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Dramatically accelerated selective oxygen-atom transfer by a nonheme iron(IV)-oxo complex: Tuning of the first and second coordination spheres
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Dramatically accelerated selective oxygen-atom transfer by a nonheme iron(IV)-oxo complex: Tuning of the first and second coordination spheres

Leland R. Widger, Casey G. Davies, Tzuhsiung Yang, Maxime A. Siegler, Oliver Troeppner, Guy N. L. Jameson, Ivana Ivanović-Burmazović 和 David P. Goldberg
Journal of the American Chemical Society, 卷.136(7), 頁碼.2699-2702
02/2014
DOI: https://doi.org/10.1021/ja410240c
PMID: 24471779

摘要

Catalysis Chemistry (all) Biochemistry Colloid and Surface Chemistry
The new ligand N3Py amide SR and its Fe II complex [Fe II (N3Py amide SR)](BF 4 ) 2 (1) are described. Reaction of 1 with PhIO at -40 C gives metastable [Fe IV (O)(N3Py amide SR)] 2+ (2), containing a sulfide ligand and a single amide H-bond donor in proximity to the terminal oxo group. Direct evidence for H-bonding is seen in a structural analogue, [Fe II (Cl)(N3Py amide SR)](BF 4 ) 2 (3). Complex 2 exhibits rapid O-atom transfer (OAT) toward external sulfide substrates, but no intramolecular OAT. However, direct S-oxygenation does occur in the reaction of 1 with mCPBA, yielding sulfoxide-ligated [Fe II (N3Py amide S(O)R)](BF 4 ) 2 (4). Catalytic OAT with 1 was also observed. © 2014 American Chemical Society.

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