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Photocatalytic H 2 Production with a Rhenium/Cobalt System in Water under Acidic Conditions
Author(s) -
Guttentag Miguel,
Rodenberg Alexander,
Kopelent René,
Probst Benjamin,
Buchwalder Christian,
Brandstätter Marco,
Hamm Peter,
Alberto Roger
Publication year - 2012
Publication title -
european journal of inorganic chemistry
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 0.667
H-Index - 136
eISSN - 1099-0682
pISSN - 1434-1948
DOI - 10.1002/ejic.201100883
Subject(s) - chemistry , photocatalysis , cobalt , turnover number , rhenium , catalysis , pyridine , photochemistry , aqueous solution , inorganic chemistry , imine , oxime , nuclear chemistry , medicinal chemistry , organic chemistry
In photocatalytic H 2 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}Br 2 ] [(DO)(DOH)pn = N 2 , N 2′ ‐propanediylbis(2,3‐butanedione 2‐imine 3‐oxime)], this system produces H 2 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.