Abstract:
:Lactone-hydrolyzing enzymes derived from some Bacillus species are capable of disrupting quorum sensing in bacteria that use N-acyl-l-homoserine lactones (AHLs) as intercellular signaling molecules. Despite the promise of these quorum-quenching enzymes as therapeutic and anti-biofouling agents, the ring opening mechanism and the role of metal ions in catalysis have not been elucidated. Labeling studies using (18)O, (2)H, and the AHL lactonase from Bacillus thuringiensis implicate an addition-elimination pathway for ring opening in which a solvent-derived oxygen is incorporated into the product carboxylate, identifying the alcohol as the leaving group. (1)H NMR is used to show that metal binding is required to maintain proper folding. A thio effect is measured for hydrolysis of N-hexanoyl-l-homoserine lactone and the corresponding thiolactone by AHL lactonase disubstituted with alternative metal ions, including Mn(2+), Co(2+), Zn(2+), and Cd(2+). The magnitude of the thio effect on k(cat) values and the thiophilicity of the metal ion substitutions vary in parallel and are consistent with a kinetically significant interaction between the leaving group and the active site metal center during turnover. X-ray absorption spectroscopy confirms that dicobalt substitution does not result in large structural perturbations at the active site. Finally, substitution of the dinuclear metal site with Cd(2+) results in a greatly enhanced catalyst that can hydrolyze AHLs 1600-24000-fold faster than other reported quorum-quenching enzymes.
journal_name
Biochemistryjournal_title
Biochemistryauthors
Momb J,Thomas PW,Breece RM,Tierney DL,Fast Wdoi
10.1021/bi061238osubject
Has Abstractpub_date
2006-11-07 00:00:00pages
13385-93issue
44eissn
0006-2960issn
1520-4995journal_volume
45pub_type
杂志文章相关文献
BIOCHEMISTRY文献大全abstract::A new series of peptide inhibitors of human Factor VIIa (FVIIa) has been identified and affinity matured from naive and partially randomized peptide phage libraries selected against the immobilized tissue factor x Factor VIIa (TF x FVIIa) complex. These "A-series" peptides contain a single disulfide bond and a 13-resi...
journal_title:Biochemistry
pub_type: 杂志文章
doi:10.1021/bi010591l
更新日期:2001-08-14 00:00:00
abstract::Only beta-beta cross-links form when the alpha(3)(betaE(395)C)(3)gammaK(36)C (MF(1) residue numbers) double mutant subcomplex of TF(1), the F(1)-ATPase from the thermophilic Bacillus PS3, is slowly inactivated with CuCl(2) in the presence or absence of MgATP. The same slow rate of inactivation and extent of beta-beta ...
journal_title:Biochemistry
pub_type: 杂志文章
doi:10.1021/bi036058i
更新日期:2004-03-09 00:00:00
abstract::Safe and effective algaecides are needed to control agriculturally and environmentally significant algal species. Four series (6, 10, 17, and 21) of 29 novel 4-aminopyrimidine derivatives were rationally designed and synthesized. A part of 10, 17, and 21 displayed potent inhibition of Escherichia coli pyruvate dehydro...
journal_title:Biochemistry
pub_type: 杂志文章
doi:10.1021/acs.biochem.7b00636
更新日期:2017-12-12 00:00:00
abstract::Enzymic catalysis proceeds via intermediates formed in the course of substrate conversion. Here, we directly detect key intermediates in thiamin diphosphate (ThDP)-dependent enzymes during catalysis using (1)H NMR spectroscopy. The quantitative analysis of the relative intermediate concentrations allows the determinat...
journal_title:Biochemistry
pub_type: 杂志文章
doi:10.1021/bi034465o
更新日期:2003-07-08 00:00:00
abstract::This paper provides further characterization of a receptor that, in cells lacking the LDL receptor (FH fibroblasts), mediates lipoprotein binding, uptake, and degradation when incubated with oleate at concentrations not exceeding albumin binding capacity. This oleate-activated receptor is genetically distinct from the...
