Towards the usage of iron(II/III) complexes as potent photosensitizers in organic photoredox catalysis
(2022)
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- Abstract
- Since many years, chemists leveraged the photophysical properties inherent to ruthenium or iridium-based photosensitizers to develop strategies towards conversion of sunlight into chemical energy such as molecular hydrogen or complex organic molecules. However, the scarcity and toxicity of these elements prevent the potential scalability of this kind of system. This is why the development of efficient photocatalytic complexes using cheap and abundant first row metals would offer an important solution to this problem. Due to its abundance in the earth’s crush, the iron element seems perfect to supplant its ruthenium analogue. Nonetheless, the Fe(II)-based polypyridyl photosensitizers suffer from their intrinsic photophysical properties that deactivate non-radiatively the low-lying excited-state and hence reduce its lifetime. Important insights were recently brought by Wärnmark et al. in the conception of Fe(II) and Fe(III)-based photosensitizers through ligand modifications strategy. During this Ph.D. thesis, we have designed and synthesized novel iron-based photosensitizers. Through coordination sphere modifications, we attempted to tune their photophysical properties and then utilized them as potent photosensitizer in photoredox catalysis. By careful investigations, we were able to determine the key parameters that could potential govern a photoreaction and to propose an in-depth reaction mechanism through time-resolved ultrafast spectroscopic techniques.
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Citations
Aydogan, A. (2022). Towards the usage of iron(II/III) complexes as potent photosensitizers in organic photoredox catalysis. https://hdl.handle.net/2078.5/103386