[Ru(NCN-Me)(bpy)(&z.dbd;O)] mediated efficient photo-driven water oxidation

The [Ru(NCN-Me)(bpy)H 2 O](PF 6 ) 2 complex ( 1 ) (where NCN-Me is the neutral N -methyl-3,5-di(2-pyridyl)pyridinium iodide after deprotonation of the C-H bond) acts as an active catalyst for the visible light driven oxidation of water, when employed with [Ru(bpy) 3 ] 2+ as the photosensitizer and N...

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Veröffentlicht in:RSC advances 2016-06, Vol.6 (66), p.61959-61965
Hauptverfasser: Patel, Jully, Majee, Karunamay, Padhi, Sumanta Kumar
Format: Artikel
Sprache:eng
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Zusammenfassung:The [Ru(NCN-Me)(bpy)H 2 O](PF 6 ) 2 complex ( 1 ) (where NCN-Me is the neutral N -methyl-3,5-di(2-pyridyl)pyridinium iodide after deprotonation of the C-H bond) acts as an active catalyst for the visible light driven oxidation of water, when employed with [Ru(bpy) 3 ] 2+ as the photosensitizer and Na 2 S 2 O 8 as the sacrificial electron acceptor in a phosphate buffer solution at pH 6.5, in the presence of a visible light emitting diode (LED; visible light 10.2 mW cm −2 ) at 20 °C. The system exhibits very high activity, achieving 130 turnovers with respect to catalyst and an initial turnover rate TOF of 0.10 s −1 . The controlled experiments conducted for the photo-oxidation of water indicate that the catalytic system is dependent upon the following: (i) a visible light source, (ii) photosensitizer, (iii) catalyst and, (iv) pH. During the photocatalysis of water oxidation for 2 h in a phosphate buffer solution at pH 6.5, there was no degradation of the catalyst 1 , which indicates the good photo-stability of the complex. The NCN-Me coordinates as a neutral ligand after deprotonation of the central C-H bond; generating the negatively charged carbon center favors a reduction in the redox potential of the complex, which considerably lowers the overpotential to 100 mV at pH 6.5 for the oxidation of water. The complex [Ru(NCN-Me)(bpy)H 2 O](PF 6 ) 2 acts as an active catalyst for the photo-driven oxidation of water, when employed with [Ru(bpy) 3 ] 2+ as photosensitizer and Na 2 S 2 O 8 as sacrificial electron acceptor at pH 6.5 phosphate buffer, with a TON of 130.
ISSN:2046-2069
DOI:10.1039/c6ra12074a