Substrate–water exchange in photosystem II is arrested before dioxygen formation

Håkan Nilsson, Fabrice Rappaport, Alain Boussac () and Johannes Messinger ()
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Håkan Nilsson: Kemiskt Biologiskt Centrum (KBC), Umeå University
Fabrice Rappaport: Institut de Biologie Physico-Chimique, UMR 7141 CNRS and Université Pierre et Marie Curie
Alain Boussac: iBiTec-S, CNRS UMR 8221, CEA Saclay
Johannes Messinger: Kemiskt Biologiskt Centrum (KBC), Umeå University

Nature Communications, 2014, vol. 5, issue 1, 1-7

Abstract: Abstract Light-driven oxidation of water into dioxygen, catalysed by the oxygen-evolving complex (OEC) in photosystem II, is essential for life on Earth and provides the blueprint for devices for producing fuel from sunlight. Although the structure of the OEC is known at atomic level for its dark-stable state, the mechanism by which water is oxidized remains unsettled. Important mechanistic information was gained in the past two decades by mass spectrometric studies of the H218O/H216O substrate–water exchange in the four (semi) stable redox states of the OEC. However, until now such data were not attainable in the transient states formed immediately before the O–O bond formation. Using modified photosystem II complexes displaying up to 40-fold slower O2 production rates, we show here that in the transient state the substrate–water exchange is dramatically slowed as compared with the earlier S states. This further constrains the possible sites for substrate–water binding in photosystem II.

Date: 2014
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DOI: 10.1038/ncomms5305

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