Towards catalyst design and databases for molecular OER catalysis

Despite fossil fuels having brought forth the dawn of civilisation as we know it, they have also left an enduring effect on the Earth’s climate. To address this, it is imperative that we devise renewable technologies to decarbonise our economy. For example, one could envision using sunlight to drive (photo)electrochemical water splitting devices to produce H2, a highly energy-dense fuel when compressed and stored. A major roadblock in realizing this, however, is the lack of affordable and high-performing catalysts for the oxygen evolution reaction (OER).[1]
In the first part of this seminar, I will describe our recent findings which demonstrate that molecular catalysts obey the same OER scaling relations observed for heterogeneous systems, and thereby are constrained to the “overpotential wall” imposed by such relations.[2-6] This part will also discuss how some of the most active complexes reported in the literature can circumvent the overpotential wall and how this knowledge can be translated into a set of catalyst design principles to advance the discovery of “ideal” molecular OER catalysts.
The second part of my presentation will be dedicated to the high-throughput screening of molecular OER catalysts using well-known ligand scaffolds and transition metals, demonstrating the universality and method independent nature of scaling relations.[7] This study has also led to the discovery of new complexes based on earth-abundant elements with predicted activities comparable to Ru-based catalysts, as well as the development of machine learning algorithms to assess OER activity at almost no computational cost and with errors comparable to state-of-the-art DFT methods.[8]
In the final part of this talk, I will describe our ongoing research efforts in the generation of a curated molecular OER database and compliant with the principles of findability, accessibility, interoperability, and reusability (FAIR).

References [1] Suen, N.-T.; Hung, S.-F.; Quan, Q.; Zhang, N.; Xu, Y.-J.; Chen, H. M. Chem. Soc. Rev. 2017, 46, 337-365. [2] Craig, M. J.; Coulter, G. O.; Dolan, E. T.; Soriano-López, J.; Mates-Torres, E.; Schmitt, W.; García-Melchor, M. Nat. Commun. 2019, 10, 4993.
[3] Craig, M. J.; García-Melchor, M. Curr. Opin. Electrochem. 2022, 35, 101044. [4] Craig, M. J.; Barda-Chatain, R.; García-Melchor, M. J. Catal. 2021, 393, 202–206. [5] Zhang, B.; Zheng, X.; Voznyy, O.; Comin, R.; Bajdich, M.; García-Melchor, M.; Xu, J.; Liu, M.; et al. Science, 2016, 352, 333-337. [6] Desmond Ng, J. W.; García-Melchor, M.; Bajdich, M.; Kirk, C.; Chakthranont, P.; Vojvodic, A.; Jaramillo, T. F. Nat. Energ. 2016, 1, 16053. [7] Craig, M. J.; García-Melchor, M. Cell Rep. Phys. Sci. 2021, 2, 100492. [8] Craig, M. J.; García-Melchor, M. Molecules, 2021, 26, 6362.