Literature DB >> 16756317

How nitrogenase shakes--initial information about P-cluster and FeMo-cofactor normal modes from nuclear resonance vibrational spectroscopy (NRVS).

Yuming Xiao1, Karl Fisher, Matt C Smith, William E Newton, David A Case, Simon J George, Hongxin Wang, Wolfgang Sturhahn, Ercan E Alp, Jiyong Zhao, Yoshitaka Yoda, Stephen P Cramer.   

Abstract

Nitrogenase catalyzes a reaction critical for life, the reduction of N(2) to 2NH(3), yet we still know relatively little about its catalytic mechanism. We have used the synchrotron technique of (57)Fe nuclear resonance vibrational spectroscopy (NRVS) to study the dynamics of the Fe-S clusters in this enzyme. The catalytic site FeMo-cofactor exhibits a strong signal near 190 cm(-)(1), where conventional Fe-S clusters have weak NRVS. This intensity is ascribed to cluster breathing modes whose frequency is raised by an interstitial atom. A variety of Fe-S stretching modes are also observed between 250 and 400 cm(-)(1). This work is the first spectroscopic information about the vibrational modes of the intact nitrogenase FeMo-cofactor and P-cluster.

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Year:  2006        PMID： 16756317      PMCID： PMC3174779          DOI： 10.1021/ja0603655

Source DB:  PubMed          Journal:  J Am Chem Soc        ISSN： 0002-7863            Impact factor:   15.419


  30 in total

1.  Nitrogenase MoFe-protein at 1.16 A resolution: a central ligand in the FeMo-cofactor.

Authors:  Oliver Einsle; F Akif Tezcan; Susana L A Andrade; Benedikt Schmid; Mika Yoshida; James B Howard; Douglas C Rees
Journal:  Science       Date:  2002-09-06       Impact factor: 47.728

2.  Atoms, molecules, solids, and surfaces: Applications of the generalized gradient approximation for exchange and correlation.

Authors: 
Journal:  Phys Rev B Condens Matter       Date:  1992-09-15

3.  The interstitial atom of the nitrogenase FeMo-cofactor: ENDOR and ESEEM evidence that it is not a nitrogen.

Authors:  Tran-Chin Yang; Nathan K Maeser; Mikhail Laryukhin; Hong-In Lee; Dennis R Dean; Lance C Seefeldt; Brian M Hoffman
Journal:  J Am Chem Soc       Date:  2005-09-21       Impact factor: 15.419

4.  Apodinitrogenase: purification, association with a 20-kilodalton protein, and activation by the iron-molybdenum cofactor in the absence of dinitrogenase reductase.

Authors:  T D Paustian; V K Shah; G P Roberts
Journal:  Biochemistry       Date:  1990-04-10       Impact factor: 3.162

5.  Structural, spectroscopic, and redox consequences of a central ligand in the FeMoco of nitrogenase: a density functional theoretical study.

Authors:  Timothy Lovell; Tiqing Liu; David A Case; L Noodleman
Journal:  J Am Chem Soc       Date:  2003-07-09       Impact factor: 15.419

6.  Normal-mode analysis of FeCl4- and Fe2S2Cl42- via vibrational mössbauer, resonance Raman, and FT-IR spectroscopies.

Authors:  Matt C Smith; Yuming Xiao; Hongxin Wang; Simon J George; Dimitri Coucouvanis; Markos Koutmos; Wolfgang Sturhahn; Ercan E Alp; Jiyong Zhao; Stephen P Cramer
Journal:  Inorg Chem       Date:  2005-08-08       Impact factor: 5.165

7.  Application of a universal force field to mixed Fe/Mo-S/Se cubane and heterocubane clusters. 1. Substitution of sulfur by selenium in the series [Fe4X4(YCH3)4]2-; X = S/Se and Y = S/Se.

Authors:  Axel Kern; Christian Näther; Felix Studt; Felix Tuczek
Journal:  Inorg Chem       Date:  2004-08-09       Impact factor: 5.165

8.  Application of a universal force field to mixed Fe/Mo-S/Se cubane and heterocubane clusters. 2. Substitution of iron by molybdenum in Fe4(S/Se)4 clusters with terminal halide and thiolate ligands.

Authors:  Axel Kern; Christian Näther; Felix Tuczek
Journal:  Inorg Chem       Date:  2004-08-09       Impact factor: 5.165

9.  An Isc-type extremely thermostable [2Fe-2S] ferredoxin from Aquifex aeolicus. Biochemical, spectroscopic, and unfolding studies.

