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Title: Reactive oxygen species leave a damage trail that reveals water channels in Photosystem II

Journal Article · · Science Advances

Photosystem II (PSII), a unique membrane-bound oxidoreductase, catalyzes light-driven oxidation of water to molecular oxygen. Although high-resolution structures of PSII are known, the exact path of the substrate water molecules to the catalytic Mn4CaO5 center within the PSII complex remains poorly understood. PSII produces reactive oxygen species (ROS), responsible for the frequent damage and turnover of this megacomplex that occur under physiological conditions. Such ROS are known to specifically modify PSII proteins. Using high-resolution tandem mass spectrometry, we identified oxidative modifications on 36 amino acid residues on the lumenal side of PSII, in the core PSII proteins D1, D2, and CP43 of the cyanobacterium Synechocystis sp. PCC 6803. Remarkably, these oxidized residues clustered into three nearly continuous formations, tracking the pathways of ROS diffusion from the manganese center all the way out to the surface of PSII. We suggest that these profiles of oxidized residues reveal the locations of water channels within PSII. Our results provide the most comprehensive experimental evidence to date of physiologically relevant oxidized residues in PSII and illuminate three possible channels for water between the catalytic Mn cluster in the PSII complex and the bulk medium around it

Research Organization:
Washington Univ., St. Louis, MO (United States); Energy Frontier Research Centers (EFRC) (United States). Photosynthetic Antenna Research Center (PARC)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences, and Biosciences Division
Grant/Contract Number:
FG02-99ER20350; SC0001035
OSTI ID:
1499939
Journal Information:
Science Advances, Vol. 3, Issue 11; ISSN 2375-2548
Publisher:
AAASCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 25 works
Citation information provided by
Web of Science

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Cited By (6)

Physiological response of the toxic and non-toxic strains of a bloom-forming cyanobacterium Microcystis aeruginosa to changing ultraviolet radiation regimes journal February 2019
Natively oxidized amino acid residues in the spinach cytochrome b 6 f complex journal January 2018
Natively oxidized amino acid residues in the spinach PS I-LHC I supercomplex journal January 2020
A novel chlorophyll protein complex in the repair cycle of photosystem II journal October 2019
Metabolic Reprogramming in Chloroplasts under Heat Stress in Plants journal March 2018
Characterization of Protein Radicals in Arabidopsis journal August 2019

Figures / Tables (6)