2006
Molecular Recognition in the Selective Oxygenation of Saturated C-H Bonds by a Dimanganese Catalyst
Das S, Incarvito CD, Crabtree RH, Brudvig GW. Molecular Recognition in the Selective Oxygenation of Saturated C-H Bonds by a Dimanganese Catalyst. Science 2006, 312: 1941-1943. PMID: 16809537, DOI: 10.1126/science.1127899.Peer-Reviewed Original ResearchConceptsHydrogen bondingMolecular recognitionH bondsCarboxylic acid groupsMolecular recognition elementsSynthetic catalystsSaturated CKemp's triacidSelective oxygenationCOOH groupRegioselective functionalizationH activationHigh selectivityAcid groupsRecognition groupReactive centerRecognition elementCatalystTriacidOrient substratesSelectivityBondingBondsControl experimentsSubstrate
2005
New Linear High-Valent Tetranuclear Manganese-Oxo Cluster Relevant to the Oxygen-Evolving Complex of Photosystem II with Oxo, Hydroxo, and Aqua Coordinated to a Single Mn(IV)
Chen, Collomb M, Duboc C, Blondin G, Rivière E, Faller J, Crabtree R, Brudvig G. New Linear High-Valent Tetranuclear Manganese-Oxo Cluster Relevant to the Oxygen-Evolving Complex of Photosystem II with Oxo, Hydroxo, and Aqua Coordinated to a Single Mn(IV). Inorganic Chemistry 2005, 44: 9567-9573. PMID: 16323946, DOI: 10.1021/ic051462m.Peer-Reviewed Original ResearchConceptsGround stateSpin statesFirst excited spin stateExcited spin statesSpin-triplet stateLarge energy gapOxygen-Evolving ComplexMn–Mn distanceDiamagnetic ground stateEnergy gapVariable-temperature magnetic susceptibility dataX-ray powder diffractionTriplet stateMagnetic susceptibility dataTetranuclear manganeseMnIV ionsGeneral Synthesis of Di-μ-oxo Dimanganese Complexes as Functional Models for the Oxygen Evolving Complex of Photosystem II
Chen H, Tagore R, Das S, Incarvito C, Faller J, Crabtree R, Brudvig G. General Synthesis of Di-μ-oxo Dimanganese Complexes as Functional Models for the Oxygen Evolving Complex of Photosystem II. Inorganic Chemistry 2005, 44: 7661-7670. PMID: 16212393, DOI: 10.1021/ic0509940.Peer-Reviewed Original ResearchMeSH KeywordsCrystallography, X-RayModels, BiologicalModels, MolecularOrganometallic CompoundsOxygenPhotosystem II Protein ComplexConceptsDimanganese complexesCatalytic activitySeries of complexesGeneral preparative methodUV-visible spectroscopyElectrospray mass spectrometryOxygen-Evolving ComplexX-ray crystallographyPhotosystem IIParent complexEPR spectroscopyOxygen-evolving activityGeneral synthesisPreparative methodLigand librariesMass spectrometryHigh product purityComplexesMn dimersSpectroscopyProduct purityPrecursorsTerpyCrystallographyOxo
2004
Dimer-of-Dimers Model for the Oxygen-Evolving Complex of Photosystem II. Synthesis and Properties of [MnIV 4O5(terpy)4(H2O)2](ClO4)6
Chen H, Faller J, Crabtree R, Brudvig G. Dimer-of-Dimers Model for the Oxygen-Evolving Complex of Photosystem II. Synthesis and Properties of [MnIV 4O5(terpy)4(H2O)2](ClO4)6. Journal Of The American Chemical Society 2004, 126: 7345-7349. PMID: 15186173, DOI: 10.1021/ja037389l.Peer-Reviewed Original Research
2003
Raman spectra and normal coordinate analyses of low-frequency vibrations of oxo-bridged manganese complexes
Cua A, Vrettos J, de Paula J, Brudvig G, Bocian D. Raman spectra and normal coordinate analyses of low-frequency vibrations of oxo-bridged manganese complexes. JBIC Journal Of Biological Inorganic Chemistry 2003, 8: 439-451. PMID: 12761665, DOI: 10.1007/s00775-002-0433-4.Peer-Reviewed Original ResearchMeSH KeywordsCrystallizationLigandsManganese CompoundsOrganometallic CompoundsOxygenSpectrum Analysis, RamanVibration
