Abstract
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 μ 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 μ 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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Dates
Type | When |
---|---|
Created | 13 years, 8 months ago (Dec. 13, 2011, 12:15 a.m.) |
Deposited | 3 years, 4 months ago (April 14, 2022, 9:05 p.m.) |
Indexed | 2 days, 2 hours ago (Aug. 23, 2025, 1:07 a.m.) |
Issued | 13 years, 8 months ago (Dec. 12, 2011) |
Published | 13 years, 8 months ago (Dec. 12, 2011) |
Published Online | 13 years, 8 months ago (Dec. 12, 2011) |
Published Print | 13 years, 7 months ago (Dec. 27, 2011) |
@article{Lubner_2011, title={Solar hydrogen-producing bionanodevice outperforms natural photosynthesis}, volume={108}, ISSN={1091-6490}, url={http://dx.doi.org/10.1073/pnas.1114660108}, DOI={10.1073/pnas.1114660108}, number={52}, journal={Proceedings of the National Academy of Sciences}, publisher={Proceedings of the National Academy of Sciences}, author={Lubner, Carolyn E. and Applegate, Amanda M. and Knörzer, Philipp and Ganago, Alexander and Bryant, Donald A. and Happe, Thomas and Golbeck, John H.}, year={2011}, month=dec, pages={20988–20991} }