activity and minimum usage of Ru will be achieved by further modulating the optimal ensembled Ru sites with rare-earth oxide (Zr doped CeO2) surface. These results are expected to provide a solution toward the target of the European Commission in reducing greenhouse gas emissions and promoting the hydrogen economy. Despite ongoing pandemic difficulties, various communication actions will be employed to publicize this research project and elevate the fellowship's impact.