Mononuclear Fe() Schiff base antipyrine complexes for catalytic hydrogen generation

Mononuclear Fe( iii ) complexes containing an antipyrine Schiff base ligand were prepared and fully characterized, demonstrating a planar tetradentate coordination geometry. These complexes were found to be active for the hydrogen evolution reaction. Catalysis occurs at −1.4 V vs. Fc + /Fc, with an...

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Veröffentlicht in:Dalton transactions : an international journal of inorganic chemistry 2024-09, Vol.53 (37), p.15421-15426
Hauptverfasser: Cropley, Jessica D, Mitchell, Amanda C, Fritsch, Nicole A, Ho, Marissa, Wells, Timothy D, Reynolds, Todd M, Brennessel, William W, McNamara, William R
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Sprache:eng
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Zusammenfassung:Mononuclear Fe( iii ) complexes containing an antipyrine Schiff base ligand were prepared and fully characterized, demonstrating a planar tetradentate coordination geometry. These complexes were found to be active for the hydrogen evolution reaction. Catalysis occurs at −1.4 V vs. Fc + /Fc, with an overpotential of 700 mV. The complexes are active electrocatalysts with a turnover frequency of 700 s −1 . Furthermore, when paired with a chromophore and sacrificial donor, the complexes are active photocatalysts demonstrating >1700 turnovers during 40 hours of irradiation with a quantum yield of up to 5.4%. The catalysts have also been found to operate in natural water samples of varying salinity. Mononuclear Fe( iii ) complexes containing an antipyrine Schiff base ligand were prepared and fully characterized, demonstrating a planar tetradentate coordination geometry. The resulting complexes are active for HER with possible ligand cooperativity.
ISSN:1477-9226
1477-9234
1477-9234
DOI:10.1039/d4dt01876a