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Absence of Mn-Centered Oxidation in the S2→ S3Transition: Implications for the Mechanism of Photosynthetic Water Oxidation
Open accessAbstract
A key question for the understanding of photosynthetic water oxidation is whether the four oxidizing equivalents necessary to oxidize water to dioxygen are accumulated on the four Mn ions of the oxygen-evolving complex (OEC), or whether some ligand-centered oxidations take place before the formation and release of dioxygen during the S(3) --> [S(4)] --> S(0) transition. Progress in instrumentation and flash sample preparation allowed us to apply Mn Kbeta X-ray emission spectroscopy (Kbeta XES) to this problem for the first time. The Kbeta XES results, in combination with Mn X-ray absorption near-edge structure (XANES) and electron paramagnetic resonance (EPR) data obtained from the same set of samples, show that the S(2) --> S(3) transition, in contrast to the S(0) --> S(1) and S(1) --> S(2) transitions, does not involve a Mn-centered oxidation. On the basis of new structural data from the S(3)-state, manganese mu-oxo bridge radical formation is proposed for the S(2) --> S(3) transition, and three possible mechanisms for the O-O bond formation are presented.
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Citations
Cited by
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
Proton-coupled electron transfer
Huynh, M. H. V., & Meyer, T. J. (2007) · Chemical Reviews · doi:10.1021/cr0500030 · Cited by 1,659
Structures and Energetics for O2 Formation in Photosystem II
Siegbahn, P. E. M. (2009) · Accounts of Chemical Research · doi:10.1021/ar900117k · Cited by 521
Zaharieva, I., Najafpour, M. M., Wiechen, M., Haumann, M., Kurz, P., & Dau, H. (2011) · Energy & Environmental Science · doi:10.1039/c0ee00815j · Cited by 276
Metadata
- Authors
- Messinger, J., Robblee, J. H., Bergmann, U., Fernandez, C., Glatzel, P., Visser, H., Cinco, R. M., McFarlane, K. L., Bellacchio, E., Pizarro, S. A., Cramer, S. P., Sauer, K., Klein, M. P., & Yachandra, V. K.
- Venue
- Journal of the American Chemical Society
- Publisher
- American Chemical Society (ACS)
- Published
- 2001-07-20
- Volume
- 123
- Issue
- 32
- Pages
- 7804-7820
- ISSN
- 0002-7863 (ISSN-L)
- 1520-5126
- OpenAlex
- W1987946602
- Cited by
- 304
- References
- 0
- FWCI
- 4.78
- Type
- journal article
- Language
- en
- Open access
- green
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- Messinger, J., Robblee, J. H., Bergmann, U., Fernandez, C., Glatzel, P., Visser, H., Cinco, R. M., McFarlane, K. L., Bellacchio, E., Pizarro, S. A., Cramer, S. P., Sauer, K., Klein, M. P., & Yachandra, V. K. (2001). Absence of Mn-Centered Oxidation in the S2→ S3Transition: Implications for the Mechanism of Photosynthetic Water Oxidation. Journal of the American Chemical Society. https://doi.org/10.1021/ja004307%2B
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Bibliographic data: Semantic Scholar, OpenAlex, Crossref.
Contains information from the Semantic Scholar Academic Graph Datasets, made available under the ODC Attribution License (ODC-BY 1.0).
Semantic Scholar’s data is described in: Kinney, R., et al. (2023). The Semantic Scholar Open Data Platform. arXiv:2301.10140.
