Molecular catalysis performed by MOFs relevant for energy conversion

The research project

We exploit structural modularity of metal-organic frameworks (MOFs) to immobilize molecular functional units to perform catalytic processes such as CO2 reduction, proton reduction, water oxidation, and organic transformations. MOFs are considered to be robust 3D porous architecture that can provide a suitable platform for the incorporation of potentially labile molecular catalysts. Using these systems, we perform electrochemical, photochemical, photoelectrochemical and thermal chemical conversions relevant for sustainable energy research. In the context of light-to-fuel conversion, investigating molecular catalysis performed by MOF-based systems should provide significant insight about structure-function relation of porous materials and also help develop efficient and robust catalysts.

Selected references

• Howe, A.; Liseev, T.; Gil-Sepulcre, M.; Gimbert-Surinach, C.; Benet-Buchholz, J.; Llobet, A.; Ott, S. Electrocatalytic Water Oxidation from a Mixed Linker MOF Based on NU-1000 with an Integrated Ruthenium-Based Metallo-Linker. Mater. Adv. 2022, 3, 4227–4234. https://doi.org/10.1039/D2MA00128D
• Amaro-Gahete, J.; Pavliuk, M. V.; Tian, H.; Esquivel, D.; Romero-Salguero, F. J.; Ott, S. Catalytic Systems Mimicking the [FeFe]-Hydrogenase Active Site for Visible-Light-Driven Hydrogen Production. Coord. Chem. Rev. 2021, 448, 214172. https://doi.org/10.1016/j.ccr.2021.214172
• Laurans, M.; Wells, J. A. L.; Ott, S. Immobilising Molecular Ru Complexes on a Protective Ultrathin Oxide Layer of P-Si Electrodes Towards Photoelectrochemical CO2 Reduction. Dalton Trans. 2021, 50, 10482–10492. https://doi.org/10.1039/D1DT01331A
• Johnson, B. A.; Ott, S. Diagnosing Surface Versus Bulk Reactivity for Molecular Catalysis within Metal-Organic Frameworks Using a Quantitative Kinetic Model. Chem. Sci. 2020, 11, 7468–7478. https://doi.org/10.1039/D0SC02601H
• Liseev, T.; Howe, A.; Hoque, M. A.; Gimbert-Suriñach, C.; Llobet, A.; Ott, S. Synthetic Strategies to Incorporate Ru-Terpyridyl Water Oxidation Catalysts into MOFs: Direct Synthesis vs. Post-Synthetic Approach. Dalton Trans. 2020, 49, 13753–13759. DOI https://doi.org/10.1039/D0DT01890B
• Roy, S.; Huang, Z.; Bhunia, A.; Castner, A.; Gupta, A. K.; Zou, X.; Ott, S. Electrocatalytic Hydrogen Evolution from a Cobaloxime-Based Metal-Organic Framework Thin Film. J. Am. Chem. Soc. 2019, 141, 15942–15950. https://doi.org/10.1021/jacs.9b07084