journal_title:Biochemistry
pub_type: 杂志文章
doi:10.1021/bi00171a017
更新日期:1994-02-08 00:00:00
abstract::Neuronal specification is regulated by the activity of transcription factors containing the basic helix-loop-helix motif (bHLH); these regulating proteins include, among others, the neurogenin (Ngn) family, related to the atonal family of genes. Neurogenin 1 (NGN1) is a 237-residue protein that contains a bHLH domain ...
journal_title:Biochemistry
pub_type: 杂志文章
doi:10.1021/bi901616z
更新日期:2010-03-02 00:00:00
abstract::One of the distinctive features of eubacterial retinal-based proton pumps, proteorhodopsins, xanthorhodopsin, and others, is hydrogen bonding of the key aspartate residue, the counterion to the retinal Schiff base, to a histidine. We describe properties of the recently found eubacterium proton pump from Exiguobacteriu...
journal_title:Biochemistry
pub_type: 杂志文章
doi:10.1021/bi300409m
更新日期:2012-07-24 00:00:00
abstract::Acyl carrier protein (ACP) is the central player in fatty acid (FA) biosynthesis. It covalently binds all FA intermediates and presents them to the enzymes needed for elongation. Bacterial ACP must interact with a large number of proteins, which raises the question of how different acyl-ACPs are recognized and disting...
journal_title:Biochemistry
pub_type: 杂志文章
doi:10.1021/bi901713r
更新日期:2010-04-06 00:00:00
abstract::Sulfenic acid is formed upon oxidation of thiols and is a central intermediate in the redox modulation of an increasing number of proteins. Methods for quantifying or even detecting sulfenic acid are scarce. Herein, the reagent 7-chloro-4-nitrobenz-2-oxa-1,3-diazole was determined not to be suitable as a chromophoric ...
journal_title:Biochemistry
pub_type: 杂志文章
doi:10.1021/bi701520y
更新日期:2008-01-08 00:00:00
abstract::Mycoplasmas are the smallest known microorganisms, with drastically reduced genome sizes. One of the essential biochemical pathways lost in mycoplasmas is methylation-mediated DNA repair (MMR), which is responsible for correction of base substitutions, insertions, and deletions in both bacteria and higher organisms. W...
journal_title:Biochemistry
pub_type: 杂志文章
doi:10.1021/bi2009097
更新日期:2011-10-11 00:00:00
abstract::The heat-stable, protein inhibitor of the cyclic adenosine monophosphate (cAMP) dependent protein kinase [Walsh, D. A., Ashby, C. D., Gonzalez, C., Calkins, D., Fischer, E., & Krebs, E (1971a) J. Biol. Chem. 246, 1977-1985] has been purified to homogeneity from rabbit skeletal muscle by preparative electrophoresis. Em...
journal_title:Biochemistry
pub_type: 杂志文章
doi:10.1021/bi00589a011
更新日期:1979-10-30 00:00:00
abstract::One way to improve the economic feasibility of biomass conversion is to enhance the catalytic efficiency of cellulases through protein engineering. This requires that high-resolution structures of cellulases be available. Here we present the structure of E2cd, the catalytic domain of the thermophilic endocellulase E2 ...
journal_title:Biochemistry
pub_type: 杂志文章
doi:10.1021/bi00089a006
更新日期:1993-09-28 00:00:00
abstract::Specific interactions of human melanocortin-4 receptor (hMC4R) with its nonpeptide and peptide agonists were studied using alanine-scanning mutagenesis. The binding affinities and potencies of two synthetic, small-molecule agonists (THIQ, MB243) were strongly affected by substitutions in transmembrane alpha-helices (T...
journal_title:Biochemistry
pub_type: 杂志文章
doi:10.1021/bi0501840
更新日期:2005-08-30 00:00:00
abstract::C-type natriuretic peptide (CNP) binds the guanylyl cyclase-linked natriuretic peptide receptor B (NPR-B) and stimulates marked elevations of the intracellular signaling molecule, cGMP. Here, the essential role of phosphorylation in the hormonal activation and deactivation of this receptor is described. Exposure of NI...
