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Long-lived photoinduced charge separation in a redox system trapped in a sol–gel glass

Abstract

A KEY feature in the mechanism of photosynthesis is the initial storage of a substantial fraction of the light energy in the form of a long-lived radical pair1. In attempts to mimic this process in artificial systems2–4, impressive progress has been made in increasing the efficiency of the charge-separation reaction between an excited photosensitizer and an appropriate electron acceptor, but prevention of the energy-wasting back-reaction to neutral species still constitutes a major challenge. The back-reaction limits the length of time during which charge separation (and thus energy storage) can be maintained. Here we report exceedingly long-lived (up to a few hours) photoinduced charge separation in an artificial photosynthetic system that does not require a secondary substrate to react with the charged species. Our system uses pyrene (Py*) as the photosensitized electron donor and N,N'-dimethy 1-4,4'-bipyridinium (methyl viologen, MV2+) as the electron acceptor, both immobilized in a porous sol–gel silica glass5. The redox reaction is carried out by the mediation of a third mobile charge carrier in the intrapore space6. The spatial separation between the donor and acceptor inhibits the back-reaction to produce the long lifetimes of the charge-separated pair.

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References

  1. Antennas and Reaction Centers of Photosynthetic Bacteria (ed. Michel-Beyerle, M. E.) (Springer, Berlin, 1985).

    Google Scholar 

  2. Photoinduced Electron Transfer (eds Fox, M. A. & Chanon, M.) (Elsevier, Amsterdam, 1988).

  3. Gratzel, M. Heterogeneous Photochemical Electron Transfer (CRC, Boca Raton, 1989).

    Google Scholar 

  4. Photochemical Energy Conversion (eds Norris, J. R. & Meisel, D.).

  5. Brinker, C. J. & Scherer, G. Sol-gel Science (Academic, San Diego, 1990).

    Google Scholar 

  6. Slama-Schwok, A., Avnir, D. & Ottolenghi, M. (1991). J. Am. chem. Soc. 113, 3984–3985 (1991).

    Article  CAS  Google Scholar 

  7. Matsuo, T. J. Photochem. 29, 41–54 (1985).

    Article  CAS  Google Scholar 

  8. Adar, E., Degani, Y., Goren, Z. & Willner, I. J. Am. chem. Soc. 108, 4696–4700 (1986).

    Article  CAS  Google Scholar 

  9. Rabani, J. & Sassoon, R. E. J. Photochem. 29, 726 (1985).

    Article  Google Scholar 

  10. Margerum, L. D., Murray, R. W. & Meyer, T. J. J. phys. Chem. 90, 728–730 (1986).

    Article  CAS  Google Scholar 

  11. Moser, J., Gratzel, M. & Gallay, R. Helv. chim. Acta 70, 1596–1604 (1987).

    Article  CAS  Google Scholar 

  12. Anderson, R. F. Ber. Bunseng. Phys. Chem. 80, 969–972 (1976).

    Article  CAS  Google Scholar 

  13. Avnir, D., Ottolenghi, M. & Braun, S. in Supramolecular Architecture in Two and Three Dimensions, ACS Symp. Series (ed. Bein, T.) (American Chemical Society, in the press).

  14. Slama-Schwok, A., Avnir, D. & Ottolenghi, M. J. phys. Chem. 93, 7544–7547 (1989).

    Article  CAS  Google Scholar 

  15. Slama-Schwok, A., Avnir, D. & Ottolenghi, M. Photochem. Photobiol. 54, 525 (1991).

    Article  CAS  Google Scholar 

  16. Grellman, K. H., Watkins, A. R. & Weller, A. J. Luminesc. 1/2, 678–692 (1970).

    Article  Google Scholar 

  17. Tsakahara, K. & Wilkins, R. G. J. Am. chem. Soc. 107, 2632–2635 (1985).

    Article  Google Scholar 

  18. Ottolenghi, M. Chem. Phys. Lett. 12, 339–342 (1971).

    Article  ADS  CAS  Google Scholar 

  19. Das, P. K. J. Chem. Soc. Faraday Trans. 79, 1135–1145 (1983).

    Article  CAS  Google Scholar 

  20. Homer, R. F. & Tomlinson, T. E. J. chem. Soc. 2498 (1960).

Download references

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Slama-Schwok, A., Ottolenghi, M. & Avnir, D. Long-lived photoinduced charge separation in a redox system trapped in a sol–gel glass. Nature 355, 240–242 (1992). https://doi.org/10.1038/355240a0

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