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Photosynthetic O 2 Formation Tracked by Time-Resolved X-ray Experiments
Abstract
Plants and cyanobacteria produce atmospheric dioxygen from water, powered by sunlight and catalyzed by a manganese complex in photosystem II. A classic S-cycle model for oxygen evolution involves five states, but only four have been identified. The missing S 4 state is particularly important because it is directly involved in dioxygen formation. Now progress comes from an x-ray technique that can monitor redox and structural changes in metal centers in real time with 10-microsecond resolution. We show that in the O 2 -formation step, an intermediate is formed—the enigmatic S 4 state. Its creation is identified with a deprotonation process rather than the expected electron-transfer mechanism. Subsequent electron transfer would give an additional S 4 ′ state, thus extending the fundamental S-state cycle of dioxygen formation.
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Cited by
Toward the rational design of non-precious transition metal oxides for oxygen electrocatalysis
Hong, W. T., Risch, M., Stoerzinger, K. A., Grimaud, A., Suntivich, J., & Shao-Horn, Y. (2015) · Energy & Environmental Science · doi:10.1039/c4ee03869j · Cited by 2,089
The Mechanism of Water Oxidation: From Electrolysis via Homogeneous to Biological Catalysis
Dau, H., Limberg, C., Reier, T., Risch, M., Roggan, S., & Strasser, P. (2010) · ChemCatChem · doi:10.1002/cctc.201000126 · Cited by 1,783
Self-citationProton-coupled electron transfer
Huynh, M. H. V., & Meyer, T. J. (2007) · Chemical Reviews · doi:10.1021/cr0500030 · Cited by 1,659
The ultrafast X-ray spectroscopic revolution in chemical dynamics
Kraus, P. M., Zürch, M., Cushing, S. K., Neumark, D. M., & Leone, S. R. (2018) · Nature Reviews Chemistry · doi:10.1038/s41570-018-0008-8 · Cited by 336
Lananan, F., Abdul Hamid, S. H., Din, W. N. S., Ali, N., Khatoon, H., Jusoh, A., & Endut, A. (2014) · International Biodeterioration & Biodegradation · doi:10.1016/j.ibiod.2014.06.013 · Cited by 183
Metadata
- Authors
- Haumann, M., Liebisch, P., Müller, C., Barra, M., Grabolle, M., & Dau, H.
- Venue
- Science
- Published
- 2005-11-11
- Volume
- 310
- Issue
- 5750
- Pages
- 1019-1021
- ISSN
- 0036-8075 (ISSN-L)
- 1095-9203
- OpenAlex
- W1996917852
- Cited by
- 461
- References
- 0
- FWCI
- 11.87
- Type
- journal article
- Language
- en
- Open access
- closed
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- Haumann, M., Liebisch, P., Müller, C., Barra, M., Grabolle, M., & Dau, H. (2005). Photosynthetic O 2 Formation Tracked by Time-Resolved X-ray Experiments. Science. https://doi.org/10.1126/science.1117551
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