Three-Coordinate Terminal Imidoiron(III) Complexes: Structure, Spectroscopy, and Mechanism of Formation

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Article discussing three-coordinate terminal imidoiron(III) complexes and the structure, spectroscopy, and the mechanism of formation.

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43 p.: ill.

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Cowley, Ryan E.; DeYonker, Nathan J.; Eckert, Nathan A.; Cundari, Thomas R., 1964-; DeBeer, Serena 1973-; Bill, E. (Eckhard), 1953- et al. 2010.

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Article discussing three-coordinate terminal imidoiron(III) complexes and the structure, spectroscopy, and the mechanism of formation.

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43 p.: ill.

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Reprinted with permission from the Journal of Chemical and Engineering Data. Copyright 2009 American Chemical Society.

Abstract: Reaction of 1-adamantyl azide with iron(I) diketiminate precursors gives metastable but isolable imidoiron(III) complexes LFe=NAd (L = bulky β-diketiminate ligand; AD = 1-adamantyl). This paper addresses: (1) the spectroscopic and structural characterization of the Fe=N multiple bond in these interesting three-coordinate iron imido complexes, and (2) the mechanism through which the imido complexes form. The iron(III) imido complexes have been examined by ¹HNMR and EPR spectroscopies and temperature-dependent magnetic susceptibility (SQUID), and structurally characterized by crystallography and/or X-ray absorption (EXAFS) measurements. These data show that the imido complexes have quartet ground states and short (1.68 ± 0.01 Å) iron-nitrogen bonds. The formation of the imido complexes proceeds through unobserved iron-RN₃ intermediates, which are indicated by QM/MM computations to be best described as iron (II) with an RN₃ radical anion. The radical character on the organoazide bends its NNN linkage to enable easy N₂ loss and imido complex formation. The product distribution between imidoiron(III) products and hexazene-bridged diiron(II) products is solvent-dependent, and the solvent dependence can be explained by coordination of certain solvents to the iron(I) precursor prior to interaction with the organoazide.

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  • Inorganic Chemistry, 2010, Washington DC: American Chemical Society, pp. 6172-6187

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  • Publication Title: Inorganic Chemistry
  • Volume: 49
  • Issue: 13
  • Page Start: 6172
  • Page End: 6187
  • Peer Reviewed: Yes

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  • 2010

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  • Sept. 6, 2013, 3:22 p.m.

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  • May 27, 2014, 2:42 p.m.

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Cowley, Ryan E.; DeYonker, Nathan J.; Eckert, Nathan A.; Cundari, Thomas R., 1964-; DeBeer, Serena 1973-; Bill, E. (Eckhard), 1953- et al. Three-Coordinate Terminal Imidoiron(III) Complexes: Structure, Spectroscopy, and Mechanism of Formation, article, 2010; [Washington, D.C.]. (digital.library.unt.edu/ark:/67531/metadc180963/: accessed October 22, 2017), University of North Texas Libraries, Digital Library, digital.library.unt.edu; crediting UNT College of Arts and Sciences.