Josep Maria Poblet
Maria Besora Bonet
Chemical Science and Technology
Water oxidation for renewable energy
In the last decade, the artificial water splitting into hydrogen (H2) and oxygen (O2) has become a hot topic in research on renewable energy sources. The main reason is that H2 has a great potential to be used as clean fuel. However, nowadays intensive production of H2 is high energy demanding. A good Water Oxidation Catalyst (WOC) would facilitate the process by reducing the cost of the crucial step: oxidation of water to molecular oxygen. Many catalysts have been proposed that facilitate this reaction, but it is hoped that better catalysts are yet to be discovered.
In this project we pretend to develop a computational modeling project in close collaboration with experimentalists. We plan to use computational tools to explore the details of water oxidation reaction mechanisms of a small number of known WOC. One type of catalysts we would like to explore are the ones synthesized by Diéguez and Pàmies (URV), who have been working on Ir-based catalysts modified with 1,2,3-triazol-5-ylidene ligands. The reason is that they are able to oxidize water at almost neutral pH conditions instead of the undesirable usually used highly corrosive low pH conditions.
The catalytic cycle of the process is not clear, up to the point that there is even, controversy about the nature of the active species. Some results support that it is a monomeric species and others that it is dimer [1,3].
The experience acquired during last years in the computational modeling of water oxidation reaction catalyzed by POM anions by the group of Prof. Poblet,  should help to carry out successfully theoretical modeling studies that should be able to put some light on the
nature of the active species and the key steps of the catalytic cycle. With this key knowledge, we plan to perform a virtual catalyst screening, that speeds up the process of finding the optimum catalyst.
Hence, the main objectives of the computational project are:
* Investigation of the reaction mechanism of water oxidation catalyzed by Ir-based catalysts modified with 1,2,3-triazol-5-ylidene ligands.
The relevance of mononuclear and dimeric active species in the catalytic cycle will be explored.
*Investigation of mechanistic similarities and differences with other successful and unsuccessful water oxidation catalysts. The choice of the systems will depend on the recent advances in the field.
* Virtual catalyst screening, pursuing a better catalyst.
-Matheu, R., Garrido-Barros, P., Gil-Sepulcre, M. Ertem, M.Z.; Sala, X; Gimbert-Suriñac C.; Llobet A. Nat Rev Chem 2019, 3, 331–341.
- Mazloomi, Z.; JMargalef, J.; Gil-Sepulcre, M.; Romero, N.; Albrecht, M.; Llobet, A; Sala, X.; Pàmies, O.; Diéguez M.Effect of ligand
chelation and sacrificial oxidant on the integrity of triazole-based carbene iridium water oxidation catalysts. Under revision (2020).
- Yang, K.R.; Matula, A.J.; Kwon, G. ; Hong, J.; Sheehan, S.W.; Thomsen, JM, Brudvig, GW; Crabtree, RH; Tiede, DM; Chen, LX;. Batista VS. J. Am. Chem. Soc. 2016 138 (17), 5511-5514
-. Soriano-López, D.G. Musaev, C.L. Hill, J.R. Galán-Mascarós, J.J. Carbó, J.M. Poblet J. Catal. 2017, 350, 56-63
Ethics: This project does not involve ethical aspects.
Workplace location: Campus Sescelades, Tarragona
37.5 hours a week
15 March 2021
|This project has received funding from the European Union's Horizon 2020 research and innovation programme under the Marie Skłodowska-Curie grant agreement No. 945413|