A more reactive trigonal-bipyramidal high-spin oxoiron(IV) complex with a cis-labile site
作者： Jason England , Yisong Guo , Katherine M. Van Heuvelen , Matthew A. Cranswick , Gregory T. Rohde
DOI: 10.1021/JA2040909
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摘要: The trigonal-bipyramidal high-spin (S = 2) oxoiron(IV) complex [FeIV(O)(TMG2dien)(CH3CN)]2+ (7) was synthesized and spectroscopically characterized. Substitution of the CH3CN ligand by anions, demonstrated here for X N3– Cl–, yielded additional S 2 complexes general formulation [FeIV(O)(TMG2dien)(X)]+ (7-X). reduced steric bulk 7 relative to published [FeIV(O)(TMG3tren)]2+ (2) reflected enhanced rates intermolecular substrate oxidation.
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John C. Price, Eric W. Barr, Bhramara Tirupati, J. Martin Bollinger,, Carsten Krebs, The First Direct Characterization of a High-Valent Iron Intermediate in the Reaction of an α-Ketoglutarate-Dependent Dioxygenase: A High-Spin Fe(IV) Complex in Taurine/α-Ketoglutarate Dioxygenase (TauD) from Escherichia coli† Biochemistry. ,vol. 42, pp. 7497- 7508 ,(2003) , 10.1021/BI030011F
Danica P Galonić, Eric W Barr, Christopher T Walsh, J Martin Bollinger, Carsten Krebs, Two interconverting Fe( IV ) intermediates in aliphatic chlorination by the halogenase CytC3 Nature Chemical Biology. ,vol. 3, pp. 113- 116 ,(2007) , 10.1038/NCHEMBIO856
Tomasz Borowski, Holger Noack, Mariusz Radoń, Konrad Zych, Per E. M. Siegbahn, Mechanism of Selective Halogenation by SyrB2: A Computational Study Journal of the American Chemical Society. ,vol. 132, pp. 12887- 12898 ,(2010) , 10.1021/JA101877A
Danica Galonić Fujimori, Eric W. Barr, Megan L. Matthews, Gretchen M. Koch, J. Ryan Yonce, Christopher T. Walsh, J. Martin Bollinger, Carsten Krebs, Pamela J. Riggs-Gelasco, Spectroscopic Evidence for a High-Spin Br-Fe(IV)-Oxo Intermediate in the α-Ketoglutarate-Dependent Halogenase CytC3 fromStreptomyces Journal of the American Chemical Society. ,vol. 129, pp. 13408- 13409 ,(2007) , 10.1021/JA076454E
Pamela J. Riggs-Gelasco, John C. Price, Robert B. Guyer, Jessica H. Brehm, Eric W. Barr, J. Martin Bollinger, Carsten Krebs, EXAFS Spectroscopic Evidence for an FeO Unit in the Fe(IV) Intermediate Observed during Oxygen Activation by Taurine:α-Ketoglutarate Dioxygenase Journal of the American Chemical Society. ,vol. 126, pp. 8108- 8109 ,(2004) , 10.1021/JA048255Q
Shanthi Pandian, Mark A. Vincent, Ian H. Hillier, Neil A. Burton, Why does the enzyme SyrB2 chlorinate, but does not hydroxylate, saturated hydrocarbons? A density functional theory (DFT) study Dalton Transactions. pp. 6201- 6207 ,(2009) , 10.1039/B906866J
Elena G Kovaleva, John D Lipscomb, Versatility of biological non-heme Fe(II) centers in oxygen activation reactions. Nature Chemical Biology. ,vol. 4, pp. 186- 193 ,(2008) , 10.1038/NCHEMBIO.71
Shaun D. Wong, Caleb B. Bell, Lei V. Liu, Yeonju Kwak, Jason England, E. Ercan Alp, Jiyong Zhao, Lawrence Que, Edward I. Solomon, Nuclear Resonance Vibrational Spectroscopy on the FeIVO S=2 Non‐Heme Site in TMG3tren: Experimentally Calibrated Insights into Reactivity Angewandte Chemie. ,vol. 50, pp. 3215- 3218 ,(2011) , 10.1002/ANIE.201007692
C. S. Neumann, L. A. Miles, T. L. Grove, S. J. Booker, C. Krebs, C. T. Walsh, J. M. Bollinger, M. L. Matthews, Substrate positioning controls the partition between halogenation and hydroxylation in the aliphatic halogenase, SyrB2 Proceedings of the National Academy of Sciences of the United States of America. ,vol. 106, pp. 17723- 17728 ,(2009) , 10.1073/PNAS.0909649106
Eric J. Klinker, József Kaizer, William W. Brennessel, Nathaniel L. Woodrum, Christopher J. Cramer, Lawrence Que, Structures of Nonheme Oxoiron(IV) Complexes from X-ray Crystallography, NMR Spectroscopy, and DFT Calculations Angewandte Chemie International Edition. ,vol. 44, pp. 3690- 3694 ,(2005) , 10.1002/ANIE.200500485