Synergism in molybdenum iron sulphur cluster compounds. Synthetic, structural, magnetic, cyclic voltammetric evidence and the reaction of dicubane clusters containing [MoFe3S4] unit

Kang, Byeong‐Cheol; Liu, Hanqin; Cai, Jinghua; Huang, Ling; Liu, Qiutian; Wu, Daxu; Weng, Linghong; Lu, Ji-Qing

doi:10.1007/bf01092584

Cited by 6 publications

(2 citation statements)

References 31 publications

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“…The average Fe−S bond distances confirm this assignment. Published Fe−S bond distances for octahedrally coordinated iron ions with at least three sulfur ligands are found in the range 2.26−2.34 Å for ls Fe II , − 2.23−2.36 Å for ls Fe III , ,− 2.51−2.57 Å for hs Fe II , ,,,− and 2.57 Å for hs Fe III 3 Selected Average Bond Distances (Å) and Angles (deg) of the Trication [LFeCrFeL] 3+ in Crystals of 1c *, of the Trication [LFeCoFeL] 3+ in 2c , and of the Dication [LFeFeFeL] 2+ in 3b * Determined by X-ray Crystallography 1c * 2c 3b * Fe t −N 2.055(10) 2.038(3) 2.059(8) Fe t −S 2.257(3) 2.234(1) 2.236(3) M c −S 2.398(3) 2.286(1) 2.297(2) Fe t ···M c 2.941(3) 2.870(1) 2.848(2) Fe t −S−M c 78.30(10) 78.82(4) 77.81(8) …”

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confidence: 99%

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Electronic Structure of Linear Thiophenolate-Bridged Heterotrinuclear Complexes [LFeMFeL]ⁿ⁺ (M = Cr, Co, Fe; n = 1−3): Localized vs Delocalized Models

et al. 1999

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The reaction of mononuclear [LFeIII] where L represents the trianionic ligand 1,4,7-tris(4-tert-butyl-2-mercaptobenzyl)-1,4,7-triazacyclononane with CrSO4·5H2O, CoCl2·6H2O, or Fe(BF4)2·6H2O and subsequent oxidation with ferrocenium hexafluorophosphate or NO(BF4) or reduction with [(tmcn)Mo(CO)3] (tmcn = 1,4,7-trimethyl-1,4,7-triazacyclononane) produced an isostructural series of [LFeMFeL] n + complexes, the following salts of which were isolated as crystalline solids: (i) [LFeCrFeL](PF6) n with n = 1 (1a), n = 2 (1b), and n = 3 (1c); (ii) [LFeCoFeL]X n with X = BPh4 and n = 2 (2b) and X = PF6 and n = 3 (2c); (iii) [LFeFeFeL](BPh4) n with n = 2 (3b) and n = 3 (3c). All compounds contain linear trinuclear cations (face-sharing octahedral) with an N3Fe(μ-SR)3M(μ-SR)3FeN3 core structure. The electron structure of all complexes has been studied by Fe and M K-edge X-ray absorption near edge structure (XANES), UV−vis, and EPR spectroscopy, variable-temperature, variable-field susceptibility measurements, and Mössbauer spectroscopy (in zero and applied field). The following electronic structures have been established: (1a) FeII(ls)CrIIIFeII(ls) (ls = low-spin) with a spin ground state of S t = 3/2; (1c) FeIII(ls)CrIIIFeIII(ls) with an S t = 1/2 ground state; (2c) FeIII(ls)CoIII(ls)FeIII(ls) with an S t = 1 ground state; (3c) FeIII(ls)FeIII(ls)FeIII(ls) with an S t = 1/2 ground state. For 1b (S t = 2) it is found that the two iron ions are spectroscopically equivalent (Fe2.5) and, therefore, the excess electron is delocalized (class III): [LFe2.5CrIIIFe2.5L]2+. For 2b clearly two different iron sites prevail at low temperatures (4.2 K); at higher temperatures (>200 K) they become equivalent on the Mössbauer time scale. Thus, 2b is class II with temperature-dependent electron hopping between the FeII and FeIII ions. 3b is again fully delocalized (class III) with an S t = 1 ground state; the excess electron is delocalized over all three iron sites. The electronic structure of all complexes is discussed in terms of double exchange and superexchange mechanisms.

