2024
Mutation-induced shift of the photosystem II active site reveals insight into conserved water channels
Flesher D, Liu J, Wang J, Gisriel C, Yang K, Batista V, Debus R, Brudvig G. Mutation-induced shift of the photosystem II active site reveals insight into conserved water channels. Journal Of Biological Chemistry 2024, 300: 107475. PMID: 38879008, PMCID: PMC11294709, DOI: 10.1016/j.jbc.2024.107475.Peer-Reviewed Original ResearchOxygen-evolving complexPhotosystem II active sitePhotosystem IIJahn-Teller distortionPhotosystem II complexD1-Asp170Jahn-TellerResolution cryo-EM structureMutation-induced structural changesCryo-EM structureMagnetic propertiesD1 subunitActive siteOxygenic photosynthesisMutagenesis studiesLight-driven water oxidationSpectroscopic propertiesStructural basisSpectroscopic dataAmino acidsWater oxidation mechanismPhotosystemMutationsMutation-induced shiftWater oxidation
2023
Bridging the Coordination Chemistry of Small Compounds and Metalloproteins Using Machine Learning
Kapuścińska K, Dukała Z, Doha M, Ansari E, Wang J, Brudvig G, Brooks B, Amin M. Bridging the Coordination Chemistry of Small Compounds and Metalloproteins Using Machine Learning. Journal Of Chemical Information And Modeling 2023, 64: 2586-2593. PMID: 38054243, DOI: 10.1021/acs.jcim.3c01564.Peer-Reviewed Original ResearchOxidation stateMetal ionsActive siteCambridge Crystallographic Data CentreMetal oxidation stateElectron transfer reactionsStandard reduction potentialLower oxidation statesX-ray crystallographyCoordination chemistryCryogenic electron microscopyMetal clustersTransfer reactionsReaction mechanismReduction potentialXFEL crystallographyMetalloproteinsAppropriate experimental conditionsSmall moleculesCrystallographySmall compoundsSpecific reactionElectron microscopyRemarkable efficiencyMetalsActive Sites of Cobalt Phthalocyanine in Electrocatalytic CO2 Reduction to Methanol
Rooney C, Lyons M, Wu Y, Hu G, Wang M, Choi C, Gao Y, Chang C, Brudvig G, Feng Z, Wang H. Active Sites of Cobalt Phthalocyanine in Electrocatalytic CO2 Reduction to Methanol. Angewandte Chemie International Edition 2023, 63: e202310623. PMID: 37820079, DOI: 10.1002/anie.202310623.Peer-Reviewed Original ResearchActive siteCobalt phthalocyanineSitu X-ray absorption spectroscopyX-ray absorption spectroscopy characterizationX-ray absorption spectroscopyElectrocatalytic CO2 reductionStructure-reactivity correlationsAbsorption spectroscopy characterizationElectrocatalytic measurementsMetal coordinationElectrocatalytic performanceCoordination environmentMolecular dispersionRelated porphyrinsCNT surfaceElectron transferAbsorption spectroscopyConductive carbonElectronic interactionsKey intermediateCO2 reductionPc macrocycleReaction mechanismSpectroscopy characterizationMethanol pathwayActive Sites of Cobalt Phthalocyanine in Electrocatalytic CO2 Reduction to Methanol
Rooney C, Lyons M, Wu Y, Hu G, Wang M, Choi C, Gao Y, Chang C, Brudvig G, Feng Z, Wang H. Active Sites of Cobalt Phthalocyanine in Electrocatalytic CO2 Reduction to Methanol. Angewandte Chemie 2023, 136 DOI: 10.1002/ange.202310623.Peer-Reviewed Original ResearchCO 2 reductionActive siteCobalt phthalocyanineSitu X-ray absorption spectroscopyX-ray absorption spectroscopy characterizationX-ray absorption spectroscopyElectrocatalytic CO2 reductionStructure-reactivity correlationsAbsorption spectroscopy characterizationCO 2 electroreductionCO 2Electrocatalytic measurementsCoordination environmentElectrocatalytic performanceMolecular dispersionRelated porphyrinsCNT surfaceElectron transferAbsorption spectroscopyConductive carbonElectronic interactionsKey intermediateCO2 reductionPc macrocycleReaction mechanism(Invited) Water Oxidation Catalysis with Atomically Defined Active Sites on Nanostructured Materials for Solar Energy Applications
