Universitat Rovira i Virgili
Chemical Science and Technology
Experimentally and computationally guided design of efficient water oxidation catalysts
The artificial photo(electro)synthesis of solar fuels from unexpensive, abundant raw materials such as water has been proposed as a promising solution to the current energy problem. A well-known obstacle to the production of solar fuels stems from retrieving the necessary electrons and protons from water oxidation. To overcome such difficulty, tremendous efforts are being devoted to develop efficient water oxidation catalysts (WOCs), including molecular systems. Molecular systems, such as organometallic Ru-WOCs, are receiving much attention because their performance can potentially be tailored and optimized by an appropriate selection of the ancillary ligands. More recently, Ir-WOCs have also emerged as efficient catalysts although intense ligand exploration is still required for improving their performance. One of the advantages of Ir-WOCs is that they are able to oxidize water at almost neutral pH (compared to the highly corrosive low pH required for Ru-WOCs) which is fundamental for large-scale application. Nevertheless, there is a controversy about the nature of the active species. While authors such as Crabtree and Brudvig have proposed dinuclear active species others (e.g., Macchioni and Bernhard) have proposed that mononuclear species are involved. Thus, while the first examples of the use of Ir-WOCs have been reported, more research needs to be done. In this respect, two main directions can be distinguished, which determine the main objectives of this present project:
1) The first objective is the systematic evaluation of the effectiveness of new ligand types to study the potentiality of Ir-catalysts for water oxidation.
2) The second objective is to elucidate the true nature of the active species in water oxidation using Ir-based catalysts. A deep understanding of the process is essential for future development of more efficient catalysts.
These interdisciplinary objectives require bringing together experimental (related to ligand library synthesis and performance testing) and computational studies. The computational studies will be carried out in collaboration with experts in the field. In this respect, the supervisors of this project have collaborations with Profs. Josep Maria Poblet (URV, Tarragona), Feliu Maseras (ICIQ Institut, Tarragona) and Per-Ola Norbby (AstraZeneca, Sweden), leaders in Europe in the field of computational chemistry. The use of the virtual catalyst screening can speed up the process of finding the optimum catalyst, which would allow significant progress in the field.
37.5 hours a week
|This project has received funding from the European Union's Horizon 2020 research and innovation programme under the Marie Skłodowska-Curie grant agreement No. 713679|