Ligand binding at the A-cluster in full-length or truncated acetyl-CoA synthase studied by X-ray absorption spectroscopy.
作者： Peer Schrapers , Julia Ilina , Christina M. Gregg , Stefan Mebs , Jae-Hun Jeoung
DOI: 10.1371/JOURNAL.PONE.0171039
关键词: Methyl group 、 Absorption spectroscopy 、 Ligand (biochemistry) 、 Protein domain 、 Enzyme 、 ATP synthase 、 Chemistry 、 Active site 、 Acetyl-CoA 、 Stereochemistry
摘要: Bacteria integrate CO2 reduction and acetyl coenzyme-A (CoA) synthesis in the Wood-Ljungdal pathway. The acetyl-CoA synthase (ACS) active site is a [4Fe4S]-[NiNi] complex (A-cluster). dinickel structure (with proximal, p, distal, d, ions) was studied by X-ray absorption spectroscopy ACS variants comprising all three protein domains or only C-terminal domain with A-cluster. Both showed two square-planar Ni(II) sites an OH- bound at Ni(II)p oxidized enzyme H2O Ni(I)p reduced enzyme; Ni(I)p-CO species induced CO incubation Ni(II)-CH3- additional water ligand methyl group donor. These findings render direct effect of N-terminal middle on A-cluster unlikely.
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sci-hub.se 参考文章(47)
Vincent C.-C. Wang, Stephen W. Ragsdale, Fraser A. Armstrong, Investigations of the Efficient Electrocatalytic Interconversions of Carbon Dioxide and Carbon Monoxide by Nickel-Containing Carbon Monoxide Dehydrogenases The Metal-Driven Biogeochemistry of Gaseous Compounds in the Environment. ,vol. 14, pp. 71- 97 ,(2014) , 10.1007/978-94-017-9269-1_4
Jae-Hun Jeoung, Jochen Fesseler, Sebastian Goetzl, Holger Dobbek, Carbon Monoxide. Toxic Gas and Fuel for Anaerobes and Aerobes: Carbon Monoxide Dehydrogenases The Metal-Driven Biogeochemistry of Gaseous Compounds in the Environment. ,vol. 14, pp. 37- 69 ,(2014) , 10.1007/978-94-017-9269-1_3
S W Ragsdale, P A Lindahl, E Münck, Mössbauer, EPR, and optical studies of the corrinoid/iron-sulfur protein involved in the synthesis of acetyl coenzyme A by Clostridium thermoaceticum. Journal of Biological Chemistry. ,vol. 262, pp. 14289- 14297 ,(1987) , 10.1016/S0021-9258(18)47936-7
Sebastian Götzl, Biochemische und strukturelle Untersuchungen an Proteinen des reduktiven Acetyl-CoA-Weges Humboldt-Universität zu Berlin, Lebenswissenschaftliche Fakultät. ,(2014) , 10.18452/17072
Weiwei Gu, Hongxin Wang, Kun Wang, Extended X‐ray absorption fine structure and multiple‐scattering simulation of nickel dithiolene complexes Ni[S2C2(CF3)2]2n (n = −2, −1, 0) and an olefin adduct Ni[S2C2(CF3)2]2(1‐hexene) Journal of Synchrotron Radiation. ,vol. 22, pp. 124- 129 ,(2015) , 10.1107/S1600577514025041
Güneş Bender, Troy A. Stich, Lifen Yan, R. David Britt, Stephen P. Cramer, Stephen W. Ragsdale, Infrared and EPR Spectroscopic Characterization of a Ni(I) Species Formed by Photolysis of a Catalytically Competent Ni(I)-CO Intermediate in the Acetyl-CoA Synthase Reaction Biochemistry. ,vol. 49, pp. 7516- 7523 ,(2010) , 10.1021/BI1010128
Xiangshi Tan, Marlène Martinho, Audria Stubna, Paul A. Lindahl, Eckard Münck, Mössbauer Evidence for an Exchange-Coupled {[Fe4S4]1+ Nip1+} A-Cluster in Isolated α Subunits of Acetyl-Coenzyme A Synthase/Carbon Monoxide Dehydrogenase Journal of the American Chemical Society. ,vol. 130, pp. 6712- 6713 ,(2008) , 10.1021/JA801981H
Simon J. George, Javier Seravalli, Stephen W. Ragsdale, EPR and Infrared Spectroscopic Evidence That a Kinetically Competent Paramagnetic Intermediate is Formed When Acetyl-Coenzyme A Synthase Reacts with CO Journal of the American Chemical Society. ,vol. 127, pp. 13500- 13501 ,(2005) , 10.1021/JA0528329
Kajsa G.V. Sigfridsson, Nils Leidel, Oliver Sanganas, Petko Chernev, Oliver Lenz, Ki-Seok Yoon, Hirofumi Nishihara, Alison Parkin, Fraser A. Armstrong, Sébastien Dementin, Marc Rousset, Antonio L. De Lacey, Michael Haumann, Structural differences of oxidized iron–sulfur and nickel–iron cofactors in O2-tolerant and O2-sensitive hydrogenases studied by X-ray absorption spectroscopy Biochimica et Biophysica Acta. ,vol. 1847, pp. 162- 170 ,(2015) , 10.1016/J.BBABIO.2014.06.011
Albert S. Reger, Jill M. Carney, Andrew M. Gulick, Biochemical and crystallographic analysis of substrate binding and conformational changes in acetyl-CoA synthetase. Biochemistry. ,vol. 46, pp. 6536- 6546 ,(2007) , 10.1021/BI6026506