Unusual Fe9 and Fe18 structural types from the use of 2,6-pyridinedimethanol in FeIII cluster chemistry

作者: Taketo Taguchi , Michael S. Thompson , Khalil A. Abboud , George Christou

DOI: 10.1039/C0DT00635A

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摘要: The syntheses, crystal structures and magnetochemical characterization are reported for two new FeIII complexes [Fe18O6(OH)8(pdm)10(pdmH)4(H2O)4](ClO4)10 (3) [Fe9O4(OH)2(O2CMe)10(pdm)(pdmH)4](NO3) (4). They were synthesized from the use of potentially O,N,O tridentate chelate, 2,6-pyridinedimethanol (pdmH2), in presence or absence carboxylate groups. Octadecanuclear complex 3 was obtained during reactivity studies on previously-reported [Fe8O3(OEt)(pdm)4(pdmH)4(EtOH)2](ClO4)5 (2), latter undergoing hydrolysis to recrystallization undried MeCN. reaction pdmH2 with preformed [Fe3O(O2CMe)6(py)3](NO3) CH2Cl2 gave enneanuclear 4. Both 4 unprecedented structural types. core comprises a central [Fe4O6] defective-dicubane attached either side [Fe7O11] unit, which can be described as [Fe4(μ4-O)] tetrahedra fused at common Fe atom. considered four vertex-fused triangular [Fe3(μ3-O)] units. Variable-temperature (T) -field (H) solid-state dc ac magnetization (M) carried out 1.8–300 K range. Analysis data revealed that possess an S = 5/2 ground state spin, respectively.

参考文章(80)
Craig A. Grapperhaus, Martin G. O’Toole, Mark S. Mashuta, Synthesis and structure of the tetradeca-iron(III) oxide–alkoxide cluster [Bu4N]2[Fe14O8(OCH2CH3)20Cl8] Inorganic Chemistry Communications. ,vol. 9, pp. 1204- 1206 ,(2006) , 10.1016/J.INOCHE.2006.07.027
B. Xu, N.D. Chasteen, Iron oxidation chemistry in ferritin. Increasing Fe/O2 stoichiometry during core formation. Journal of Biological Chemistry. ,vol. 266, pp. 19965- 19970 ,(1991) , 10.1016/S0021-9258(18)54877-8
E. K. Brechin, E. C. Sañudo, W. Wernsdorfer, C. Boskovic, J. Yoo, D. N. Hendrickson, A. Yamaguchi, H. Ishimoto, T. E. Concolino, A. L. Rheingold, G. Christou, Single-Molecule Magnets:  Structure and Properties of [Mn18O14(O2CMe)18(hep)4(hepH)2(H2O)2](ClO4)2with SpinS= 13 Inorganic Chemistry. ,vol. 44, pp. 502- 511 ,(2005) , 10.1021/IC048857A
Hitoshi Miyasaka, Kazuya Nakata, Lollita Lecren, Claude Coulon, Yasuhiro Nakazawa, Tatsuya Fujisaki, Ken-ichi Sugiura, Masahiro Yamashita, Rodolphe Clérac, Two-dimensional networks based on Mn4 complex linked by dicyanamide anion: from single-molecule magnet to classical magnet behavior. Journal of the American Chemical Society. ,vol. 128, pp. 3770- 3783 ,(2006) , 10.1021/JA0574062
Hong-Chang Yao, Jun-Jie Wang, Yun-Sheng Ma, Oliver Waldmann, Wen-Xin Du, You Song, Yi-Zhi Li, Li-Min Zheng, Silvio Decurtins, Xin-Quan Xin, An iron(III) phosphonate cluster containing a nonanuclear ring Chemical Communications. pp. 1745- 1747 ,(2006) , 10.1039/B600763E
Taketo Taguchi, Theocharis C. Stamatatos, Khalil A. Abboud, Candace M. Jones, Katye M. Poole, Ted A. O’Brien, George Christou, New Fe4, Fe6, and Fe8 clusters of iron(III) from the use of 2-pyridyl alcohols: structural, magnetic, and computational characterization. Inorganic Chemistry. ,vol. 47, pp. 4095- 4108 ,(2008) , 10.1021/IC701756P
Simon Parsons, Gregory A. Solan, Richard E. P. Winpenny, Synthesis, structure and preliminary magnetic studies of a heptadecanuclear iron complex Journal of the Chemical Society, Chemical Communications. pp. 1987- 1988 ,(1995) , 10.1039/C39950001987
Guy W. Powell, Hannah N. Lancashire, Euan K. Brechin, David Collison, Sarah L. Heath, Talal Mallah, Wolfgang Wernsdorfer, Building molecular minerals: All ferric pieces of molecular magnetite Angewandte Chemie. ,vol. 43, pp. 5772- 5775 ,(2004) , 10.1002/ANIE.200460636
O. Waldmann, T. C. Stamatatos, G. Christou, H. U. Güdel, I. Sheikin, H. Mutka, Quantum phase interference and Néel-vector tunneling in antiferromagnetic molecular wheels. Physical Review Letters. ,vol. 102, pp. 157202- ,(2009) , 10.1103/PHYSREVLETT.102.157202