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showing 10 items of 184 documents

Intramolecular electron transfer between molybdenum and iron mimicking bacterial sulphite dehydrogenase

2014

Diferrocenyl/diferrocenium substituted dioxido molybdenum(VI) complexes [Fe2MoO2] 2(Fc)/[2(FC)]²⁺ mimic the catalytic active site including the redox subunits as well as the catalytic function of bacterial sulphite oxidases.

IronSulfite DehydrogenaseMolecular Conformationchemistry.chemical_elementBiocompatible MaterialsElectronsCrystallography X-RayPhotochemistryRedoxCatalysisCatalysisElectron TransportElectron transferCoordination ComplexesCatalytic DomainPolymer chemistryMaterials ChemistrySulfite dehydrogenaseFerrous CompoundsMolybdenumBacteriabiologyMetals and AlloysActive siteGeneral ChemistryElectron transport chainSurfaces Coatings and FilmsElectronic Optical and Magnetic MaterialschemistryMolybdenumIntramolecular forceCeramics and Compositesbiology.proteinOxidation-ReductionChemical Communications
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A fundamental catalytic difference between zinc and manganese dependent enzymes revealed in a bacterial isatin hydrolase

2018

Scientific reports 8(1), 13104 (2018). doi:10.1038/s41598-018-31259-y

IsatinModels Molecular0301 basic medicineStereochemistryGlutaminelcsh:Medicine010402 general chemistry01 natural sciencesArticleAmidohydrolasesCatalysisEvolution Molecular03 medical and health scienceschemistry.chemical_compoundBacterial ProteinsCatalytic DomainHydrolaseCatalytic triadAmino Acid SequenceRhodobacteraceaelcsh:ScienceConserved SequenceKynureninechemistry.chemical_classificationManganeseMultidisciplinarybiologyAmidohydrolaseHydrolysisIsatinlcsh:RActive site6000104 chemical sciencesZinc030104 developmental biologyEnzymechemistryBiocatalysisArylformamidaseBiocatalysisbiology.proteinQuantum Theorylcsh:QProtonsddc:600
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Protein Conformational Landscapes and Catalysis. Influence of Active Site Conformations in the Reaction Catalyzed by L-Lactate Dehydrogenase

2015

In the past decade, L-Lactate Dehydrogenase (LDH) has become an extremely useful marker in both clinical diagnosis and in monitoring the course of many human diseases. It has been assumed since the 1980s that the full catalytic process of LDH starts with the binding of the cofactor and the substrate followed by the enclosure of the active site by a mobile loop of the protein before the reaction takes place. In this paper, we show that the chemical step of the LDH-catalyzed reaction can proceed within the open loop conformation, and the different reactivity of the different protein conformations would be in agreement with the broad range of rate constants measured in single-molecule spectrom…

KIEsReaction mechanismFree energy surfacesbiologyLDHChemistryStereochemistryActive siteSubstrate (chemistry)Single-molecule experimentsGeneral ChemistryQM/MMArticleCatalysisCatalysisQM/MMReaction rate constantTetramerbiology.proteinReactivity (chemistry)Reaction mechanism
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Inhibition Mechanism of SARS‐CoV‐2 Main Protease with Ketone‐Based Inhibitors Unveiled by Multiscale Simulations: Insights for Improved Designs**

2021

Abstract We present the results of classical and QM/MM simulations for the inhibition of SARS‐CoV‐2 3CL protease by a hydroxymethylketone inhibitor, PF‐00835231. In the noncovalent complex the carbonyl oxygen atom of the warhead is placed in the oxyanion hole formed by residues 143 to 145, while P1–P3 groups are accommodated in the active site with interactions similar to those observed for the peptide substrate. According to alchemical free energy calculations, the P1′ hydroxymethyl group also contributes to the binding free energy. Covalent inhibition of the enzyme is triggered by the proton transfer from Cys145 to His41. This step is followed by the nucleophilic attack of the Sγ atom on …

KetoneMolecular modelStereochemistrySubstituentMolecular Dynamics SimulationSARS‐CoV‐2 Inhibitors | Hot PaperCatalysisQM/MM3CL proteasechemistry.chemical_compoundCatalytic DomaininhibitorsHumansHydroxymethylProtease InhibitorsCoronavirus 3C ProteasesResearch Articleschemistry.chemical_classificationPF-00835231Binding SitesbiologySARS-CoV-2molecular modelingActive siteCOVID-19General ChemistryGeneral MedicineKetonesCOVID-19 Drug TreatmentKineticschemistryCovalent bondDrug Designbiology.proteinThermodynamicsOxyanion holeResearch ArticleAngewandte Chemie
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Acetylcholine-binding protein in the hemolymph of the planorbid snail Biomphalaria glabrata is a pentagonal dodecahedron (60 subunits).

