Mechanism of Water Delivery to the Active Site of Photosystem II along the S(2) to S(3) Transition.

The Journal of Physical Chemistry Letters
Matteo CaponeLeonardo Guidoni

Abstract

The two water molecules serving as substrate for the oxygen evolution in Photosystem II are already bound in the S2 state of the Kok-Joliot's cycle. Nevertheless, an additional water molecule is supposed to bind the cluster during the transition between the S2 and S3 states, which has been recently revealed to have the Mn4CaO5 catalytic cluster arranged in an open cubane fashion. In this Letter, by means of ab initio calculations, we investigated the possible pathways for the binding of the upcoming water molecule. Upon the four different possibilities checked in our calculations, the binding of the crystallographic water molecule, originally located nearby the Cl(-) binding site, showed the lowest activation energy barrier. Our findings therefore support the view in which the W2 hydroxyl group and the O5 oxygen act as substrates for the oxygen evolution. Within this framework the role of the open and closed Mn4CaO5 conformers is clarified as well as the exact mechanistic events occurring along the S2 to S3 transition.

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Citations

Jun 18, 2016·Photosynthesis Research·Ulrich SiggelJohannes Messinger
Jan 13, 2017·The Journal of Physical Chemistry. B·David J VinyardGary W Brudvig
Feb 23, 2017·Annual Review of Physical Chemistry·David J Vinyard, Gary W Brudvig
Oct 25, 2016·Dalton Transactions : an International Journal of Inorganic Chemistry·Vera Krewald, Dimitrios A Pantazis
Apr 3, 2019·Future Medicinal Chemistry·Jacopo SgrignaniAlessandra Magistrato
Jul 25, 2019·Chemistry : a European Journal·Aliya TychengulovaLeonardo Guidoni
Dec 7, 2019·Physical Chemistry Chemical Physics : PCCP·Shin NakamuraLeonardo Guidoni
May 7, 2020·Physical Chemistry Chemical Physics : PCCP·Casper de Lichtenberg, Johannes Messinger
Mar 27, 2020·Annual Review of Biochemistry·Nicholas CoxWolfgang Lubitz
Aug 9, 2019·Proceedings of the National Academy of Sciences of the United States of America·Maria ChrysinaNicholas Cox
Aug 22, 2018·Dalton Transactions : an International Journal of Inorganic Chemistry·Biaobiao Zhang, Licheng Sun
Sep 14, 2019·Physical Chemistry Chemical Physics : PCCP·Muhamed AminVictor Batista
May 22, 2020·Proceedings of the National Academy of Sciences of the United States of America·Mohamed IbrahimJunko Yano
Oct 9, 2020·Angewandte Chemie·Georgia ZahariouDimitrios A Pantazis
Aug 9, 2019·Biochimica Et Biophysica Acta. Bioenergetics·Keisuke Saito, Hiroshi Ishikita
Jul 22, 2021·Chemistry : a European Journal·Maria Drosou, Dimitrios A Pantazis
Mar 16, 2017·Inorganic Chemistry·Satadal PaulDimitrios A Pantazis
Jul 4, 2019·The Journal of Physical Chemistry. B·Koji OgataShinichiro Nakamura
Aug 24, 2017·Inorganic Chemistry·Matthew A StuberJohn G Brennan
Nov 16, 2019·The Journal of Physical Chemistry Letters·Manoj MandalHiroshi Ishikita
Sep 28, 2017·Journal of the American Chemical Society·Marius Retegan, Dimitrios A Pantazis

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