Quantum yield measurements of light-induced H2 generation in a photosystem I鈥揫FeFe]-H2ase nanoconstruct

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• 作者：Amanda M. Applegate ; Carolyn E. Lubner ; Philipp Kn枚rzer…
• 关键词：Biohydrogen ; Photosystem I ; Hydrogenase ; Photosystem I ; hydrogenase ; Bioconjugate ; Solar biofuels ; Molecular wire
• 刊名：Photosynthesis Research
• 出版年：2016
• 出版时间：January 2016
• 年：2016
• 卷：127
• 期：1
• 页码：5-11
• 全文大小：802 KB
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• 作者单位：Amanda M. Applegate (1)
  Carolyn E. Lubner (1) (3)
  Philipp Kn枚rzer (2)
  Thomas Happe (2)
  John H. Golbeck (1) (3)
  
  1. Department of Chemistry, The Pennsylvania State University, University Park, PA, 16802, USA
  3. Department of Biochemistry and Molecular Biology, The Pennsylvania State University, University Park, PA, 16802, USA
  2. Lehrstuhl f眉r Biochemie der Pflanzen, AG Photobiotechnologie, Ruhr-Universit盲t Bochum, 44780, Bochum, Germany
  
• 刊物类别：Biomedical and Life Sciences
• 刊物主题：Life Sciences
  Plant Physiology
  
• 出版者：Springer Netherlands
• ISSN：1573-5079

文摘

The quantum yield for light-induced H₂ generation was measured for a previously optimized bio-hybrid cytochrome c ₆-crosslinked PSI_C13G鈥?,8-octanedithiol鈥揫FeFe]-H₂ase_C97G (PSI鈥揌₂ase) nanoconstruct. The theoretical quantum yield for the PSI鈥揌₂ase nanoconstruct is 0.50 molecules of H₂ per photon absorbed, which equates to a requirement of two photons per H₂ generated. Illumination of the PSI鈥揌₂ase nanoconstruct with visible light between 400 and 700 nm resulted in an average quantum yield of 0.10鈥?.15 molecules of H₂ per photon absorbed, which equates to a requirement of 6.7鈥?0 photons per H₂ generated. A possible reason for the difference between the theoretical and experimental quantum yield is the occurrence of non-productive PSI_C13G鈥?,8-octanedithiol鈥揚SI_C13G (PSI鈥揚SI) conjugates, which would absorb light without generating H₂. Assuming the thiol-Fe coupling is equally efficient at producing PSI鈥揚SI conjugates as well as in producing PSI鈥揌₂ase nanoconstructs, the theoretical quantum yield would decrease to 0.167 molecules of H₂ per photon absorbed, which equates to 6 photons per H₂ generated. This value is close to the range of measured values in the current study. A strategy that purifies the PSI鈥揌₂ase nanoconstructs from the unproductive PSI鈥揚SI conjugates or that incorporates different chemistries on the PSI and [FeFe]-H₂ase enzyme sites could potentially allow the PSI鈥揌₂ase nanoconstruct to approach the expected theoretical quantum yield for light-induced H₂ generation. Keywords Biohydrogen Photosystem I Hydrogenase Photosystem I-hydrogenase Bioconjugate Solar biofuels Molecular wire