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

Author

Listed:
  • 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
    Present address: Department of Chemical Physiology, The Scripps Research Institute, La Jolla, California 92307, USA.)

  • 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 III

    (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
    Pennsylvania State University, University Park)

  • J. Martin Bollinger

    (Pennsylvania State University, University Park
    Pennsylvania State University, University Park)

  • Edward I. Solomon

    (Stanford University, Stanford, California 94305, USA
    SLAC National Accelerator Laboratory, Menlo Park, California 94025, USA)

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.

Suggested Citation

  • Shaun D. Wong & Martin Srnec & Megan L. Matthews & Lei V. Liu & Yeonju Kwak & Kiyoung Park & Caleb B. Bell III & E. Ercan Alp & Jiyong Zhao & Yoshitaka Yoda & Shinji Kitao & Makoto Seto & Carsten Kreb, 2013. "Elucidation of the Fe(iv)=O intermediate in the catalytic cycle of the halogenase SyrB2," Nature, Nature, vol. 499(7458), pages 320-323, July.
    • Handle: RePEc:nat:nature:v:499:y:2013:i:7458:d:10.1038_nature12304
    DOI: 10.1038/nature12304
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