Sequential oxidation of the cubane [4Fe--4S] cluster from [4Fe--4S](-) to [4Fe--4S](3+) in Fe(4)S(4)L(n)(-) complexes

Journal of the American Chemical Society
Hua-Jin ZhaiLai-Sheng Wang

Abstract

Gaseous Fe(4)S(n)(-) (n = 4-6) clusters and synthetic analogue complexes, Fe(4)S(4)L(n)(-) (L = Cl, Br, I; n = 1-4), were produced by laser vaporization of a solid Fe/S target and electrospray from solution samples, respectively, and their electronic structures were probed by photoelectron spectroscopy. Low binding energy features derived from minority-spin Fe 3d electrons were clearly distinguished from S-derived bands. We showed that the electronic structure of the simplest Fe(4)S(4)(-) cubane cluster can be described by the two-layer spin-coupling model previously developed for the [4Fe] cubane analogues. The photoelectron data revealed that each extra S atom in Fe(4)S(5)(-) and Fe(4)S(6)(-) removes two minority-spin Fe 3d electrons from the [4Fe--4S] cubane core and each halogen ligand removes one Fe 3d electron from the cubane core in the Fe(4)S(4)L(n)(-) complexes, clearly revealing a behavior of sequential oxidation of the cubane over five formal oxidation states: [4Fe--4S](-) --> [4Fe--4S](0) --> [4Fe--4S](+) --> [4Fe-4S](2+) --> [4Fe-4S](3+). The current work shows the electron-storage capability of the [4Fe--4S] cubane, contributes to the understanding of its electronic structure, and further demonstrates the robustne...Continue Reading

References

Feb 19, 2002·Chemical Reviews·Hiroshi OginoHiromi Tobita
Oct 26, 2002·Physical Review Letters·Xin YangLai-Sheng Wang
Feb 13, 2003·Journal of the American Chemical Society·Rhonda A TorresDavid A Case

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Citations

Apr 22, 2009·The Journal of Physical Chemistry. a·Shuqiang Niu, Toshiko Ichiye
May 22, 2013·Journal of Biological Inorganic Chemistry : JBIC : a Publication of the Society of Biological Inorganic Chemistry·Bradley Scott Perrin, Toshiko Ichiye
Nov 2, 2012·Journal of Computational Chemistry·Bradley Scott PerrinToshiko Ichiye

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