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• W1993231363 abstract "The synthesis of efficient water-oxidation catalysts demands insight into the only known, naturally occurring water-oxidation catalyst, the oxygen-evolving complex (OEC) of photosystem II (PSII). Understanding the water oxidation mechanism requires knowledge of where and when substrate water binds to the OEC. Mn catalase in its Mn(III)–Mn(IV) state is a protein model of the OEC’s S2 state. From 17O-labeled water exchanged into the di-μ-oxo di-Mn(III,IV) coordination sphere of Mn catalase, CW Q-band ENDOR spectroscopy revealed two distinctly different 17O signals incorporated in distinctly different time regimes. First, a signal appearing after 2 h of 17O exchange was detected with a 13.0 MHz hyperfine coupling. From similarity in the time scale of isotope incorporation and in the 17O μ-oxo hyperfine coupling of the di-μ-oxo di-Mn(III,IV) bipyridine model (Usov, O. M.; Grigoryants, V. M.; Tagore, R.; Brudvig, G. W.; Scholes, C. P.J. Am. Chem. Soc. 2007,, 129, 11886−11887), this signal was assigned to μ-oxo oxygen. EPR line broadening was obvious from this 17O μ-oxo species. Earlier exchange proceeded on the minute or faster time scale into a non-μ-oxo position, from which 17O ENDOR showed a smaller 3.8 MHz hyperfine coupling and possible quadrupole splittings, indicating a terminal water of Mn(III). Exchangeable proton/deuteron hyperfine couplings, consistent with terminal water ligation to Mn(III), also appeared. Q-band CW ENDOR from the S2 state of the OEC was obtained following multihour 17O exchange, which showed a 17O hyperfine signal with a 11 MHz hyperfine coupling, tentatively assigned as μ-oxo-17O by resemblance to the μ-oxo signals from Mn catalase and the di-μ-oxo di-Mn(III,IV) bipyridine model." @default.
• W1993231363 created "2016-06-24" @default.
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• W1993231363 date "2012-01-09" @default.
• W1993231363 modified "2023-10-16" @default.
• W1993231363 title "EPR–ENDOR Characterization of (¹⁷O, ¹H, ²H) Water in Manganese Catalase and Its Relevance to the Oxygen-Evolving Complex of Photosystem II" @default.
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• W1993231363 doi "https://doi.org/10.1021/ja203465y" @default.
• W1993231363 hasPubMedCentralId "https://www.ncbi.nlm.nih.gov/pmc/articles/3471538" @default.
• W1993231363 hasPubMedId "https://pubmed.ncbi.nlm.nih.gov/22142421" @default.
• W1993231363 hasPublicationYear "2012" @default.
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