期刊
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
卷 108, 期 52, 页码 20988-20991出版社
NATL ACAD SCIENCES
DOI: 10.1073/pnas.1114660108
关键词
biohybrid; solar fuels; light harvesting; green biophysics; renewable energy
资金
- US Department of Energy, Basic Energy Sciences, Division of Materials Sciences and Engineering [DE-FG-05-05-ER46222]
- EU
- Bundesministrium fur Bildung und Forschung (Bio-H2)
- Volkswagen foundation (LigH2t)
Although a number of solar biohydrogen systems employing photosystem I (PSI) have been developed, few attain the electron transfer throughput of oxygenic photosynthesis. We have optimized a biological/organic nanoconstruct that directly tethers F-B, the terminal [4Fe-4S] cluster of PSI from Synechococcus sp. PCC 7002, to the distal [4Fe-4S] cluster of the [FeFe]-hydrogenase (H(2)ase) from Clostridium acetobutylicum. On illumination, the PSI-[FeFe]-H(2)ase nanoconstruct evolves H-2 at a rate of 2,200 +/- 460 mu mol mg chlorophyll(-1) h(-1), which is equivalent to 105 +/- 22 e(-)PSI(-1) s(-1). Cyanobacteria evolve O-2 at a rate of approximately 400 mu mol mg chlorophyll(-1) h(-1), which is equivalent to 47 e(-)PSI(-1) s(-1), given a PSI to photosystem II ratio of 1.8. The greater than twofold electron throughput by this hybrid biological/organic nanoconstruct over in vivo oxygenic photosynthesis validates the concept of tethering proteins through their redox cofactors to overcome diffusion-based rate limitations on electron transfer.
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