journal_title:Biochemistry
pub_type: 杂志文章
doi:10.1021/bi972303k
更新日期:1998-02-24 00:00:00
abstract::Deuterium NMR has been used to investigate the structure and dynamic state of cytochrome c complexed with bilayers of cardiolipin. Reductive methylation was employed to prepare [N epsilon, N epsilon-C2H3]lysyl cytochrome c, and deuterium exchange provided labeling of backbone sites to give [amide-2H]cytochrome c or mo...
journal_title:Biochemistry
pub_type: 杂志文章
doi:10.1021/bi00230a010
更新日期:1991-04-23 00:00:00
abstract::Multimodular enzymes, including polyketide synthases (PKSs), nonribosomal peptide synthetases (NRPSs), and mixed PKS/NRPS systems, contain functional domains with similar functions. Domain swapping and module fusion are potential powerful strategies for creating hybrid enzymes to synthesize modified natural products. ...
journal_title:Biochemistry
pub_type: 杂志文章
doi:10.1021/bi047538s
更新日期:2005-03-29 00:00:00
abstract::Understanding the evolution of allostery in multidomain enzymes remains an important step in improving our ability to identify and exploit structure-function relationships in allosteric mechanisms. A recent protein similarity network for the DRE-TIM metallolyase superfamily indicated there are two evolutionarily disti...
journal_title:Biochemistry
pub_type: 杂志文章
doi:10.1021/bi500702u
更新日期:2014-07-29 00:00:00
abstract::Seven mutant LH1 polypeptides of Rhodobactor sphaeroides have been isolated, and their behaviors in in vitro reconstitution of LH1 and its subunit complex have been characterized. Two mutants were selected to address the increased stability of the subunit complex of Rb. sphaeroides compared with that of Rhodobacter ca...
journal_title:Biochemistry
pub_type: 杂志文章
doi:10.1021/bi962386p
更新日期:1997-03-25 00:00:00
abstract::To better understand the mechanism of nitric oxide (NO) synthesis, we studied conversion of N-hydroxy-L-arginine (NOHA) or L-arginine (Arg) to citrulline and NO under single-turnover conditions using the oxygenase domain of neuronal nitric oxide synthase (nNOSoxy) and rapid scanning stopped-flow spectroscopy. When ana...
journal_title:Biochemistry
pub_type: 杂志文章
doi:10.1021/bi9920228
更新日期:2000-03-07 00:00:00
abstract::Decorin-binding protein A (DBPA) is an important lipoprotein from the bacterium Borrelia burgdorferi, the causative agent of Lyme disease. The absence of DBPA drastically reduces the pathogenic potential of the bacterium, and biochemical evidence indicates DBPA's interactions with the glycosaminoglycan (GAG) portion o...
journal_title:Biochemistry
pub_type: 杂志文章
doi:10.1021/bi3007093
更新日期:2012-10-23 00:00:00
abstract::Histone redistributions between endogenous DNA in calf thymus chromatin and exogenous DNA from Clostridium perfringens (69% A + T) or from Micrococcus luteus (30% A + T) induced by 0.6 M NaCl or by 2% formaldehyde were studied by thermal denaturation. The observed redistribution occurred on histone Hl when the exogeno...
journal_title:Biochemistry
pub_type: 杂志文章
doi:10.1021/bi00666a002
更新日期:1976-10-19 00:00:00
abstract::A solubilized preparation of steroid 5 alpha-reductase (EC 1.3.1.30) from rat liver has been used in studies focused toward an understanding of the kinetic mechanism associated with enzyme catalysis. From the results of analyses with product and dead-end inhibitors, a preferentially ordered binding of substrates and r...
