Structural and spectroscopic features of a cis (hydroxo)-FeIII-(carboxylato) configuration as an active site model for lipoxygenases

Seiji Ogo, Ryo Yamahara, Mark Roach, Tomoyoshi Suenobu, Michihiko Aki, Takashi Ogura, Teizo Kitagawa, Hideki Masuda, Shunichi Fukuzumi, Yoshihito Watanabe

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51 Citations (Scopus)

Abstract

In our preliminary communication (Ogo, S.; Wada, S.; Watanabe, Y.; Iwase, M.; Wada, A.; Harata, M.; Jitsukawa, K.; Masuda, H.; Einaga, H. Angew. Chem., Int. Ed. 1998, 37, 2102-2104), we reported the first example of X-ray analysis of a mononuclear six-coordinate (hydroxo)iron(III) non-heme complex, [FeIII(tnpa)(OH)(RCO2)]-CIO4 [tnpa = tris(6-neopentylamino-2-pyridylmethyl)amine; for 1, R = C6H5], which has a characteristic cis (hydroxo)-FeIII-(carboxylato) configuration that models the cis (hydroxo)-FeIII-(carboxylato) moiety of the proposed (hydroxo)- iron(III) species of lipoxygenases. In this full account, we report structural and spectroscopic characterization of the cis (hydroxo)-FeIII-(carboxylato) configuration by extending the model complexes from 1 to [FeIII(tnpa)(OH)(RCO2)]-CIO4 (2, R = CH3; 3, R = H) whose cis (hydroxo)-FeIII-(carboxylato) moieties are isotopically labeled by 18OH-, 16OD-, 18OD-, 12CH3 12 C18O2 -, 12CH3 13C16 O2 -, 13CH3 12C16 O2 -, 13CH3 13C16 O2 -, and H13C16O2 -. Complexes 1-3 are characterized by X-ray analysis, IR, EPR, and UV-vis spectroscopy, and electrospray ionization mass spectrometry (ESI-MS).

Original languageEnglish
Pages (from-to)5513-5520
Number of pages8
JournalInorganic Chemistry
Volume41
Issue number21
DOIs
Publication statusPublished - Oct 21 2002
Externally publishedYes

All Science Journal Classification (ASJC) codes

  • Physical and Theoretical Chemistry
  • Inorganic Chemistry

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    Ogo, S., Yamahara, R., Roach, M., Suenobu, T., Aki, M., Ogura, T., Kitagawa, T., Masuda, H., Fukuzumi, S., & Watanabe, Y. (2002). Structural and spectroscopic features of a cis (hydroxo)-FeIII-(carboxylato) configuration as an active site model for lipoxygenases. Inorganic Chemistry, 41(21), 5513-5520. https://doi.org/10.1021/ic0200040