M-and-M · Modelling Molecular and Multi-atom Site Catalysts for Oxygen Electrocatalysis

Molecular & dual-metal site catalysts (M&M) are an emerging and promising class of materials that simultaneously enable non-fossil fuel cell technologies and reduce the impact of intensive mining by optimizing resources. There is a variety of strategies to tune their catalytic properties, due to their adaptable geometry and different ligands combinations, but M&M catalysts are particularly unexplored due to their novelty, and therefore the focus of this proposal. The M&M project aims to develop a computational approach to accurately predict the catalytic properties of these materials for the oxygen reduction reaction (ORR). The methodology will be refined by validating computational results against experimental data. It will benefit the scientific community and move beyond the state-of-the-art, while achieving: databases of 1) Hubbard parameters and 2) ORR adsorption energies; 3) a computational workflow; 4) a set of empirical corrections. This work addresses a key gap in electrocatalysis - the need for an updated computational approach and the lack of experimental validation for computational predictions. To achieve these results, the scientific work will proceed through a funnel-like approach, beginning with a database of ~50,000 structures. This database will be computationally screen to obtain transferable Hubbard correction parameters for a selected set of 8,192 M&M catalysts. The next step involves calculating adsorption energies for ORR intermediates on 300 of these catalysts, from which 42 promising candidates will be selected for experimental validation. A final selection of 24 catalysts will be synthesized and tested electrochemically during a secondment to establish empirical corrections.The project is extremely relevant to the programme as it will provide machine learning-ready data and a validated computational approach to accelerate the discovery of catalysts for green energy generation, directly supporting the EU Green Deal climate goals.