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          Institute: MPI für bioanorganische Chemie     Collection: MPI für bioanorganische Chemie     Display Documents

ID: 712231.0, MPI für bioanorganische Chemie / MPI für bioanorganische Chemie
Spectroscopic Characterization of the Bridging Amine in the Active Site of [FeFe] Hydrogenase Using lsotopologues of the H-Cluster
Authors:Adamska-Venkatesh, Agnieszka; Roy, Souvik; Siebel, Judith F.; Simmons, Trevor R.; Fontecave, Marc; Artero, Vincent; Reijerse, Edward J.; Lubitz, Wolfgang
Date of Publication (YYYY-MM-DD):2015
Title of Journal:Journal of the American Chemical Society
Journal Abbrev.:J.Am.Chem.Soc.
Issue / Number:40
Start Page:12744
End Page:12747
Review Status:Internal review
Audience:Experts Only
Abstract / Description:The active site of [Fe Fe] hydrogenase contains a catalytic binuclear iron subsite coordinated by CN- and CO ligands as well as a unique azadithiolate (adt(2-)) bridging ligand. It has been established that this binuclear cofactor is synthesized and assembled by three maturation proteins HydE, -F, and -G. By means of in vitro maturation in the presence of N-15- and C-13-labeled tyrosine it has been shown that the CN- and CO ligands originate from tyrosine. The source of the bridging adt(2-)ligand, however, remains unknown. In order to identify the nitrogen of the bridging amine using HYSCORE spectroscopy and distinguish its spectroscopic signature from that of the CN- nitrogens, we studied three isotope-labeled variants of the H-cluster (N-15-adt(2-)/c(14)N(-), N-15-adt(2-)/(CN-)-N-15, and N-14-adt(2-)/(CN-)-N-15) and extracted accurate values of the hyperfine and quadrupole couplings of both CN- and adt(2-) nitrogens. This will allow an evaluation of isotopologues of the H-cluster generated by in vitro bioassembly in the presence of various N-15-labeled potential precursors as possible sources of the bridging ligand.
Comment of the Author/Creator:Date: 2015, OCT 14 2015
External Publication Status:published
Document Type:Article
Version Comment:Automatic journal name synchronization
Communicated by:N. N.
Affiliations:MPI für bioanorganische Chemie
External Affiliations:[Roy,S.; Simmons,T.R.; Fontecave,M.; Artero,V.] Univ.Grenoble Alpes, CNRS, CEA, Lab Chim & Biol Met, F-38000 Grenoble, France.
Identifiers:ISI:000363002900004 [ID No:1]
ISSN:0002-7863 [ID No:2]
DOI:10.1021/jacs.5b06240 [ID No:3]
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