journal_title:Biochemistry
pub_type: 杂志文章
doi:10.1021/bi00463a025
更新日期:1990-03-20 00:00:00
abstract::The effect of monoclonal anti-(DNA polymerase alpha) immunoglobulin G (IgG) and F(ab) fragments on DNA replication in lysolecithin-permeabilized human cells and on DNA polymerase alpha activity was determined. DNA polymerase alpha activity in vitro was inhibited equally by the same concentrations of monoclonal IgGs an...
journal_title:Biochemistry
pub_type: 杂志文章
doi:10.1021/bi00346a061
更新日期:1985-12-03 00:00:00
abstract::The 24-kDa subunit of mitochondrial NADH-ubiquinone reductase (complex I) is an iron-sulfur protein that is present in the flavoprotein or NADH dehydrogenase II subcomplex. It is a nuclear gene product and is imported into the organelle. A group of human patients with mitochondrial myopathy have been shown to have red...
journal_title:Biochemistry
pub_type: 杂志文章
doi:10.1021/bi00434a021
更新日期:1989-04-18 00:00:00
abstract::The binding of bleomycin to DNA in the presence and absence of ferric iron was measured by fluorescence spectroscopy. In millimolar concentrations of tris(hydroxymethyl)aminomethane, pH 7.5, approximately 80% of the bleomycin binds to DNA. Ferric iron seems to have no significant effect on the binding of DNA to bleomy...
journal_title:Biochemistry
pub_type: 杂志文章
doi:10.1021/bi00531a021
更新日期:1982-01-19 00:00:00
abstract::The effects of GDP and of aurodox (N-methylkirromycin) on the affinity of elongation factor Tu (EF-Tu) for aminoacyl-tRNA (aa-tRNA) have been quantified spectroscopically by using Phe-tRNA(Phe)-Fl8, a functionally active analogue of Phe-tRNA(Phe) with a fluorescein dye convalently attached to the s4U-8 base. The assoc...
journal_title:Biochemistry
pub_type: 杂志文章
doi:10.1021/bi00459a014
更新日期:1990-02-20 00:00:00
abstract::The synthesis and secretion of several acute-phase proteins increases markedly following physiological stress. alpha 1-Acid glycoprotein (AGP), a major acute-phase reactant made by the liver, is strongly induced by inflammatory agents such as lipopolysaccharide (LPS). Nuclear run-on assay showed a 17-fold increase in ...
journal_title:Biochemistry
pub_type: 杂志文章
doi:10.1021/bi00122a005
更新日期:1992-02-25 00:00:00
abstract::The first epidermal growth factor-like domain (EGF-1) from blood coagulation factor VII (FVII) contains two unusual O-linked glycosylation sites at Ser-52 and Ser-60. We report here a detailed study of the effect of O-fucosylation at Ser-60 on the structure of FVII EGF-1, its Ca2+-binding affinity, and its interaction...
journal_title:Biochemistry
pub_type: 杂志文章
doi:10.1021/bi990234z
更新日期:1999-06-01 00:00:00
abstract::Recent studies on cytochrome oxidase have indicated that the putative "peroxy" intermediate in the catalytic cycle (P(R)) is a mixture of intermediates, including P and F [Sucheta, A., et al. (1998) Biochemistry 37, 17905-17914], and the bench-made P and F forms appear to have the same redox state (Fe(a3)(4+)=O(2-)), ...
journal_title:Biochemistry
pub_type: 杂志文章
doi:10.1021/bi020482m
更新日期:2003-05-06 00:00:00
abstract::The interaction of Ca2+ and vanadate with fluorescein isothiocyanate (FITC) labeled sarcoplasmic reticulum (SR) Ca2+-ATPase has been studied by following the kinetics of changes in the reporter group fluorescence and equilibrium fluorescence levels. The vanadate species bound to the enzyme is clearly monomeric orthova...
journal_title:Biochemistry
pub_type: 杂志文章
doi:10.1021/bi00428a057
更新日期:1989-01-24 00:00:00