2024
Water Ligands Regulate the Redox Leveling Mechanism of the Oxygen-Evolving Complex of the Photosystem II
Liu J, Yang K, Long Z, Armstrong W, Brudvig G, Batista V. Water Ligands Regulate the Redox Leveling Mechanism of the Oxygen-Evolving Complex of the Photosystem II. Journal Of The American Chemical Society 2024, 146: 15986-15999. PMID: 38833517, DOI: 10.1021/jacs.4c02926.Peer-Reviewed Original ResearchProton-coupled electron transferOxygen-evolving complexWater insertionWater ligandsCatalytic cycleMolecular dynamicsO-O bondQuantum mechanics/molecular mechanicsConformational changesFree energy changeLigand environmentElectron transferLigand exchangePhotosystem IIOxygen evolutionWater binding mechanismsEnergy changeLigandBinding mechanismAqueous environmentRedoxWater bindingLigand bindingCatalystIsomerization
2019
Synthesis and Reactivity of Paramagnetic Nickel Polypyridyl Complexes Relevant to C(sp2)–C(sp3)Coupling Reactions
Beromi M, Brudvig G, Hazari N, Lant H, Mercado B. Synthesis and Reactivity of Paramagnetic Nickel Polypyridyl Complexes Relevant to C(sp2)–C(sp3)Coupling Reactions. Angewandte Chemie 2019, 131: 6155-6159. DOI: 10.1002/ange.201901866.Peer-Reviewed Original Research
2017
Antimony Complexes for Electrocatalysis: Activity of a Main‐Group Element in Proton Reduction
Jiang J, Materna K, Hedström S, Yang K, Crabtree R, Batista V, Brudvig G. Antimony Complexes for Electrocatalysis: Activity of a Main‐Group Element in Proton Reduction. Angewandte Chemie 2017, 129: 9239-9243. DOI: 10.1002/ange.201704700.Peer-Reviewed Original ResearchMain group catalysisRedox-active ligandsMain group complexesQuantum chemistry calculationsMain group elementsViable electrocatalystsPorphyrin ligandChemistry calculationsHydroxy ligandsElectrocatalysis applicationsProton reductionCatalytic propertiesAntimony complexesRedox activityAxial ligandsCatalytic cycleSb centerLigandsCatalysisComplexesElectrocatalysisElectrocatalystsPorphyrinsReactionAcid
2013
Water oxidation chemistry of photosystem II
Brudvig G. Water oxidation chemistry of photosystem II. The FASEB Journal 2013, 27: 98.1-98.1. DOI: 10.1096/fasebj.27.1_supplement.98.1.Peer-Reviewed Original ResearchOxygen-evolving complexWater oxidation chemistryOxidation chemistryCrystal structurePhotosystem IISubstrate water moleculesRedox-active tyrosinesX-ray crystal structureFour-electron oxidationIntermediate oxidation statesSolar fuel productionSignificant side reactionsSpecific redox stateCyanobacterial photosystem IIDesign of materialsInorganic chemistryX-ray crystallographic informationRedox stateOxidation stateWater moleculesCatalytic cycleENDOR spectroscopySide reactionsChemical problemsSpectroscopic data3.15 Complex Systems: Photosynthesis
Pokhrel R, Brudvig G. 3.15 Complex Systems: Photosynthesis. 2013, 385-422. DOI: 10.1016/b978-0-08-097774-4.00313-2.Peer-Reviewed Original ResearchOxygen-evolving complexQuantum mechanics/molecular mechanicsPhotosystem IIOO bond formationDensity functional theory calculationsComplete catalytic cycleFunctional theory calculationsProton exit pathwayIron-sulfur centersMetal centerNatural photosynthesisModel complexesCatalytic cycleBond formationMolecular mechanicsFunctional mimicsElectronic characterizationTheory calculationsRole of chlorideOxygenic photosynthesisComplexesDetailed mechanismExit pathwayHydrogenasesPlastocyanin
2012
A tridentate Ni pincer for aqueous electrocatalytic hydrogen production
Luca O, Konezny S, Blakemore J, Colosi D, Saha S, Brudvig G, Batista V, Crabtree R. A tridentate Ni pincer for aqueous electrocatalytic hydrogen production. New Journal Of Chemistry 2012, 36: 1149-1152. DOI: 10.1039/c2nj20912h.Peer-Reviewed Original Research
2008
Quantum Mechanics/Molecular Mechanics Study of the Catalytic Cycle of Water Splitting in Photosystem II
Sproviero EM, Gascón JA, McEvoy JP, Brudvig GW, Batista VS. Quantum Mechanics/Molecular Mechanics Study of the Catalytic Cycle of Water Splitting in Photosystem II. Journal Of The American Chemical Society 2008, 130: 3428-3442. PMID: 18290643, DOI: 10.1021/ja076130q.Peer-Reviewed Original ResearchConceptsSubstrate water moleculesWater moleculesMu-oxo bridgeOxygen-evolving complexWater splittingQuantum mechanics/molecular mechanics (QM/MM) hybrid methodsQuantum Mechanics/Molecular Mechanics StudySolar fuel production systemsPhotosystem IIX-ray diffraction structureMolecular mechanics studySecond coordination shellCyanobacterium Thermosynechococcus elongatusOxomanganese clusterDioxygen evolutionTerminal ligandsXRD structureCatalytic clustersCP43-R357Ligand exchangeCatalytic reactionCatalytic cycleReaction intermediatesS0 stateNucleophilic attack
1989
Oxidation of exogenous substrates by the O2-evolving center of photosystem II and related catalytic air oxidation of secondary alcohols via a tetranuclear manganese(IV) complex.
Beck W, Sears J, Brudvig G, Kulawiec R, Crabtree* R. Oxidation of exogenous substrates by the O2-evolving center of photosystem II and related catalytic air oxidation of secondary alcohols via a tetranuclear manganese(IV) complex. Tetrahedron 1989, 45: 4903-4911. DOI: 10.1016/s0040-4020(01)85159-0.Peer-Reviewed Original ResearchMn complexesH2O oxidationOxidation stateAir oxidationStrong oxidantsSecondary alcoholsPhotosynthetic H2O oxidationPhotosystem IIS1 stateLower oxidation statesCatalytic air oxidationLight-driven generationO2 evolution activityOxidation chemistryO2-evolving centerCatalytic cycleOxidizing statePrimary aminesSecondary aminesReductive mechanismOxidationComplexesExogenous ligandsCenter actsOxidants