Structural and spectroscopic features of a cis (hydroxo)-Fe(III)-(carboxylato) configuration as an active site model for lipoxygenases |
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Authors: | Ogo Seiji Yamahara Ryo Roach Mark Suenobu Tomoyoshi Aki Michihiko Ogura Takashi Kitagawa Teizo Masuda Hideki Fukuzumi Shunichi Watanabe Yoshihito |
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Institution: | Department of Material and Life Science, Graduate School of Engineering, Osaka University, PRESTO & CREST, Japan Science and Technology Corporation (JST), Suita, Osaka 565-0871, Japan. ogo@chem.eng.osaka-u.ac.jp |
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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, Fe(III)(tnpa)(OH)(RCO(2))]ClO(4) tnpa = tris(6-neopentylamino-2-pyridylmethyl)amine; for 1, R = C(6)H(5)], which has a characteristic cis (hydroxo)-Fe(III)-(carboxylato) configuration that models the cis (hydroxo)-Fe(III)-(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)-Fe(III)-(carboxylato) configuration by extending the model complexes from 1 to Fe(III)(tnpa)(OH)(RCO(2))]ClO(4) (2, R = CH(3); 3, R = H) whose cis (hydroxo)-Fe(III)-(carboxylato) moieties are isotopically labeled by (18)OH(-), (16)OD(-), (18)OD(-), (12)CH(3)(12)C(18)O(2)(-), (12)CH(3)(13)C(16)O(2)(-), (13)CH(3)(12)C(16)O(2)(-), (13)CH(3)(13)C(16)O(2)(-), and H(13)C(16)O(2)(-). Complexes 1-3 are characterized by X-ray analysis, IR, EPR, and UV-vis spectroscopy, and electrospray ionization mass spectrometry (ESI-MS). |
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