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Boas, John F.
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article
Stabilization of Low-Valent Iron(I) in a High-Valent Vanadium(V) Oxide Cluster
Abstract
<p>Low-valent iron centers are critical intermediates in chemical and bio-chemical processes. Herein, we show the first example of a low-valent Fe<sup>I</sup> center stabilized in a high-valent polyoxometalate framework. Electrochemical studies show that the Fe<sup>III</sup>-functionalized molecular vanadium(V) oxide (DMA)[Fe<sup>III</sup>ClV<sup>V</sup> <sub>12</sub>O<sub>32</sub>Cl]<sup>3−</sup> (DMA=dimethylammonium) features two well-defined, reversible, iron-based electrochemical reductions which cleanly yield the Fe<sup>I</sup> species (DMA)[Fe<sup>I</sup>ClV<sup>V</sup> <sub>12</sub>O<sub>32</sub>Cl]<sup>5−</sup>. Experimental and theoretical studies including electron paramagnetic resonance spectroscopy and density functional theory computations verify the formation of the Fe<sup>I</sup> species. The study presents the first example for the seemingly paradoxical embedding of low-valent metal species in high-valent metal oxide anions and opens new avenues for reductive electron transfer catalysis by polyoxometalates.</p>