A molecular photocatalyst consisting of a RuII photocenter, a tetrapyridophenazine bridging ligand, and a PtX2 (X=Cl or I) moiety as the catalytic center functions as a stable system for light-driven hydrogen production. The catalytic activity of this photochemical molecular device (PMD) is significantly enhanced by exchanging the terminal chlorides at the Pt center for iodide ligands. Ultrafast transient absorption spectroscopy shows that the intramolecular photophysics are not affected by this change. Additionally, the general catalytic behavior, that is, instant hydrogen formation, a constant turnover frequency, and stability are maintained. Unlike as observed for the Pd analogue, the presence of excess halide does not affect the hydrogen generation capacity of the PMD. The highly improved catalytic efficiency is explained by an increased electron density at the Pt catalytic center, this is confirmed by DFT studies.
Autorzy
- M. Pfeffer,
- Tanja Kowacs,
- Maria Wachtler,
- prof. dr hab. Julien Guthmuller link otwiera się w nowej karcie ,
- Benjamin Dietzek,
- Johannes Vos,
- Sven Rau
Informacje dodatkowe
- DOI
- Cyfrowy identyfikator dokumentu elektronicznego link otwiera się w nowej karcie 10.1002/anie.201409442
- Kategoria
- Publikacja w czasopiśmie
- Typ
- artykuł w czasopiśmie wyróżnionym w JCR
- Język
- angielski
- Rok wydania
- 2015
Źródło danych: MOSTWiedzy.pl - publikacja "Optimization of Hydrogen - Evolving Photochemical Molecular Devices" link otwiera się w nowej karcie