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  Mechanism and dynamics of fatty acid photodecarboxylase

Sorigué, D., Hadjidemetriou, K., Blangy, S., Gotthard, G., Bonvalet, A., Coquelle, N., et al. (2021). Mechanism and dynamics of fatty acid photodecarboxylase. Science, 372(6538): eabd5687, pp. 1-13. doi:10.1126/science.abd5687.

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Sorigué, D, Author
Hadjidemetriou, K, Author
Blangy, S, Author
Gotthard, G, Author
Bonvalet, A, Author
Coquelle, N, Author
Samire, P, Author
Aleksandrov, A, Author
Antonucci, L, Author
Benachir, A, Author
Boutet, S, Author
Byrdin, M, Author
Cammarata, M, Author
Carbajo, S, Author
Cuiné, S, Author
Doak, R B1, Author              
Foucar, L1, Author              
Gorel, A1, Author              
Grünbein, M1, Author              
Hartmann, E1, Author              
Hienerwadel, R, AuthorHilpert, M1, Author              Kloos, M1, Author              Lane, T J, AuthorLégeret, B, AuthorLegrand, P, AuthorLi-Beisson, Y, AuthorMoulin, S L Y, AuthorNurizzo, D, AuthorPeltier, G, AuthorSchirò, G, AuthorShoeman, R L1, Author              Sliwa, M, AuthorSolinas, X, AuthorZhuang, B, AuthorBarends, T R M1, Author              Colletier, J-P, AuthorJoffre, M, AuthorRoyant, A, AuthorBerthomieu, C, AuthorWeik, M, AuthorDomratcheva, T1, Author              Brettel, K, AuthorVos, M H, AuthorSchlichting, I1, Author              Arnoux, P, AuthorMüller, P, AuthorBeisson, F, Author more..
Affiliations:
1Department of Biomolecular Mechanisms, Max Planck Institute for Medical Research, Max Planck Society, ou_1497700              

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 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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Language(s): eng - English
 Dates: 2020-06-292021-02-172021-04-09
 Publication Status: Published online
 Pages: 13
 Publishing info: -
 Table of Contents: -
 Rev. Type: Peer
 Identifiers: DOI: 10.1126/science.abd5687
 Degree: -

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Title: Science
  Abbreviation : Science
Source Genre: Journal
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Publ. Info: Washington, D.C. : American Association for the Advancement of Science
Pages: - Volume / Issue: 372 (6538) Sequence Number: eabd5687 Start / End Page: 1 - 13 Identifier: ISSN: 0036-8075
CoNE: https://pure.mpg.de/cone/journals/resource/991042748276600_1