Rationalizing the Geometries of the Water Oxidising Complex in the Atomic Resolution, Nominal S3 State Crystal Structures of Photosystem II

Chemphyschem : a European Journal of Chemical Physics and Physical Chemistry
Simon PetrieRon J Pace

Abstract

Three atomic resolution crystal structures of Photosystem II, in the double flashed, nominal S3 intermediate state of its Mn4 Ca Water Oxidising Complex (WOC), have now been presented, at 2.25, 2.35 and 2.08 Å resolution. Although very similar overall, the S3 structures differ within the WOC catalytic site. The 2.25 Å structure contains only one oxy species (O5) in the WOC cavity, weakly associated with Mn centres, similar to that in the earlier 1.95 Å S1 structure. The 2.35 Å structure shows two such species (O5, O6), with the Mn centres and O5 positioned as in the 2.25 Å structure and O5-O6 separation of ∼1.5 Å. In the latest S3 variant, two oxy species are also seen (O5, Ox), with the Ox group appearing only in S3 , closely ligating one Mn, with O5-Ox separation <2.1 Å. The O5 and O6/Ox groups were proposed to be substrate water derived species. Recently, Petrie et al. (Chem. Phys. Chem., 2017) presented large scale Quantum Chemical modelling of the 2.25 Å structure, quantitatively explaining all significant features within the WOC region. This, as in our earlier studies, assumed a 'low' Mn oxidation paradigm (mean S1 Mn oxidation level of +3.0, Petrie et al., Angew. Chem. Int. Ed., 2015), rather than a 'high' oxidation mode...Continue Reading

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Citations

Apr 22, 2021·The Journal of Physical Chemistry Letters·Manoj MandalHiroshi Ishikita
Jun 3, 2021·Molecules : a Journal of Synthetic Chemistry and Natural Product Chemistry·Bernard Baituti, Sebusi Odisitse
Nov 20, 2020·The Journal of Physical Chemistry Letters·Manoj MandalHiroshi Ishikita

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