Authors:  Géraldine Mitou; Catherine Higgins; Pernilla Wittung-Stafshede; Richard C Conover; Archer D Smith; Michael K Johnson; Jacques Gaillard; Audria Stubna; Eckard Münck; Jacques Meyer
Journal:  Biochemistry       Date:  2003-02-11       Impact factor: 3.162

10.  Modeling a central ligand in the nitrogenase FeMo cofactor.

Authors:  Berit Hinnemann; Jens K Nørskov
Journal:  J Am Chem Soc       Date:  2003-02-12       Impact factor: 15.419
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  27 in total

1.  A combined NRVS and DFT study of Fe(IV)=O model complexes: a diagnostic method for the elucidation of non-heme iron enzyme intermediates.

Authors:  Caleb B Bell; Shaun D Wong; Yuming Xiao; Eric J Klinker; Adam L Tenderholt; Matt C Smith; Jan-Uwe Rohde; Lawrence Que; Stephen P Cramer; Edward I Solomon
Journal:  Angew Chem Int Ed Engl       Date:  2008       Impact factor: 15.336

2.  Energy calibration issues in nuclear resonant vibrational spectroscopy: observing small spectral shifts and making fast calibrations.

Authors:  Hongxin Wang; Yoshitaka Yoda; Weibing Dong; Songping D Huang
Journal:  J Synchrotron Radiat       Date:  2013-08-17       Impact factor: 2.616

3.  Metal-dioxygen and metal-dinitrogen complexes: where are the electrons?

Authors:  Patrick L Holland
Journal:  Dalton Trans       Date:  2010-04-01       Impact factor: 4.390

Review 4.  Reduction of Substrates by Nitrogenases.

Authors:  Lance C Seefeldt; Zhi-Yong Yang; Dmitriy A Lukoyanov; Derek F Harris; Dennis R Dean; Simone Raugei; Brian M Hoffman
Journal:  Chem Rev       Date:  2020-03-16       Impact factor: 60.622

5.  Reduction of N2 by Fe2+ via homogeneous and heterogeneous reactions Part 2: the role of metal binding in activating N2 for reduction; a requirement for both pre-biotic and biological mechanisms.

Authors:  Matthew C F Wander; James D Kubicki; Martin A A Schoonen
Journal:  Orig Life Evol Biosph       Date:  2008-05-02       Impact factor: 1.950

6.  Extended X-ray absorption fine structure and nuclear resonance vibrational spectroscopy reveal that NifB-co, a FeMo-co precursor, comprises a 6Fe core with an interstitial light atom.

Authors:  Simon J George; Robert Y Igarashi; Yuming Xiao; Jose A Hernandez; Marie Demuez; Dehua Zhao; Yoshitaka Yoda; Paul W Ludden; Luis M Rubio; Stephen P Cramer
Journal:  J Am Chem Soc       Date:  2008-04-02       Impact factor: 15.419

7.  Nuclear resonance vibrational spectroscopy and electron paramagnetic resonance spectroscopy of 57Fe-enriched [FeFe] hydrogenase indicate stepwise assembly of the H-cluster.

Authors:  Jon M Kuchenreuther; Yisong Guo; Hongxin Wang; William K Myers; Simon J George; Christine A Boyke; Yoshitaka Yoda; E Ercan Alp; Jiyong Zhao; R David Britt; James R Swartz; Stephen P Cramer
Journal:  Biochemistry       Date:  2013-01-24       Impact factor: 3.162

8.  NRVS for Fe in Biology: Experiment and Basic Interpretation.

Authors:  Leland B Gee; Hongxin Wang; Stephen P Cramer
Journal:  Methods Enzymol       Date:  2017-12-16       Impact factor: 1.600

9.  Predicting Nuclear Resonance Vibrational Spectra of [Fe(OEP)(NO)].

Authors:  Qian Peng; Jeffrey W Pavlik; W Robert Scheidt; Olaf Wiest
Journal:  J Chem Theory Comput       Date:  2011-11-29       Impact factor: 6.006

10.  Characterization of [4Fe-4S] cluster vibrations and structure in nitrogenase Fe protein at three oxidation levels via combined NRVS, EXAFS, and DFT analyses.

Authors:  Devrani Mitra; Simon J George; Yisong Guo; Saeed Kamali; Stephen Keable; John W Peters; Vladimir Pelmenschikov; David A Case; Stephen P Cramer
Journal:  J Am Chem Soc       Date:  2013-02-11       Impact factor: 15.419
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