Ligand binding at the A-cluster in full-length or truncated acetyl-CoA synthase studied by X-ray absorption spectroscopy.

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). The dinickel site structure (with proximal, p, and distal, d, ions) was studied by X-ray absorption spectroscopy in...

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Main Authors: Peer Schrapers, Julia Ilina, Christina M Gregg, Stefan Mebs, Jae-Hun Jeoung, Holger Dau, Holger Dobbek, Michael Haumann
Format: Article
Language:English
Published: Public Library of Science (PLoS) 2017-01-01
Series:PLoS ONE
Online Access:https://journals.plos.org/plosone/article/file?id=10.1371/journal.pone.0171039&type=printable
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author Peer Schrapers
Julia Ilina
Christina M Gregg
Stefan Mebs
Jae-Hun Jeoung
Holger Dau
Holger Dobbek
Michael Haumann
author_facet Peer Schrapers
Julia Ilina
Christina M Gregg
Stefan Mebs
Jae-Hun Jeoung
Holger Dau
Holger Dobbek
Michael Haumann
author_sort Peer Schrapers
collection DOAJ
description 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). The dinickel site structure (with proximal, p, and distal, d, ions) was studied by X-ray absorption spectroscopy in ACS variants comprising all three protein domains or only the C-terminal domain with the A-cluster. Both variants showed two square-planar Ni(II) sites and an OH- bound at Ni(II)p in oxidized enzyme and a H2O at Ni(I)p in reduced enzyme; a Ni(I)p-CO species was induced by CO incubation and a Ni(II)-CH3- species with an additional water ligand by a methyl group donor. These findings render a direct effect of the N-terminal and middle domains on the A-cluster structure unlikely.
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issn 1932-6203
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publisher Public Library of Science (PLoS)
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series PLoS ONE
spelling doaj-art-703ef1f0bf3845a4862a5bf790ef31d52025-08-20T03:04:34ZengPublic Library of Science (PLoS)PLoS ONE1932-62032017-01-01122e017103910.1371/journal.pone.0171039Ligand binding at the A-cluster in full-length or truncated acetyl-CoA synthase studied by X-ray absorption spectroscopy.Peer SchrapersJulia IlinaChristina M GreggStefan MebsJae-Hun JeoungHolger DauHolger DobbekMichael HaumannBacteria 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). The dinickel site structure (with proximal, p, and distal, d, ions) was studied by X-ray absorption spectroscopy in ACS variants comprising all three protein domains or only the C-terminal domain with the A-cluster. Both variants showed two square-planar Ni(II) sites and an OH- bound at Ni(II)p in oxidized enzyme and a H2O at Ni(I)p in reduced enzyme; a Ni(I)p-CO species was induced by CO incubation and a Ni(II)-CH3- species with an additional water ligand by a methyl group donor. These findings render a direct effect of the N-terminal and middle domains on the A-cluster structure unlikely.https://journals.plos.org/plosone/article/file?id=10.1371/journal.pone.0171039&type=printable
spellingShingle Peer Schrapers
Julia Ilina
Christina M Gregg
Stefan Mebs
Jae-Hun Jeoung
Holger Dau
Holger Dobbek
Michael Haumann
Ligand binding at the A-cluster in full-length or truncated acetyl-CoA synthase studied by X-ray absorption spectroscopy.
PLoS ONE
title Ligand binding at the A-cluster in full-length or truncated acetyl-CoA synthase studied by X-ray absorption spectroscopy.
title_full Ligand binding at the A-cluster in full-length or truncated acetyl-CoA synthase studied by X-ray absorption spectroscopy.
title_fullStr Ligand binding at the A-cluster in full-length or truncated acetyl-CoA synthase studied by X-ray absorption spectroscopy.
title_full_unstemmed Ligand binding at the A-cluster in full-length or truncated acetyl-CoA synthase studied by X-ray absorption spectroscopy.
title_short Ligand binding at the A-cluster in full-length or truncated acetyl-CoA synthase studied by X-ray absorption spectroscopy.
title_sort ligand binding at the a cluster in full length or truncated acetyl coa synthase studied by x ray absorption spectroscopy
url https://journals.plos.org/plosone/article/file?id=10.1371/journal.pone.0171039&type=printable
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