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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

European Journal of Inorganic Chemistry, 2012, Vol.2012 (1), p.59-64 [Periódico revisado por pares]

Weinheim: WILEY-VCH Verlag

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  • Título:
    Photocatalytic H2 Production with a Rhenium/Cobalt System in Water under Acidic Conditions
  • Autor: Guttentag, Miguel ; Rodenberg, Alexander ; Kopelent, René ; Probst, Benjamin ; Buchwalder, Christian ; Brandstätter, Marco ; Hamm, Peter ; Alberto, Roger
  • Assuntos: Cobalt ; Green chemistry ; Homogeneous catalysis ; Hydrogen ; Photochemistry
  • É parte de: European Journal of Inorganic Chemistry, 2012, Vol.2012 (1), p.59-64
  • Notas: istex:77D2AA8CBB79FE0374D1DC815752AB5E95B108D3
    University of Zürich
    Swiss National Foundation - No. 200021-119798
    ark:/67375/WNG-9W0SCW2W-L
    ArticleID:EJIC201100883
  • Descrição: 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. Ascorbic acid was used as electron donor in a homogeneous rhenium/cobalt‐based system for photocatalytic hydrogen evolution to lower the pH of the reaction solution. The system showed higher stability in terms of turnover numbers and reaction times than similar systems that work under basic conditions with triethanolamine as electron donor.
  • Editor: Weinheim: WILEY-VCH Verlag
  • Idioma: Inglês

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