Elucidation of the Fe(iv)=O intermediate in the catalytic cycle of the halogenase SyrB2

Shaun D. Wong, Martin Srnec, Megan L. Matthews, Lei V. Liu, Yeonju Kwak, Kiyoung Park, Caleb B. Bell, E. Ercan Alp, Jiyong Zhao, Yoshitaka Yoda, Shinji Kitao, Makoto Seto, Carsten Krebs (), J. Martin Bollinger () and Edward I. Solomon ()
Additional contact information
Shaun D. Wong: Stanford University, Stanford, California 94305, USA
Martin Srnec: Stanford University, Stanford, California 94305, USA
Megan L. Matthews: Pennsylvania State University, University Park
Lei V. Liu: Stanford University, Stanford, California 94305, USA
Yeonju Kwak: Stanford University, Stanford, California 94305, USA
Kiyoung Park: Stanford University, Stanford, California 94305, USA
Caleb B. Bell: Stanford University, Stanford, California 94305, USA
E. Ercan Alp: Argonne National Laboratory, APS/XFD, 431/D003, Argonne, Illinois 60439, USA
Jiyong Zhao: Argonne National Laboratory, APS/XFD, 431/D003, Argonne, Illinois 60439, USA
Yoshitaka Yoda: SPring-8, JASRI, Hyogo 679-5198, Japan
Shinji Kitao: Research Reactor Institute, Kyoto University
Makoto Seto: Research Reactor Institute, Kyoto University
Carsten Krebs: Pennsylvania State University, University Park
J. Martin Bollinger: Pennsylvania State University, University Park
Edward I. Solomon: Stanford University, Stanford, California 94305, USA

Nature, 2013, vol. 499, issue 7458, 320-323

Abstract: Synchrotron-based nuclear resonance vibrational spectroscopy is used to characterize the reactive Fe(iv)=O intermediate of the halogenase SyrB2; the substrate directs the orientation of this intermediate, presenting specific frontier molecular orbitals that can activate the selective halogenation.

Date: 2013
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DOI: 10.1038/nature12304

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