Mechanism and dynamics of fatty acid photodecarboxylase

被引：141

作者：

Sorigue, D. ^{[1
]}

Hadjidemetriou, K. ^{[2
]}

Blangy, S. ^{[1
]}

Gotthard, G. ^{[3
]}

Bonvalet, A. ^{[4
]}

Coquelle, N. ^{[5
]}

Samire, P. ^{[1
,6
]}

Aleksandrov, A. ^{[4
]}

Antonucci, L. ^{[4
]}

Benachir, A. ^{[4
]}

Boutet, S. ^{[7
]}

Byrdin, M. ^{[2
]}

Cammarata, M. ^{[8
,13
]}

Carbajo, S. ^{[7
]}

Cuine, S. ^{[1
]}

Doak, R. B. ^{[9
]}

Foucar, L. ^{[9
]}

Gorel, A. ^{[9
]}

Grunbein, M. ^{[9
]}

Hartmann, E. ^{[9
]}

Hienerwadel, R. ^{[1
]}

Hilpert, M. ^{[9
]}

Kloos, M. ^{[9
,14
]}

Lane, T. J. ^{[7
]}

Legeret, B. ^{[1
]}

Legrand, P. ^{[10
]}

Li-Beisson, Y. ^{[1
]}

Moulin, S. L. Y. ^{[1
]}

Nurizzo, D. ^{[3
]}

Peltier, G. ^{[1
]}

Schiro, G. ^{[2
]}

Shoeman, R. L. ^{[9
]}

Sliwa, M. ^{[11
]}

Solinas, X. ^{[4
]}

Zhuang, B. ^{[4
,6
]}

Barends, T. R. M. ^{[9
]}

Colletier, J-P ^{[2
]}

Joffre, M. ^{[4
]}

Royant, A. ^{[2
,3
]}

Berthomieu, C. ^{[1
]}

Weik, M. ^{[2
]}

Domratcheva, T. ^{[9
,12
]}

Brettel, K. ^{[6
]}

Vos, M. H. ^{[4
]}

Schlichting, I ^{[9
]}

Arnoux, P. ^{[1
]}

Mueller, P. ^{[6
]}

Beisson, F. ^{[1
]}

机构：

[1] Aix Marseille Univ, Inst Biosci & Biotechnol, BIAM Cadarache, CNRS,CEA, F-13108 St Paul Les Durance, France

[2] Univ Grenoble Alpes, Inst Biol Struct, CNRS, CEA, F-38000 Grenoble, France

[3] European Synchrotron Radiat Facil, F-38043 Grenoble, France

[4] Inst Polytech Paris, Ecole Polytech, INSERM, CNRS,LOB, F-91128 Palaiseau, France

[5] Inst Laue Langevin, Large Scale Struct Grp, F-38042 Grenoble 9, France

[6] Univ Paris Saclay, Inst Integrat Biol Cell I2BC, CNRS, CEA, F-91198 Gif Sur Yvette, France

[7] SLAC Natl Accelerator Lab, Linac Coherent Light Source LCLS, Menlo Pk, CA 94025 USA

[8] Univ Rennes 1, Dept Phys, UMR UR1 CNRS 6251, Rennes, France

[9] Max Planck Inst Med Res, Jahnstr 29, D-69120 Heidelberg, Germany

[10] Synchrotron SOLEIL Orme Merisiers St Aubin, F-91192 Gif Sur Yvette, France

[11] Univ Lille, Lab Spect Interact Reactivite & Environm, UMR 8516, LASIRE,CNRS, F-59000 Lille, France

[12] Lomonosov Moscow State Univ, Dept Chem, Moscow 119991, Russia

[13] European Synchrotron Radiat Facil ESRF, F-38043 Grenoble, France

[14] Sample Enykonment & Cwacterizat European XFEL, D-22869 Schenefeld, Germany

来源：

SCIENCE | 2021年 / 372卷 / 6538期

基金：

欧洲研究理事会;

关键词：

INFRARED DIFFERENCE SPECTROSCOPY; GRAPHICAL USER-INTERFACE; CRYSTAL-STRUCTURE; ELECTRON-TRANSFER; SEQUENCE ALIGNMENT; PROTEIN FUNCTION; DNA-REPAIR; CRYSTALLOGRAPHY; STATE; DIFFRACTION;

D O I：

10.1126/science.abd5687

中图分类号：

O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];

学科分类号：

07 ; 0710 ; 09 ;

摘要：

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.

引用

页码：148 / +

页数：117

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