2012

Nicotinic acetylcholine receptors (nAChR) play important neurophysiological roles and are of considerable medical relevance. They have been studied extensively, greatly facilitated by the gastropod acetylcholine-binding proteins (AChBP) which represent soluble structural and functional homologues of the ligand-binding domain of nAChR. All these proteins are ring-like pentamers. Here we report that AChBP exists in the hemolymph of the planorbid snail Biomphalaria glabrata (vector of the schistosomiasis parasite) as a regular pentagonal dodecahedron, 22 nm in diameter (12 pentamers, 60 active sites). We sequenced and recombinantly expressed two ∼25 kDa polypeptides (BgAChBP1 and BgAChBP2) wit…

Macromolecular AssembliesProtein StructureProtein FoldingScienceBiophysicsBiochemistryProtein ChemistryHomology (biology)Ion ChannelsProtein Structure Secondarylaw.inventionDodecahedronAcetylcholine bindinglawHemolymphHemolymphMacromolecular Structure AnalysisBiomphalaria glabrataAnimal PhysiologyAnimalsBiomacromolecule-Ligand InteractionsBiologyAcetylcholine receptorMultidisciplinaryHemoproteinsbiologyBiomphalariaQRActive siteProteinsComputational BiologyAnatomybiology.organism_classificationRecombinant ProteinsAcetylcholineProtein Structure TertiaryBiochemistryAcetylcholine Receptorsbiology.proteinRecombinant DNAMedicineCarrier ProteinsZoologyResearch ArticlePLoS ONE
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Endothelium- and nitric oxide-dependent vasorelaxing activities of gamma-butyrobetaine esters: possible link to the antiischemic activities of mildro…

2004

Mildronate [3-(2,2,2-trimethylhydrazine) propionate (THP)] is an antiischemic drug acting mainly via inhibition of fatty acid beta-oxidation. Some effects of the drug cannot be explained by the latter mechanism. We tested the eventual nitric oxide (NO) dependence of the mildronate action. Mildronate, gamma-butyrobetaine (GBB) and GBB methyl ester induced transient increases in nitric oxide (NO) concentrations in rat blood and myocardium. In vitro, these compounds neither modified the activities of purified neuronal and endothelial recombinant nitric oxide synthases (NOSs) nor were able to interact with their active site. GBB induced vasodilatation at high concentrations only (EC50 = 5 x 10(…

MaleEndotheliumNitric Oxide Synthase Type IIIStereochemistryDrug Evaluation PreclinicalMyocardial IschemiaVasodilationAorta ThoracicNitric OxideMuscle Smooth VascularNitric oxidechemistry.chemical_compoundCarnitinemedicineAnimalsEndotheliumRats WistarPharmacologychemistry.chemical_classificationbiologyElectron Spin Resonance SpectroscopyActive siteFatty acidDrug SynergismRatsNitric oxide synthaseBetaineVasodilationDrug Combinationsmedicine.anatomical_structureEnzymeNG-Nitroarginine Methyl Esterchemistrybiology.proteinPropionateNitric Oxide SynthaseDitiocarbMethylhydrazinesEuropean journal of pharmacology
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The N-terminal domain of mammalian soluble epoxide hydrolase is a phosphatase

2003

The mammalian soluble epoxide hydrolase (sEH) is an enzyme with multiple functions, being implicated in detoxification of xenobiotic epoxides as well as in regulation of physiological processes such as blood pressure. The enzyme is a homodimer, in which each subunit is composed of two domains. The 35-kDa C-terminal domain has an α/β hydrolase fold and harbors the catalytic center for the EH activity. The 25-kDa N-terminal domain has a different α/β fold and belongs to the haloacid dehalogenase superfamily of enzymes. The catalytic properties of the enzyme reported so far can all be explained by the action of the C-terminal domain alone. The function of the N-terminal domain, other than in …

