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The modulation of the reactivity of metal oxo species by redox inactive metals has attracted much interest due to the observation of redox inactive metal effects on processes involving electron transfer both in nature (the oxygen-evolving complex of Photosystem II) and in heterogeneous catalysis (mixed-metal oxides). Studies of small-molecule models of these systems have revealed numerous instances of effects of redox inactive metals on electron- and group-transfer reactivity. However, the heterometallic species directly involved in these transformations have rarely been structurally characterized and are often generated in situ. We have previously reported the preparation and structural characterization of multiple series of heterometallic clusters based on Mn and Fe cores and described the effects of Lewis acidity of the heterometal incorporated in these complexes on cluster reduction potential. To determine the effects of Lewis acidity of redox inactive metals on group transfer reactivity in structurally well-defined complexes, we studied [MnMO], [MnMO(OH)], and [FeMO(OH)] clusters in oxygen atom transfer (OAT) reactions with phosphine substrates. The qualitative rate of OAT correlates with the Lewis acidity of the redox inactive metal, confirming that Lewis acidic metal centers can affect the chemical reactivity of metal oxo species by modulating cluster electronics.
This article was published in the following journal.
Name: Inorganic chemistry
Metal oxo species play key roles as oxidants in chemical and biological systems. Although Brønsted acids have long been known to enhance the oxidizing power of metal oxo complexes, the use of Lewis a...
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A family of soluble metal binding proteins that are involved in the intracellular transport of specific metal ions and their transfer to the appropriate metalloprotein precursor.
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Carbon-containing thiophosphonic acid compounds. Included under this heading are compounds that have carbon bound to either SULFUR atom, PHOSPHOROUS atom, or the OXYGEN atom of the SPO2 core structure.
Galactosides in which the oxygen atom linking the sugar and aglycone is replaced by a sulfur atom.
Carbon-containing thiophosphoric acid derivatives. Included under this heading are compounds that have carbon bound to either SULFUR atom, or the OXYGEN atom of the SPO3 core structure.