Open Access
Open access
Science, volume 372, issue 6538, pages eabd5687

Mechanism and dynamics of fatty acid photodecarboxylase

Bonvalet A. 4
Coquelle N 5
Samire P 1, 6
Antonucci L. 4
Benachir A 4
Carbajo S. 7
Doak R. B. 9
Foucar L. 9
Grünbein M 9
HARTMANN E. 9
Kloos M. 9
Lane T.M. 7
Légeret B 1
Schiró G 2
Sliwa M. 11
Zhuang Bo 4, 6
Royant Antoine 2, 3
Weik Martin 2
4
 
LOB, CNRS, INSERM, Ecole Polytechnique, Institut Polytechnique de Paris, 91128 Palaiseau, France.
5
 
Large-Scale Structures Group, Institut Laue Langevin, 38042 Grenoble Cedex 9, France.
6
 
Université Paris-Saclay, CEA, CNRS, Institute for Integrative Biology of the Cell (I2BC), 91198 Gif-sur-Yvette, France.
7
 
Linac Coherent Light Source (LCLS), SLAC National Accelerator Laboratory, Menlo Park, CA 94025, USA.
8
 
Department of Physics, UMR UR1-CNRS 6251, University of Rennes 1, F-Rennes, France.
10
 
Synchrotron SOLEIL. L’Orme des Merisiers Saint-Aubin, BP 48, 91192 Gif-sur-Yvette, France.
11
 
Univ. Lille, CNRS, UMR 8516, LASIRE, LAboratoire de Spectroscopie pour les Interactions, la Réactivité et l’Environnement, 59000 Lille, France.
Publication typeJournal Article
Publication date2021-04-09
Journal: Science
Quartile SCImago
Q1
Quartile WOS
Q1
Impact factor56.9
ISSN00368075, 10959203
Multidisciplinary
Abstract

Fatty acid photodecarboxylase (FAP) is a photoenzyme with potential green chemistry applications. By combining static, time-resolved, and cryotrapping spectroscopy and crystallography as well as computation, we characterized Chlorella variabilis FAP reaction intermediates on time scales from subpicoseconds to milliseconds. High-resolution crystal structures from synchrotron and free electron laser x-ray sources highlighted an unusual bent shape of the oxidized flavin chromophore. We demonstrate that decarboxylation occurs directly upon reduction of the excited flavin by the fatty acid substrate. Along with flavin reoxidation by the alkyl radical intermediate, a major fraction of the cleaved carbon dioxide unexpectedly transformed in 100 nanoseconds, most likely into bicarbonate. This reaction is orders of magnitude faster than in solution. Two strictly conserved residues, R451 and C432, are essential for substrate stabilization and functional charge transfer.

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Sorigué D. et al. Mechanism and dynamics of fatty acid photodecarboxylase // Science. 2021. Vol. 372. No. 6538. p. eabd5687.
GOST all authors (up to 50) Copy
Sorigué D. et al. Mechanism and dynamics of fatty acid photodecarboxylase // Science. 2021. Vol. 372. No. 6538. p. eabd5687.
RIS |
Cite this
RIS Copy
TY - JOUR
DO - 10.1126/science.abd5687
UR - https://doi.org/10.1126%2Fscience.abd5687
TI - Mechanism and dynamics of fatty acid photodecarboxylase
T2 - Science
AU - Sorigué, Damien
AU - Hadjidemetriou, Kyprianos
AU - Blangy, Stéphanie
AU - Gotthard, Guillaume
AU - Bonvalet, A.
AU - Coquelle, N
AU - Samire, P
AU - Antonucci, L.
AU - Benachir, A
AU - Boutet, Sébastien
AU - Byrdin, Martin
AU - Cammarata, Marco
AU - Carbajo, S.
AU - Cuiné, Stephan
AU - Doak, R. B.
AU - Foucar, L.
AU - Gorel, Alexander
AU - Grünbein, M
AU - HARTMANN, E.
AU - Hienerwadel, Rainer
AU - Hilpert, Mario
AU - Kloos, M.
AU - Lane, T.M.
AU - Légeret, B
AU - Legrand, Pierre
AU - Li-Beisson, Yonghua
AU - Moulin, Solène
AU - Nurizzo, Didier
AU - Peltier, Gilles
AU - Schiró, G
AU - Shoeman, Robert
AU - Sliwa, M.
AU - Solinas, Xavier
AU - Zhuang, Bo
AU - Barends, Thomas R. M.
AU - Colletier, Jacques-Philippe
AU - Joffre, Manuel
AU - Royant, Antoine
AU - Berthomieu, Catherine
AU - Weik, Martin
AU - Domratcheva, Tatiana
AU - Brettel, Klaus
AU - Vos, Marten H.
AU - Schlichting, Ilme
AU - Arnoux, Pascal
AU - Müller, Pavel
AU - Beisson, Fred
AU - Aleksandrov, Alexey
PY - 2021
DA - 2021/04/09 00:00:00
PB - American Association for the Advancement of Science (AAAS)
SP - eabd5687
IS - 6538
VL - 372
SN - 0036-8075
SN - 1095-9203
ER -
BibTex |
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BibTex Copy
@article{2021_Sorigué,
author = {Damien Sorigué and Kyprianos Hadjidemetriou and Stéphanie Blangy and Guillaume Gotthard and A. Bonvalet and N Coquelle and P Samire and L. Antonucci and A Benachir and Sébastien Boutet and Martin Byrdin and Marco Cammarata and S. Carbajo and Stephan Cuiné and R. B. Doak and L. Foucar and Alexander Gorel and M Grünbein and E. HARTMANN and Rainer Hienerwadel and Mario Hilpert and M. Kloos and T.M. Lane and B Légeret and Pierre Legrand and Yonghua Li-Beisson and Solène Moulin and Didier Nurizzo and Gilles Peltier and G Schiró and Robert Shoeman and M. Sliwa and Xavier Solinas and Bo Zhuang and Thomas R. M. Barends and Jacques-Philippe Colletier and Manuel Joffre and Antoine Royant and Catherine Berthomieu and Martin Weik and Tatiana Domratcheva and Klaus Brettel and Marten H. Vos and Ilme Schlichting and Pascal Arnoux and Pavel Müller and Fred Beisson and Alexey Aleksandrov},
title = {Mechanism and dynamics of fatty acid photodecarboxylase},
journal = {Science},
year = {2021},
volume = {372},
publisher = {American Association for the Advancement of Science (AAAS)},
month = {apr},
url = {https://doi.org/10.1126%2Fscience.abd5687},
number = {6538},
pages = {eabd5687},
doi = {10.1126/science.abd5687}
}
MLA
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MLA Copy
Sorigué, Damien, et al. “Mechanism and dynamics of fatty acid photodecarboxylase.” Science, vol. 372, no. 6538, Apr. 2021, p. eabd5687. https://doi.org/10.1126%2Fscience.abd5687.
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