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• W2327883945 endingPage "7928" @default.
• W2327883945 startingPage "7914" @default.
• W2327883945 abstract "The binding of the substrate analogue methanol to the catalytic Mn4CaO5 cluster of the water-oxidizing enzyme photosystem II is known to alter the electronic structure properties of the oxygen-evolving complex without retarding O2-evolution under steady-state illumination conditions. We report the binding mode of 13C-labeled methanol determined using 9.4 GHz (X-band) hyperfine sublevel-correlation (HYSCORE) and 34 GHz (Q-band) electron spin–echo electron nuclear double resonance (ESE-ENDOR) spectroscopies. These results are compared to analogous experiments on a mixed-valence Mn(III)Mn(IV) complex (2-OH-3,5-Cl2-salpn)2Mn(III)Mn(IV) (salpn = N,N′-bis(3,5-dichlorosalicylidene)-1,3-diamino-2-hydroxypropane) in which methanol ligates to the Mn(III) ion (Larson et al. (1992) J. Am. Chem. Soc., 114, 6263). In the mixed-valence Mn(III,IV) complex, the hyperfine coupling to the 13C of the bound methanol (Aiso = 0.65 MHz, T = 1.25 MHz) is appreciably larger than that observed for 13C methanol associated with the Mn4CaO5 cluster poised in the S2 state, where only a weak dipolar hyperfine interaction (Aiso = 0.05 MHz, T = 0.27 MHz) is observed. An evaluation of the 13C hyperfine interaction using the X-ray structure coordinates of the Mn4CaO5 cluster indicates that methanol does not bind as a terminal ligand to any of the manganese ions in the oxygen-evolving complex. We favor methanol binding in place of a water ligand to the Ca2+ in the Mn4CaO5 cluster or in place of one of the waters that form hydrogen bonds with the oxygen bridges of the cluster." @default.
• W2327883945 created "2016-06-24" @default.
• W2327883945 creator A5004809017 @default.
• W2327883945 creator A5019706721 @default.
• W2327883945 creator A5027572501 @default.
• W2327883945 creator A5073169777 @default.
• W2327883945 creator A5084987684 @default.
• W2327883945 creator A5086254191 @default.
• W2327883945 date "2014-12-11" @default.
• W2327883945 modified "2023-10-10" @default.
• W2327883945 title "Pulse Electron Paramagnetic Resonance Studies of the Interaction of Methanol with the S₂ State of the Mn₄O₅Ca Cluster of Photosystem II" @default.
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