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Photocatalytic H2 production with a Rhenium/Cobalt system in water under acidic conditions


Guttentag, Miguel; Rodenberg, Alexander; Kopelent, René; Probst, Benjamin; Buchwalder, Christian; Brandstätter, Marco; Hamm, Peter; Alberto, Roger (2012). Photocatalytic H2 production with a Rhenium/Cobalt system in water under acidic conditions. European Journal of Inorganic Chemistry, 2012(1):59-64.

Abstract

In photocatalytic H2 formation, tertiary amines are commonly used as sacrificial electron donors, thereby limiting the pH range for studies in water and the concentration of free protons. We found that ascorbate rapidly reductively quenches the excited state of [Re(CO)3(bipy)(py)]+ (bpy = 2,2′-bipyridyl; py = pyridine). In combination with the water reduction catalyst (WRC) [Co{(DO)(DOH)pn}Br2] [(DO)(DOH)pn = N2,N2′-propanediylbis(2,3-butanedione 2-imine 3-oxime)], this system produces H2 upon irradiation with light under acidic conditions (pH range 2–6) and with significantly enhanced turnover numbers. Furthermore, we observed that, in contrast to similar systems with tertiary amines, oxidized ascorbate (dehydroascorbic acid) is slowly re-reduced during the course of photocatalysis.

Abstract

In photocatalytic H2 formation, tertiary amines are commonly used as sacrificial electron donors, thereby limiting the pH range for studies in water and the concentration of free protons. We found that ascorbate rapidly reductively quenches the excited state of [Re(CO)3(bipy)(py)]+ (bpy = 2,2′-bipyridyl; py = pyridine). In combination with the water reduction catalyst (WRC) [Co{(DO)(DOH)pn}Br2] [(DO)(DOH)pn = N2,N2′-propanediylbis(2,3-butanedione 2-imine 3-oxime)], this system produces H2 upon irradiation with light under acidic conditions (pH range 2–6) and with significantly enhanced turnover numbers. Furthermore, we observed that, in contrast to similar systems with tertiary amines, oxidized ascorbate (dehydroascorbic acid) is slowly re-reduced during the course of photocatalysis.

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Additional indexing

Item Type:Journal Article, refereed, original work
Communities & Collections:07 Faculty of Science > Department of Chemistry
Dewey Decimal Classification:540 Chemistry
Language:English
Date:2012
Deposited On:11 Apr 2012 06:30
Last Modified:23 Sep 2018 05:25
Publisher:Wiley-Blackwell
ISSN:1434-1948
OA Status:Closed
Publisher DOI:https://doi.org/10.1002/ejic.201100883

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