Journal
BIOCHEMISTRY
Volume 54, Issue 38, Pages 5783-5786Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.biochem.5b00974
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- U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences, and Biosciences [DESC0001423, DE-FG0205ER15646]
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Ammonia binds directly to the oxygen-evolving complex of photosystem II (PSII) upon formation of the S-2 intermediate, as evidenced by electron paramagnetic resonance spectroscopy. We explore the binding mode by using quantum mechanics/molecular mechanics methods and simulations of extended X-ray absorption fine structure spectra. We find that NH3 binds as an additional terminal ligand to the dangling Mn4, instead of exchanging with terminal water. Because water and ammonia are electronic and structural analogues, these findings suggest that water binds analogously during the S-2 -> S-3 transition, leading to rearrangement of ligands in a carrousel around Mn4.
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