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

作者：Nilsson Hakan; Rappaport Fabrice; Boussac Alain^*; Messinger Johannes

来源：Nature Communications, 2014, 5(1): 4305.

DOI：10.1038/ncomms5305

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 (H2O)-O-18/(H2O)-O-16 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 O-2 production rates, we show here that in the transient S3YZ 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.

• 出版日期2014-7
• 单位中国地震局