Versatile reactivity of a solvent-coordinated diiron(II) compound: synthesis and dioxygen reactivity of a mixed-valent Fe(II)Fe(III) species

Inorganic Chemistry
Amit MajumdarStephen J Lippard

Abstract

A new, DMF-coordinated, preorganized diiron compound [Fe2(N-Et-HPTB)(DMF)4](BF4)3 (1) was synthesized, avoiding the formation of [Fe(N-Et-HPTB)](BF4)2 (10) and [Fe2(N-Et-HPTB)(μ-MeCONH)](BF4)2 (11), where N-Et-HPTB is the anion of N,N,N',N'-tetrakis[2-(1-ethylbenzimidazolyl)]-2-hydroxy-1,3-diaminopropane. Compound 1 is a versatile reactant from which nine new compounds have been generated. Transformations include solvent exchange to yield [Fe2(N-Et-HPTB)(MeCN)4](BF4)3 (2), substitution to afford [Fe2(N-Et-HPTB)(μ-RCOO)](BF4)2 (3, R = Ph; 4, RCOO = 4-methyl-2,6-diphenyl benzoate]), one-electron oxidation by (Cp2Fe)(BF4) to yield a Robin-Day class II mixed-valent diiron(II,III) compound, [Fe2(N-Et-HPTB)(μ-PhCOO)(DMF)2](BF4)3 (5), two-electron oxidation with tris(4-bromophenyl)aminium hexachloroantimonate to generate [Fe2(N-Et-HPTB)Cl3(DMF)](BF4)2 (6), reaction with (2,2,6,6-tetramethylpiperidin-1-yl)oxyl to form [Fe5(N-Et-HPTB)2(μ-OH)4(μ-O)(DMF)2](BF4)4 (7), and reaction with dioxygen to yield an unstable peroxo compound that decomposes at room temperature to generate [Fe4(N-Et-HPTB)2(μ-O)3(H2O)2](BF4)·8DMF (8) and [Fe4(N-Et-HPTB)2(μ-O)4](BF4)2 (9). Compound 5 loses its bridging benzoate ligand upon further oxidation to form [Fe2...Continue Reading

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Citations

Jul 6, 2016·Journal of Biological Inorganic Chemistry : JBIC : a Publication of the Society of Biological Inorganic Chemistry·Andrew J JasniewskiLawrence Que
Mar 24, 2016·Dalton Transactions : an International Journal of Inorganic Chemistry·Yuji MikataShin-Ichiro Sato
Jan 17, 2019·Dalton Transactions : an International Journal of Inorganic Chemistry·Nabhendu Pal, Amit Majumdar
Sep 4, 2015·Acta Crystallographica. Section D, Biological Crystallography·Cecilia PozziStefano Mangani
Aug 11, 2021·Chemical Communications : Chem Comm·Nabhendu PalAmit Majumdar
Mar 14, 2020·Journal of the American Chemical Society·Manish JanaAmit Majumdar
May 29, 2019·Inorganic Chemistry·Suman K BarmanRabindranath Mukherjee
Aug 4, 2021·Chemistry : a European Journal·Silvia CiambellottiCecilia Pozzi

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