Brudvig G. (Invited) Water Oxidation Catalysis with Atomically Defined Active Sites on Nanostructured Materials for Solar Energy Applications. ECS Meeting Abstracts 2023, MA2023-01: 2149-2149. DOI: 10.1149/ma2023-01372149mtgabs.Peer-Reviewed Original ResearchWater oxidation catalystsMolecular catalystsSolar fuel productionWater oxidationMolecular water oxidation catalystsPhoto-electrochemical water oxidationWater oxidation catalysisNatural photosynthetic systemsPhotoelectrochemical water oxidationMetal oxide surfacesMetal oxide photoanodesFuel productionOxidation catalysisCatalytic performanceOxide photoanodesOxide surfaceNanostructured materialsBioinspired materialsCatalystLimited stabilityActive siteOxide materialsHigh activityPhotosynthetic systemsSolar energy applicationsObservation of Support-Dependent Water Oxidation Kinetics on Molecularly-Derived Heterogeneous Ir-Oxide Catalysts
Zhang H, Liu T, Dulock N, William B, Wang Y, Chen B, Wikar H, Wang D, Brudvig G, Wang D, Waegele M. Observation of Support-Dependent Water Oxidation Kinetics on Molecularly-Derived Heterogeneous Ir-Oxide Catalysts. ECS Meeting Abstracts 2023, MA2023-01: 2154-2154. DOI: 10.1149/ma2023-01372154mtgabs.Peer-Reviewed Original ResearchWater oxidation activityIndium tin oxideActive siteHeterogeneous catalystsOxidation activityHeterogeneous water oxidation catalysisHigh water oxidation activityMost heterogeneous catalystsWater oxidation catalysisWater oxidation catalystsWater oxidation kineticsRate-determining stepOxidation catalysisCeO2 supportSurface chemistryOxidative chargeCatalyst influenceOxidation catalystMolecular structurePhotocatalytic activityCatalystElectronic structureDifferent oxidesTin oxideOxidation kineticsAtomically dispersed Ir catalysts exhibit support-dependent water oxidation kinetics during photocatalysis
Zhang H, Liu T, Dulock N, Williams B, Wang Y, Chen B, Wikar H, Wang D, Brudvig G, Wang D, Waegele M. Atomically dispersed Ir catalysts exhibit support-dependent water oxidation kinetics during photocatalysis. Chemical Science 2023, 14: 6601-6607. PMID: 37350819, PMCID: PMC10283500, DOI: 10.1039/d3sc00603d.Peer-Reviewed Original ResearchWater oxidation activityIndium tin oxideActive siteOxidation activityHeterogeneous water oxidation catalysisHigh water oxidation activityWater oxidation catalysisWater oxidation kineticsOxidation catalysisWater oxidationIr catalystHeterogeneous catalystsDistinct active sitesLight sensitizerPrototypical reactionReaction mechanismDifferent supportsElectron scavengerCatalystTin oxideOxidation kineticsHigh temperatureLow temperatureStudied rangeCatalysis
2020
Cryo-EM Structure of Monomeric Photosystem II from Synechocystis sp. PCC 6803 Lacking the Water-Oxidation Complex
Gisriel C, Zhou K, Huang H, Debus R, Xiong Y, Brudvig G. Cryo-EM Structure of Monomeric Photosystem II from Synechocystis sp. PCC 6803 Lacking the Water-Oxidation Complex. Joule 2020, 4: 2131-2148. DOI: 10.1016/j.joule.2020.07.016.Peer-Reviewed Original ResearchOxygen-evolving complexPhotosystem II enzymeWater oxidation complexWater oxidationMetal clustersMechanism of photoactivationActive siteMonomeric photosystem IIPhotosystem IICryo-EM structureStructural rearrangementsComplexesPhotoactivationSynechocystis spPeripheral subunitsCationsComputational techniquesOxidationOverall biogenesisStructureMesophilic cyanobacteriumOxygenPCC 6803II enzymesPSII
2005