MaleModels MolecularEpoxide hydrolase 2HydrolasesStereochemistryProtein subunitMolecular Sequence DataPhosphatase10050 Institute of Pharmacology and Toxicology610 Medicine & healthDephosphorylationHydrolaseAnimalsHumansAmino Acid SequenceDNA PrimersEpoxide Hydrolaseschemistry.chemical_classification1000 MultidisciplinaryMultidisciplinaryBase SequenceSequence Homology Amino AcidbiologyChemistryActive siteBiological SciencesPhosphoric Monoester HydrolasesRats Inbred F344Recombinant ProteinsRatsAmino acidEnzymeSolubilityBiochemistryMutagenesis Site-Directedbiology.protein570 Life sciences; biologyProceedings of the National Academy of Sciences
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Globally Optimized Equilibrium Shapes of Zirconia-Supported Rh and Pt Nanoclusters: Insights into Site Assembly and Reactivity

2019

Metal–support interfaces form an active site for many important catalytic reactions. The modeling of these interfacial sites calls for approximations to set up a structure model, which in turn may ...

Materials science02 engineering and technology010402 general chemistry01 natural sciencesCatalysisNanoclustersTurn (biochemistry)nanorakenteetnanostructuresReactivity (chemistry)Cubic zirconiaPhysical and Theoretical ChemistryStructured modelta116ta114biologysite assemblyActive site021001 nanoscience & nanotechnology0104 chemical sciencesSurfaces Coatings and FilmsElectronic Optical and Magnetic MaterialsreactivityGeneral EnergyChemical engineeringbiology.protein0210 nano-technologyThe Journal of Physical Chemistry C
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Structure-Guided, Single-Point Modifications in the Phosphinic Dipeptide Structure Yield Highly Potent and Selective Inhibitors of Neutral Aminopepti…

2014

Seven crystal structures of alanyl aminopeptidase from Neisseria meningitides (the etiological agent of meningitis, NmAPN) complexed with organophosphorus compounds were resolved to determine the optimal inhibitor–enzyme interactions. The enantiomeric phosphonic acid analogs of Leu and hPhe, which correspond to the P1 amino acid residues of well-processed substrates, were used to assess the impact of the absolute configuration and the stereospecific hydrogen bond network formed between the aminophosphonate polar head and the active site residues on the binding affinity. For the hPhe analog, an imperfect stereochemical complementarity could be overcome by incorporating an appropriate P1 side…

MeningitidesStereochemistryHeteroatomAminopeptidases01 natural sciencesArticleLeucyl AminopeptidaseStructure-Activity Relationship03 medical and health scienceschemistry.chemical_compoundDrug DiscoveryHumansProtease Inhibitors030304 developmental biology0303 health sciencesBinding SitesDipeptidebiology010405 organic chemistryHydrogen bondAbsolute configurationActive siteLigand (biochemistry)0104 chemical scienceschemistryAminophosphonateDrug Designbiology.proteinMolecular MedicineJournal of Medicinal Chemistry
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Substrate promiscuity in DNA methyltransferase M.PvuII. A mechanistic insight

2012

M.PvuII is a DNA methyltransferase from the bacterium Proteus vulgaris that catalyzes methylation of cytosine at the N4 position. This enzyme also displays promiscuous activity catalyzing methylation of adenine at the N6 position. In this work we use QM/MM methods to investigate the reaction mechanism of this promiscuous activity. We found that N6 methylation in M.PvuII takes place by means of a stepwise mechanism in which deprotonation of the exocyclic amino group is followed by the methyl transfer. Deprotonation involves two residues of the active site, Ser53 and Asp96, while methylation takes place directly from the AdoMet cofactor to the target nitrogen atom. The same reaction mechanism…

MethyltransferaseDNA-Cytosine MethylasesDNA methyltransferaseM.PvuIIMolecular Dynamics SimulationBiochemistryDNA methyltransferaseMethylationSubstrate Specificitychemistry.chemical_compoundCytosineDeprotonationCatalytic DomainProteus vulgarisPhysical and Theoretical ChemistrybiologyThermus aquaticusAdenineOrganic ChemistryActive siteMethylationbiology.organism_classificationBiochemistrychemistryDNA methylationbiology.proteinCytosine
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