2002
Two New Terpyridine Dimanganese Complexes: A Manganese(III,III) Complex with a Single Unsupported Oxo Bridge and a Manganese(III,IV) Complex with a Dioxo Bridge. Synthesis, Structure, and Redox Properties
Baffert C, Collomb M, Deronzier A, Pécaut J, Limburg J, Crabtree R, Brudvig G. Two New Terpyridine Dimanganese Complexes: A Manganese(III,III) Complex with a Single Unsupported Oxo Bridge and a Manganese(III,IV) Complex with a Dioxo Bridge. Synthesis, Structure, and Redox Properties. Inorganic Chemistry 2002, 41: 1404-1411. PMID: 11896708, DOI: 10.1021/ic0107375.Peer-Reviewed Original ResearchConceptsOxo bridgeElectrochemical behaviorX-ray structureMononuclear complexesComplexes 4Oxo complexesRedox propertiesAqua complexesDimanganese complexesOrganic mediaTrans complexesCis geometrySolid stateDioxo bridgeTrans geometryCis complexesDisproportionation processTrans configurationCrystallographic formsComplexesMn atomsCisMonooxoLigandsSynthesis
2001
High-Frequency EPR Study of a New Mononuclear Manganese(III) Complex: [(terpy)Mn(N3)3] (terpy = 2,2‘:6‘,2‘ ‘-Terpyridine)
Limburg J, Vrettos J, Crabtree R, Brudvig G, de Paula J, Hassan A, Barra A, Duboc-Toia C, Collomb M. High-Frequency EPR Study of a New Mononuclear Manganese(III) Complex: [(terpy)Mn(N3)3] (terpy = 2,2‘:6‘,2‘ ‘-Terpyridine). Inorganic Chemistry 2001, 40: 1698-1703. PMID: 11261982, DOI: 10.1021/ic001118j.Peer-Reviewed Original ResearchMeSH KeywordsCrystallography, X-RayElectron Spin Resonance SpectroscopyManganese CompoundsModels, MolecularMolecular StructureOrganometallic CompoundsPyridinesMechanism of photosynthetic water oxidation: combining biophysical studies of photosystem II with inorganic model chemistry
Vrettos J, Limburg J, Brudvig G. Mechanism of photosynthetic water oxidation: combining biophysical studies of photosystem II with inorganic model chemistry. Biochimica Et Biophysica Acta 2001, 1503: 229-245. PMID: 11115636, DOI: 10.1016/s0005-2728(00)00214-0.Peer-Reviewed Original ResearchMeSH KeywordsCrystallographyElectron TransportHemerythrinHydrogen-Ion ConcentrationKineticsManganeseModels, ChemicalModels, MolecularOrganometallic CompoundsOxidation-ReductionOxygenPhotosynthesisPhotosynthetic Reaction Center Complex ProteinsPhotosystem II Protein ComplexProtonsThylakoidsTyrosineWaterConceptsPhotosynthetic water oxidationWater oxidationOxygen-evolving complexProton-coupled electron transferTetranuclear manganese clusterMu-oxo bridgePhotosystem IIReduction of manganeseOOH speciesWater moleculesElectron transferModel chemistryManganese clusterNucleophilic attackDiferric siteFerric hydroperoxideOxidationD1 polypeptideBiophysical studiesOxyhemerythrinBiophysical resultsStructural modelDioxygenChemistryProtonation
2000
Characterization of the O2-Evolving Reaction Catalyzed by [(terpy)(H2O)MnIII(O)2MnIV(OH2)(terpy)](NO3)3 (terpy = 2,2‘:6,2‘ ‘-Terpyridine)
Limburg J, Vrettos J, Chen H, de Paula J, Crabtree R, Brudvig G. Characterization of the O2-Evolving Reaction Catalyzed by [(terpy)(H2O)MnIII(O)2MnIV(OH2)(terpy)](NO3)3 (terpy = 2,2‘:6,2‘ ‘-Terpyridine). Journal Of The American Chemical Society 2000, 123: 423-430. PMID: 11456544, DOI: 10.1021/ja001090a.Peer-Reviewed Original Research