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• W2077604889 startingPage "14373" @default.
• W2077604889 abstract "Synthetic model compounds have been targeted to benchmark and better understand the electronic structure, geometry, spectroscopy, and reactivity of the oxygen-evolving complex (OEC) of photosystem II, a low-symmetry Mn4CaOn cluster. Herein, low-symmetry Mn(IV)3GdO4 and Mn(IV)3CaO4 cubanes are synthesized in a rational, stepwise fashion through desymmetrization by ligand substitution, causing significant cubane distortions. As a result of increased electron richness and desymmetrization, a specific μ3-oxo moiety of the Mn3CaO4 unit becomes more basic allowing for selective protonation. Coordination of a fifth metal ion, Ag(+), to the same site gives a Mn3CaAgO4 cluster that models the topology of the OEC by displaying both a cubane motif and a dangler transition metal. The present synthetic strategy provides a rational roadmap for accessing more accurate models of the biological catalyst." @default.
• W2077604889 created "2016-06-24" @default.
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• W2077604889 date "2014-10-03" @default.
• W2077604889 modified "2023-10-16" @default.
• W2077604889 title "Toward Models for the Full Oxygen-Evolving Complex of Photosystem II by Ligand Coordination To Lower the Symmetry of the Mn₃CaO₄ Cubane: Demonstration That Electronic Effects Facilitate Binding of a Fifth Metal" @default.
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• W2077604889 doi "https://doi.org/10.1021/ja508160x" @default.
• W2077604889 hasPubMedCentralId "https://www.ncbi.nlm.nih.gov/pmc/articles/4210109" @default.
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