Catalytic Oxygen Evolution by a Bioinorganic Model of the Photosystem II Oxygen-Evolving Complex
Howard D, Tinoco A, Brudvig G, Vrettos J, Allen B. Catalytic Oxygen Evolution by a Bioinorganic Model of the Photosystem II Oxygen-Evolving Complex. Journal Of Chemical Education 2005, 82: 791. DOI: 10.1021/ed082p791.Peer-Reviewed Original ResearchBioinorganic modelsWater oxidationMn4 clusterArtificial water oxidation catalystsBioinorganic model complexesCatalytic oxygen evolutionWater oxidation catalystsPhotosystem IIPhotosynthetic water oxidationUV-visible spectroscopyOxygen-Evolving ComplexDeuterium kinetic isotope effectsPhotosystem II Oxygen Evolving ComplexKinetic isotope effectsBioinorganic chemistryTerpy complexesInorganic synthesisPlace of H2OManganese complexesModel complexesPrimary oxidantManganese clusterOne-electronOxygen evolutionActive siteMechanistic Comparisons Between Photosystem II and Cytochrome c Oxidase
Brudvig G, Wikström M. Mechanistic Comparisons Between Photosystem II and Cytochrome c Oxidase. Advances In Photosynthesis And Respiration 2005, 22: 697-713. DOI: 10.1007/1-4020-4254-x_32.Peer-Reviewed Original ResearchFour-electron reductionSingle reaction stepSame chemical reactionPhotosystem IIRole of protonsOxygen reductionProton transferMolecular oxygenReaction mechanismReaction stepsActive siteWater reactionChemical reactionsRequirement of electronsMechanistic comparisonReverse reactionReactionCytochrome c oxidaseProtonsC oxidaseMechanistic similaritiesChemistryElectronsWaterRespiratory enzymes
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 Research
1999
A Functional Model for O-O Bond Formation by the O2-Evolving Complex in Photosystem II
Limburg J, Vrettos J, Liable-Sands L, Rheingold A, Crabtree R, Brudvig G. A Functional Model for O-O Bond Formation by the O2-Evolving Complex in Photosystem II. Science 1999, 283: 1524-1527. PMID: 10066173, DOI: 10.1126/science.283.5407.1524.Peer-Reviewed Original ResearchConceptsMolecular oxygenPhotosystem IIO bond formationPhotosynthetic water oxidationWater oxidationManganese dimerBond formationOxygen atomsActive siteIsotope labelingManganese ionsOxygenPhotosynthesisWaterSodium hypochloriteOxidationIonsFormationAtomsDimersComplexesO2Functional modelConversionHypochlorite
1995
High-valent oxomanganese clusters: structural and mechanistic work relevant to the oxygen-evolving center in photosystem II
Manchanda R, Brudvig G, Crabtree R. High-valent oxomanganese clusters: structural and mechanistic work relevant to the oxygen-evolving center in photosystem II. Coordination Chemistry Reviews 1995, 144: 1-38. DOI: 10.1016/0010-8545(95)01147-h.Peer-Reviewed Original ResearchO2-evolving centerActive siteOxygen-evolving centerPhotosystem IIOxomanganese clusterBioinorganic chemistryInorganic chemistsWater oxidationComplex chemistryMechanistic aspectsBiophysical studiesChemistryMagnetic propertiesNative enzymeMechanistic workPS IINuclearityChemistsMetalloproteinsSuch clustersConsiderable interestOxidationRecent effortsChemicalsTetramer[22] Electron paramagnetic resonance spectroscopy
Brudvig G. [22] Electron paramagnetic resonance spectroscopy. Methods In Enzymology 1995, 246: 536-554. PMID: 7752937, DOI: 10.1016/0076-6879(95)46024-1.Peer-Reviewed Original ResearchConceptsElectron paramagnetic resonance spectroscopyParamagnetic resonance spectroscopyX-band EPR spectrometerEPR spectroscopyParamagnetic speciesResonance spectroscopyParamagnetic centersBiological systemsEPR spectrometerRedox reactionsDiamagnetic proteinsEPR spectraActive siteEPR methodSpectroscopySample requirementsSpectrometerEPRReactionValuable techniqueSpectraApplicationsSpeciesStructure