Synthesis and Characterization of Diiron(II) Complex with the Asymmetric Ligand Fixed into Internal Surface of Mesoporous Silica

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A new diferrous complex with asymmetric coordination sites, [Fe2(μ-OBz)(L)](ClO4)2 (1) (L = N,N-bis(6-methyl-2-pyridylmethyl)-N’,N’-bis(6-pivalamido-2-pyridylmethyl)-1,3-diaminopropan- 2-ol), was synthesized, which was immobilized in the internal surface of mesoporous silica (FSM-16) to construct a functional material (1A). The reaction of 1 with O2 in acetone at –50°C generated a peroxo complex 2 [λmax = 589 nm (ε = 2200 M-1 cm-1), ν16O-16O = 890 and 908 cm-1 (ν18O-18O = 852 cm-1)]. The μ-peroxo complex 2 was decomposed by bubbling of Ar gas without releasing O2, but the reaction of 1A with O2 at ambient temperature also formed a peroxo complex (2A) without decomposition. The reflectance spectrum of 2A showed a band assignable to the LMCT band from peroxo to a Fe(III) ion at 588 nm. Compound 2A is very stable, whose half-life time is 45 min, in contrast to a short life of 2 (310 sec). 2A released dioxygen by heating up to 75°C in vacuo, which was regenerated by bubbling of dioxygen at ambient temperature.

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Periodical:

Advanced Materials Research (Volumes 11-12)

Main Theme:

Edited by:

Masayuki Nogami, Riguang Jin, Toshihiro Kasuga and Wantai Yang

Pages:

285-290

DOI:

10.4028/www.scientific.net/AMR.11-12.285

Citation:

Y. Kajita et al., "Synthesis and Characterization of Diiron(II) Complex with the Asymmetric Ligand Fixed into Internal Surface of Mesoporous Silica", Advanced Materials Research, Vols. 11-12, pp. 285-290, 2006

Online since:

February 2006

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$35.00

[1] A.L. Feig and S.J. Lippard: Chem. Rev. Vol. 94 (1994), p.759.

[2] R.H. Holm, P. Kennepohl and E.I. Solomon: Chem. Rev. Vol. 96 (1994), p.759.

[3] L. Que Jr.: J. Chem. Soc., Dalton Trans. (1997), p.3933.

[4] R.E. Stenkamp: Chem. Rev. Vol. 94 (1994), p.715.

[5] A.C. Rosenzweig, C.A. Frederick, S.J. Lippard and P. Nordlund: Nature Vol. 366 (1993), p.537.

[6] E.Y. Tshuva and S.J. Lippard: Chem. Rev. Vol. 104 (2004), p.987.

[7] D.E.D. Vos, M. Dams, B.F. Sels and P.A. Jacobs: Chem. Rev. Vol. 102 (2002), p.3615.

[8] H. Arii: Ph. D. Dissertation, Nagoya Institute of Technology (2003).

[9] M. Nowotny, L.N. Pedersen, U. Hanefeld and T. Maschmeyer: Chem. Eur. J. Vol. 8 (2002), p.3724.

[10] Crystal data for 1 (C46H56Cl2Fe2N8O13, Fw = 1111. 59) at 173K: yellow plates, monoclinic space group P21/n (No. 14), a = 11. 2215 (7) Å, b = 11. 6157 (5) Å, c = 38. 597 (2) Å, β = 94. 919 (3) ˚, V = 5012. 4 (5) Å 3, Z = 4. For 11217 unique, observed reflections with I > 2. 00σ(I) and 640 Variables parameters, the current discrepancy indices are R = 0. 073 and Rw = 0. 223.

[11] Y. Dong, S. Yan, V.G. Young and L. Que Jr.: Angew. Chem., Int. Ed. Vol. 35 (1996), p.618.

[12] T. Ookubo, H. Sugimoto, T. Nagayama, H. Masuda, T. Sato, K. Tanaka, Y. Maeda, H. Okawa, Y. Hayashi, A. Uehara and M. Suzuki: J. Am. Chem. Soc. Vol. 118 (1996), p.701.

DOI: 10.1021/ja953705n

[13] K. Kim and S.J. Lippard: J. Am. Chem. Soc. Vol. 118 (1996), p.4914.

[14] Y. Dong, S. Ménage, B.A. Brennan, T.E. Elgren, H.G. Jang, L.L. Pearce and L. Que Jr: J. Am. Chem. Soc. Vol. 115 (1993), p.1851.

[15] H. Arii, Y. Funahashi, K. Jitsukawa and H. Masuda: J. Inorg. Biochem. Vol. 82 (2000), p.153.

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