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Section: Resultsmentioning

confidence: 99%

“…2.23-2.36 Å for ls Fe III ,46,[53][54][55][56][57][58] 2.51-2.57 Å for hs Fe II ,39,41,53,[59][60][61][62][63][64] and 2.57 Å for hs Fe III 65. …”

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confidence: 99%

Electronic Structure of Linear Thiophenolate-Bridged Heterotrinuclear Complexes [LFeMFeL]ⁿ⁺ (M = Cr, Co, Fe; n = 1−3): Localized vs Delocalized Models

et al. 1999

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Chemical Modelling of the Active Site of Molybdenum—Iron Protein. Synergism of MoFe3S4 Cubane-Like Unit from Physical and Chemical Evidence

Kang¹,

Liu²,

Lu³

1992

The Nitrogen Fixation and Its Research in China

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Cobalt (iron) thiolato complexes containing the Co-ligand phosphine and reaction products of the structural fragment ML 2 L? (L = 1,2-bidentate thiolate,L?= tertiary phosphine)

Kang¹,

Chen²,

Zhou

et al. 1996

J Clust Sci

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Synergism in molybdenum iron sulphur cluster compounds. Synthetic, structural, magnetic, cyclic voltammetric evidence and the reaction of dicubane clusters containing [MoFe3S4] unit

Cited by 6 publications

References 31 publications

Electronic Structure of Linear Thiophenolate-Bridged Heterotrinuclear Complexes [LFeMFeL]ⁿ⁺ (M = Cr, Co, Fe; n = 1−3): Localized vs Delocalized Models

Electronic Structure of Linear Thiophenolate-Bridged Heterotrinuclear Complexes [LFeMFeL]ⁿ⁺ (M = Cr, Co, Fe; n = 1−3): Localized vs Delocalized Models

Chemical Modelling of the Active Site of Molybdenum—Iron Protein. Synergism of MoFe3S4 Cubane-Like Unit from Physical and Chemical Evidence

Cobalt (iron) thiolato complexes containing the Co-ligand phosphine and reaction products of the structural fragment ML 2 L? (L = 1,2-bidentate thiolate,L?= tertiary phosphine)

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Synergism in molybdenum iron sulphur cluster compounds. Synthetic, structural, magnetic, cyclic voltammetric evidence and the reaction of dicubane clusters containing [MoFe3S4] unit

Cited by 6 publications

References 31 publications

Electronic Structure of Linear Thiophenolate-Bridged Heterotrinuclear Complexes [LFeMFeL]n+ (M = Cr, Co, Fe; n = 1−3): Localized vs Delocalized Models

Electronic Structure of Linear Thiophenolate-Bridged Heterotrinuclear Complexes [LFeMFeL]n+ (M = Cr, Co, Fe; n = 1−3): Localized vs Delocalized Models

Chemical Modelling of the Active Site of Molybdenum—Iron Protein. Synergism of MoFe3S4 Cubane-Like Unit from Physical and Chemical Evidence

Cobalt (iron) thiolato complexes containing the Co-ligand phosphine and reaction products of the structural fragment ML 2 L? (L = 1,2-bidentate thiolate,L?= tertiary phosphine)

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Electronic Structure of Linear Thiophenolate-Bridged Heterotrinuclear Complexes [LFeMFeL]ⁿ⁺ (M = Cr, Co, Fe; n = 1−3): Localized vs Delocalized Models

Electronic Structure of Linear Thiophenolate-Bridged Heterotrinuclear Complexes [LFeMFeL]ⁿ⁺ (M = Cr, Co, Fe; n = 1−3): Localized vs Delocalized Models