Spin crossover in a supramolecular FeII-FeIII system

Hiromi Ohta, Yukinari Sunatsuki, Yuichi Ikuta, Naohide Matsumoto, Seiichiro Iijima, Haruo Akashi, Takashi Kambe, Masaaki Kojevia

Research output: Contribution to journalArticle

8 Citations (Scopus)

Abstract

The structure of [FeII(H3L)](ClO4)2·3H 2O, where H3L is a tripodal hexadentate ligand derived from the 1:3 condensation of tris(2-aminoethyl)amine and 4-formylimidazole, has been determined by X-ray crystallography at 113 and 293 K. A spin transition was inferred from the Fe-N bond distances. The temperature dependence of the magnetic susceptibility revealed that the complex undergoes a gradual spin transition in the temperature range of 150-270 K. A mixed-valence complex, [FeII(H3L)][FeIII(L)]- (BF4)2-1.5H2O, was prepared by the controlled deprotonation of the protonated species, [FeII(H3L)](BF4)2-1.5H2O, under aerobic conditions, and the X-ray structure was determined at 293 K. Two species, [FeII(H3L)]2+ and [FeIII(L)], are linked by imidazole-imidazolate (NH-N) hydrogen bonds to form a puckered sheet structure. Magnetic susceptibility measurements and Mössbauer spectra provided an evidence for spin-crossover at both the FeII and FeIII sites. There are three accessible electronic states: (LS FeII-LS FeIII), (HS FeII-LS FeIII), and (HS FeII-HS FeIII) that occur in passing from lower to higher temperatures.

Original languageEnglish
Pages (from-to)191-198
Number of pages8
JournalMaterials Science- Poland
Volume21
Issue number2
Publication statusPublished - 2003

Fingerprint

crossovers
Magnetic susceptibility
magnetic permeability
Deprotonation
X ray crystallography
Electronic states
imidazoles
Temperature
crystallography
Condensation
Amines
Hydrogen bonds
amines
x rays
condensation
Ligands
hydrogen bonds
valence
X rays
temperature dependence

Keywords

  • Hydrogen bonds
  • Spin crossover
  • Tripodal ligand

ASJC Scopus subject areas

  • Materials Science(all)
  • Condensed Matter Physics
  • Mechanical Engineering
  • Mechanics of Materials

Cite this

Ohta, H., Sunatsuki, Y., Ikuta, Y., Matsumoto, N., Iijima, S., Akashi, H., ... Kojevia, M. (2003). Spin crossover in a supramolecular FeII-FeIII system. Materials Science- Poland, 21(2), 191-198.

Spin crossover in a supramolecular FeII-FeIII system. / Ohta, Hiromi; Sunatsuki, Yukinari; Ikuta, Yuichi; Matsumoto, Naohide; Iijima, Seiichiro; Akashi, Haruo; Kambe, Takashi; Kojevia, Masaaki.

In: Materials Science- Poland, Vol. 21, No. 2, 2003, p. 191-198.

Research output: Contribution to journalArticle

Ohta, H, Sunatsuki, Y, Ikuta, Y, Matsumoto, N, Iijima, S, Akashi, H, Kambe, T & Kojevia, M 2003, 'Spin crossover in a supramolecular FeII-FeIII system', Materials Science- Poland, vol. 21, no. 2, pp. 191-198.
Ohta H, Sunatsuki Y, Ikuta Y, Matsumoto N, Iijima S, Akashi H et al. Spin crossover in a supramolecular FeII-FeIII system. Materials Science- Poland. 2003;21(2):191-198.
Ohta, Hiromi ; Sunatsuki, Yukinari ; Ikuta, Yuichi ; Matsumoto, Naohide ; Iijima, Seiichiro ; Akashi, Haruo ; Kambe, Takashi ; Kojevia, Masaaki. / Spin crossover in a supramolecular FeII-FeIII system. In: Materials Science- Poland. 2003 ; Vol. 21, No. 2. pp. 191-198.
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AB - The structure of [FeII(H3L)](ClO4)2·3H 2O, where H3L is a tripodal hexadentate ligand derived from the 1:3 condensation of tris(2-aminoethyl)amine and 4-formylimidazole, has been determined by X-ray crystallography at 113 and 293 K. A spin transition was inferred from the Fe-N bond distances. The temperature dependence of the magnetic susceptibility revealed that the complex undergoes a gradual spin transition in the temperature range of 150-270 K. A mixed-valence complex, [FeII(H3L)][FeIII(L)]- (BF4)2-1.5H2O, was prepared by the controlled deprotonation of the protonated species, [FeII(H3L)](BF4)2-1.5H2O, under aerobic conditions, and the X-ray structure was determined at 293 K. Two species, [FeII(H3L)]2+ and [FeIII(L)], are linked by imidazole-imidazolate (NH-N) hydrogen bonds to form a puckered sheet structure. Magnetic susceptibility measurements and Mössbauer spectra provided an evidence for spin-crossover at both the FeII and FeIII sites. There are three accessible electronic states: (LS FeII-LS FeIII), (HS FeII-LS FeIII), and (HS FeII-HS FeIII) that occur in passing from lower to higher temperatures.

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