ArticleProceedings of the National Academy of Sciences of the United States of America2015
High-spin Mn-oxo complexes and their relevance to the oxygen-evolving complex within photosystem II.
Article in Proceedings of the National Academy of Sciences of the United States of America, 2015. The graph could read no effect estimate from its abstract, so it casts no vote on the map. Cited by 38 papers.
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38 citing papers in PubMed.
- Selective Electrosynthesis of High-Concentration MnAngewandte Chemie (International ed. in English) · 2026Article
- Steric Mapping, Ligand Dynamics, and Cycloisomerization Catalysis with Redox Robust MnOrganometallics · 2026Article
- Formation and Reactivity of an Elusive Monomeric Mn(IV)-Oxo Species Inside a Cavitand Pore.Journal of the American Chemical Society · 2025Article
- High-Spin Manganese(V) in an Active Center Analogue of the Oxygen-Evolving Complex.Journal of the American Chemical Society · 2025Article
- Structure Function Studies of Photosystem II Using X-Ray Free Electron Lasers.Annual review of biophysics · 2024Review
- Identification, Characterization, and Electronic Structures of Interconvertible Cobalt-Oxygen TAML Intermediates.Journal of the American Chemical Society · 2024Article
- Accessing a synthetic FeChemical science · 2024Article
- Formation of a Reactive [Mn(III)-O-Ce(IV)] Species and its Facile Equilibrium with Related Mn(IV)(OX) (X = Sc or H) Complexes.Angewandte Chemie (International ed. in English) · 2024Article
- CaMnAngewandte Chemie (International ed. in English) · 2021Article
- Arrested Substrate Binding Resolves Catalytic Intermediates in Higher-Plant Water Oxidation.Angewandte Chemie (International ed. in English) · 2021Article
- Spectroscopic capture of a low-spin Mn(IV)-oxo species in Ni-MnNature communications · 2020Article
- Oxoiron(v) mediated selective electrochemical oxygenation of unactivated C-H and C[double bond, length as m-dash]C bonds using water as the oxygen source.Chemical science · 2020Article
- Concerted proton-electron transfer reactions of manganese-hydroxo and manganese-oxo complexes.Chemical communications (Cambridge, England) · 2020Article
- Article
- Investigation of structural, electronic and magnetic properties of breathing metal-organic framework MIL-47(Mn): a first principles approach.RSC advances · 2020Article
- How Metal Ion Lewis Acidity and Steric Properties Influence the Barrier to Dioxygen Binding, Peroxo O-O Bond Cleavage, and Reactivity.Journal of the American Chemical Society · 2019Article
- Electrochemical C-H oxygenation and alcohol dehydrogenation involving Fe-oxo species using water as the oxygen source.Chemical science · 2019Article
- Regulating the Basicity of Metal-Oxido Complexes with a Single Hydrogen Bond and Its Effect on C-H Bond Cleavage.Journal of the American Chemical Society · 2019Article
- A Terminal FeJournal of the American Chemical Society · 2019Article
- Low overpotential water oxidation at neutral pH catalyzed by a copper(ii) porphyrin.Chemical science · 2019Article
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Abstract
The structural and electronic properties of a series of manganese complexes with terminal oxido ligands are described. The complexes span three different oxidation states at the manganese center (III-V), have similar molecular structures, and contain intramolecular hydrogen-bonding networks surrounding the Mn-oxo unit. Structural studies using X-ray absorption methods indicated that each complex is mononuclear and that oxidation occurs at the manganese centers, which is also supported by electron paramagnetic resonance (EPR) studies. This gives a high-spin Mn(V)-oxo complex and not a Mn(IV)-oxy radical as the most oxidized species. In addition, the EPR findings demonstrated that the Fermi contact term could experimentally substantiate the oxidation states at the manganese centers and the covalency in the metal-ligand bonding. Oxygen-17-labeled samples were used to determine spin density within the Mn-oxo unit, with the greatest delocalization occurring within the Mn(V)-oxo species (0.45 spins on the oxido ligand). The experimental results coupled with density functional theory studies show a large amount of covalency within the Mn-oxo bonds. Finally, these results are examined within the context of possible mechanisms associated with photosynthetic water oxidation; specifically, the possible identity of the proposed high valent Mn-oxo species that is postulated to form during turnover is discussed.
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