Reactive oxygen species leave a damage trail that reveals water channels in Photosystem II
Abstract
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
- Authors:
-
- Washington Univ., St. Louis, MO (United States)
- Publication Date:
- Research Org.:
- Washington Univ., St. Louis, MO (United States); Energy Frontier Research Centers (EFRC) (United States). Photosynthetic Antenna Research Center (PARC)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Chemical Sciences, Geosciences & Biosciences Division
- OSTI Identifier:
- 1499939
- Grant/Contract Number:
- FG02-99ER20350; SC0001035
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Science Advances
- Additional Journal Information:
- Journal Volume: 3; Journal Issue: 11; Journal ID: ISSN 2375-2548
- Publisher:
- AAAS
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 59 BASIC BIOLOGICAL SCIENCES; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Citation Formats
Weisz, Daniel A., Gross, Michael L., and Pakrasi, Himadri B. Reactive oxygen species leave a damage trail that reveals water channels in Photosystem II. United States: N. p., 2017.
Web. doi:10.1126/sciadv.aao3013.
Weisz, Daniel A., Gross, Michael L., & Pakrasi, Himadri B. Reactive oxygen species leave a damage trail that reveals water channels in Photosystem II. United States. doi:10.1126/sciadv.aao3013.
Weisz, Daniel A., Gross, Michael L., and Pakrasi, Himadri B. Fri .
"Reactive oxygen species leave a damage trail that reveals water channels in Photosystem II". United States. doi:10.1126/sciadv.aao3013. https://www.osti.gov/servlets/purl/1499939.
@article{osti_1499939,
title = {Reactive oxygen species leave a damage trail that reveals water channels in Photosystem II},
author = {Weisz, Daniel A. and Gross, Michael L. and Pakrasi, Himadri B.},
abstractNote = {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},
doi = {10.1126/sciadv.aao3013},
journal = {Science Advances},
number = 11,
volume = 3,
place = {United States},
year = {2017},
month = {11}
}
Web of Science
Figures / Tables:

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