Insights into the Mechanism of a Covalently-Linked Organic Dye-Cobaloxime Catalyst System for Dye Sensitized Solar Fuel Device
(English)Manuscript (preprint) (Other (popular science, discussion, etc.)) [Artistic work]
A covalently-linked organic dye-cobaloxime catalyst system is developed by facile click reaction for mechanistic studies and application in a dye sensitized solar fuel device based on mesoporous NiO. This system has been systematically investigated by photophysical measurements, density functional theory, time resolved fluorescence, transient absorption spectroscopy as well as photoelectron spectroscopy. The results show that irradiation of the dye-catalyst on NiO leads to ultrafast hole injection into NiO from the excited dye, followed by a fast electron transfer to reduce the catalyst unit. Moreover, they suggest that the dye undergoes structural changes in the excited state and that excitation energy transfer occurs between neighboring molecules. The photoelectrochemical experiments also show the hydrogen production by this system-based NiO photocathode. The axial chloride ligands of the catalyst are released during photocatalysis to create the active sites for proton reduction. A working mechanism of the dye-catalyst on photocathode is eventually proposed on the basis of this study.
DSSFDs, electron transfer, Cobaloxime catalyst
Research subject Chemistry with specialization in Chemical Physics
IdentifiersURN: urn:nbn:se:uu:diva-301412OAI: oai:DiVA.org:uu-301412DiVA: diva2:954567