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  New Insights into the Nature of Observable Reaction Intermediates in Cytochrome P450 NO Reductase by Using a Combination of Spectroscopy and Quantum Mechanics/Molecular Mechanics Calculations

Riplinger, C., Bill, E., Daiber, A., Ullrich, V., Shoun, H., & Neese, F. (2014). New Insights into the Nature of Observable Reaction Intermediates in Cytochrome P450 NO Reductase by Using a Combination of Spectroscopy and Quantum Mechanics/Molecular Mechanics Calculations. Chemistry – A European Journal, 20(6), 1602-1614. doi:10.1002/chem.201302443.

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 Creators:
Riplinger, Christoph1, Author              
Bill, Eckhard1, Author              
Daiber, Andreas2, Author
Ullrich, Volker3, Author
Shoun, Hirofumi4, Author
Neese, Frank1, Author              
Affiliations:
1Research Department Neese, Max Planck Institute for Chemical Energy Conversion, Max Planck Society, ou_3023886              
2University Medical Center Mainz, Molecular Cardiology, Obere Zahlbacher Str. 63, 55101 Mainz (Germany), ou_persistent22              
3Department of Biology University of Konstanz, 78457 Konstanz (Germany), ou_persistent22              
4Department of Biotechnology, University of Tokyo, Tokyo 113‐8657 (Japan), ou_persistent22              

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Free keywords: enzymes; metalloenzymes; qm/mm calculations; spectroscopy; theoretical spectroscopy
 Abstract: Cytochrome P450 NO reductase is an unusual member of the cytochrome P450 superfamily. It catalyzes the reduction of nitric oxide to nitrous oxide. The reaction intermediates were studied in detail by a combination of experimental and computational methods. They have been characterized experimentally by UV/Vis, EPR, Mössbauer, and MCD spectroscopy. In conjunction with quantum mechanics/molecular mechanics (QM/MM) calculations, we sought to characterize the resting state and the two detectable intermediates in detail and to elucidate the nature of the key intermediate I of the reaction. Six possible candidates were taken into account for the unknown key intermediate in the computational study, differing in protonation state and electronic structure. Two out of the six candidates could be identified as putative intermediates I with the help of the spectroscopic data: singlet diradicals FeIII‐NHO.− and FeIII‐NHOH.. In a companion publication (C. Riplinger, F. Neese, ChemPhysChem­ 2011, 12, 3192) we have used QM/MM models based on these structures and performed a kinetic simulation. The combination of these two studies shows the nature of the key intermediate to be the singlet diradical, FeIII‐NHOH..

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Language(s): eng - English
 Dates: 2013-06-252014-01-222014-02-03
 Publication Status: Published in print
 Pages: 13
 Publishing info: -
 Table of Contents: -
 Rev. Type: Peer
 Identifiers: DOI: 10.1002/chem.201302443
 Degree: -

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Title: Chemistry – A European Journal
  Other : Chem. – Eur. J.
  Other : Chem. Eur. J.
Source Genre: Journal
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Publ. Info: Weinheim : Wiley-VCH
Pages: - Volume / Issue: 20 (6) Sequence Number: - Start / End Page: 1602 - 1614 Identifier: ISSN: 0947-6539
CoNE: https://pure.mpg.de/cone/journals/resource/954926979058