Optimizing Photocatalytic H2 Production by Introduction of Pyrazinyls to WRCs and a New tris‐Rhenium Photosensitizer

The replacement of pyridyl by pyrazinyl in ligands of polypyridyl‐based cobalt water reducing catalysts (WRC) shifts reduction potentials anodically. Together with a new, trinuclear ReI photosensitizer, these WRCs show strongly improved photocatalytic performances in turnover numbers (TONs) and maxi...

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Bibliographic Details
Published in:Chemistry : a European journal 2024-08, Vol.30 (43), p.e202401595-n/a
Main Authors: Grundmann, Nora S., Heydari, Neda, Jäggi, Sarah I., Blacque, Olivier, Alberto, Roger
Format: Article
Language:English
Subjects:
artificial photosynthesis
Catalysts
Cobalt
hydrogen
Hydrogen evolution
photocatalysis
Rhenium
solar fuels
water reduction
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Summary:The replacement of pyridyl by pyrazinyl in ligands of polypyridyl‐based cobalt water reducing catalysts (WRC) shifts reduction potentials anodically. Together with a new, trinuclear ReI photosensitizer, these WRCs show strongly improved photocatalytic performances in turnover numbers (TONs) and maximal H2 evolution rate. Depending on the catalyst structure, up to 65 kTONs at 1 μM WRC concentration were reached. Under electrocatalytic conditions in both DMF and H2O, one of the reported WRCs displays remarkable stability, producing H2 steadily over 21 and 14 d, respectively. Polypyridyl‐based cobalt catalysts for the hydrogen evolving reaction were optimized by the introduction of electron‐poor pyrazine in place of pyridine. Photocatalysis experiments with a new tris‐rhenium photosensitizer and detailed electrochemical studies showed trends in turnover numbers and H2 evolution rates and gave grounds for hypotheses on the mechanistic pathway.
ISSN:0947-6539
1521-3765
1521-3765
DOI:10.1002/chem.202401595