Detection of the Water-Binding Sites of the Oxygen-Evolving Complex of Photosystem II Using W-Band 17O Electron–Electron Double Resonance-Detected NMR Spectroscopy
作者： Leonid Rapatskiy , Nicholas Cox , Anton Savitsky , William M. Ames , Julia Sander
DOI: 10.1021/JA3053267
关键词: Electron paramagnetic resonance 、 Water binding 、 Hyperfine structure 、 Oxygen-evolving complex 、 Crystallography 、 Nuclear magnetic resonance spectroscopy 、 Crystal structure 、 Analytical chemistry 、 Chemistry 、 Photosystem II 、 Spectroscopy
摘要: Water binding to the Mn4O5Ca cluster of oxygen-evolving complex (OEC) Photosystem II (PSII) poised in S2 state was studied via H217O- and 2H2O-labeling high-field electron paramagnetic resonance (EPR) spectroscopy. Hyperfine couplings coordinating 17O (I = 5/2) nuclei were detected using W-band (94 GHz) electron–electron double (ELDOR) NMR Davies/Mims electron–nuclear (ENDOR) techniques. Universal 15N 1/2) labeling employed clearly discriminate hyperfine that overlap with 14N 1) signals from D1-His332 ligand OEC (StichBiochemistry 2011, 50 (34), 7390−7404). Three classes identified: (i) one μ-oxo bridge; (ii) a terminal Mn–OH/OH2 ligand; (iii) Mn/Ca–H2O ligand(s). These assignments are based on model data, comparison recent 1.9 A resolution PSII crystal structure (UmenaNature 473, 55−60), NH3 perturbation signal envelope density functi...
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