2024
Structure of a biohybrid photosystem I-platinum nanoparticle solar fuel catalyst
Gisriel C, Malavath T, Qiu T, Menzel J, Batista V, Brudvig G, Utschig L. Structure of a biohybrid photosystem I-platinum nanoparticle solar fuel catalyst. Nature Communications 2024, 15: 9519. PMID: 39496605, PMCID: PMC11535483, DOI: 10.1038/s41467-024-53476-y.Peer-Reviewed Original ResearchLight-driven H2 productionFuel catalystUnity quantum efficiencyPhotosynthetic biohybrid systemsPigment-protein complexesLight-driven enzymePlatinum nanoparticlesH2 productionQuantum efficiencyPhotosystem I complexCatalystChemical energyCryo-EM structureResolution cryo-EM structureBiohybrid systemsFuel productionStored solar energyPhotosystem IBiology platformReducing equivalentsMolecular basisI complexSolar energyBinding sitesStructureModeling Electrochemical Vacancy Regeneration in Single-Walled Carbon Nanotubes
Jelušić J, Menzel J, Bertrand Q, Crabtree R, Wang H, Brudvig G, Batista V. Modeling Electrochemical Vacancy Regeneration in Single-Walled Carbon Nanotubes. The Journal Of Physical Chemistry Letters 2024, 15: 7788-7792. PMID: 39048317, DOI: 10.1021/acs.jpclett.4c01293.Peer-Reviewed Original ResearchProton-coupled electron transferDensity functional theorySingle-walled carbon nanotubesC-H bondsQuantum mechanics/molecular mechanicsDiverse catalytic reactionsCarbene characterCarbon nanotubesC-HAdjacent carbonWater dissociationElectron transferCatalytic reactionsCatalytic intermediatesFunctional theoryHydrogen atomsKetone groupForce-fieldCarbon atomsHydroxyl groupsElectrochemical regenerationZigzag single-walled carbon nanotubesElectrochemical potentialKetonesVacancy defectsAssignment of chlorophyll d in the ChlD1 site of the electron transfer chain of far-red light acclimated photosystem II supported by MCCE binding calculations
Gisriel C, Ranepura G, Brudvig G, Gunner M. Assignment of chlorophyll d in the ChlD1 site of the electron transfer chain of far-red light acclimated photosystem II supported by MCCE binding calculations. Biochimica Et Biophysica Acta (BBA) - Bioenergetics 2024, 1865: 149496. PMID: 39038640, DOI: 10.1016/j.bbabio.2024.149496.Peer-Reviewed Original ResearchElectron Transfer Dynamics at Dye-Sensitized SnO2/TiO2 Core/Shell Electrodes in Aqueous/Nonaqueous Electrolyte Mixtures
Xiao L, Spies J, Sheehan C, Zeng Z, Gao Y, Gao T, Ehrlacher A, Zuerch M, Brudvig G, Mallouk T. Electron Transfer Dynamics at Dye-Sensitized SnO2/TiO2 Core/Shell Electrodes in Aqueous/Nonaqueous Electrolyte Mixtures. Journal Of The American Chemical Society 2024, 146: 18117-18127. PMID: 38900942, DOI: 10.1021/jacs.4c05187.Peer-Reviewed Original ResearchFlat band potentialOptical-pump terahertz-probe spectroscopyTransient absorption spectroscopyCore/shell electrodesSolvent electrolytesElectron transferElectron injectionBand potentialDynamics of photoinduced electron transferNanosecond transient absorption spectroscopyNegative flat band potentialSemiconductor flat-band potentialDye-sensitized photoanodeOxidized dye moleculesPhotoinduced electron injectionPhotoinduced electron transferElectron transfer dynamicsElectron injection efficiencySlow electron transferInjection efficiencyIncreasing acetonitrile concentrationConcentration of acetonitrileIncreasing concentrations of acetonitrileConduction band electronsCharge separationMutation-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 oxidationWater 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 bindingCatalystIsomerizationPhotochemical Oxidation of Substrate Water Analogs and Halides by Photosystem II
Shin J, Kanyo J, Debus R, Brudvig G. Photochemical Oxidation of Substrate Water Analogs and Halides by Photosystem II. Advanced Energy Materials 2024, 14 DOI: 10.1002/aenm.202401292.Peer-Reviewed Original ResearchWater oxidation catalysisRedox-active cofactorsOxidation catalysisWater oxidationSubstrate photooxidationProtein-pigment complexesRedox chemistryPhotochemical reductionSubstrate waterNative PSIISmall moleculesO 2 evolutionHalidesO-2ChloridePhotooxidationPhotochemical oxidationPSII complexesBound chlorideKinetic profilesPhotosystem IISubstratePutative water channelsCatalystCatalysisBODIPY Chemisorbed on SnO2 and TiO2 Surfaces for Photoelectrochemical Applications
Jayworth J, Decavoli C, Capobianco M, Menzel J, Adler S, Kocoj C, Freeze J, Crabtree R, Guo P, Batista V, Brudvig G. BODIPY Chemisorbed on SnO2 and TiO2 Surfaces for Photoelectrochemical Applications. ACS Applied Materials & Interfaces 2024, 16: 14841-14851. PMID: 38488153, DOI: 10.1021/acsami.3c18827.Peer-Reviewed Original ResearchCarboxylic acid anchoring groupsAnchoring groupsElectron injectionSolar-driven water splittingTransient absorption spectroscopic studiesDye-sensitized photoelectrochemical cellsEfficiency of electron injectionSacrificial electron donorEfficient electron injectionElectron-hole recombinationAbsorption spectroscopic studiesBODIPY-based dyesWater splittingPhotoelectrochemical applicationsPhotoelectrochemical cellsSemiconducting photoelectrodesTiO2 surfacePhotoelectrochemical studiesPhotoexcited dyeSolar fuelsCharge transferMetal oxidesBinding modeCarboxylic acidsSpectroscopic studiesOccupancy Analysis of Water Molecules inside Channels within 25 Å Radius of the Oxygen-Evolving Center of Photosystem II in Molecular Dynamics Simulations
Kaur D, Reiss K, Wang J, Batista V, Brudvig G, Gunner M. Occupancy Analysis of Water Molecules inside Channels within 25 Å Radius of the Oxygen-Evolving Center of Photosystem II in Molecular Dynamics Simulations. The Journal Of Physical Chemistry B 2024, 128: 2236-2248. PMID: 38377592, DOI: 10.1021/acs.jpcb.3c05367.Peer-Reviewed Original ResearchOxygen-evolving centerWater moleculesPhotosystem IIPositions of water moleculesAnalysis of water moleculesCatalyze water oxidationHydrogen bond networkOccupancy of water moleculesMolecular dynamics simulationsD1-D61Electron density mapsMolecular dynamics analysisProton transferWater oxidationCrystallographic dataIce latticeMD simulationsMolecular dynamicsStructural transitionDynamics simulationsSubstrate waterOxygen-evolvingRoom temperatureProtein residuesMoleculesSelecting between Ammonia and Water Oxidation: Electrochemical Oxidation of Ammonia in Water Using an Organometallic–Inorganic Hybrid Anode
Liu H, Jayworth J, Crabtree R, Brudvig G. Selecting between Ammonia and Water Oxidation: Electrochemical Oxidation of Ammonia in Water Using an Organometallic–Inorganic Hybrid Anode. ACS Catalysis 2024, 14: 2842-2846. DOI: 10.1021/acscatal.3c05899.Peer-Reviewed Original ResearchHybrid anodeWater oxidationBlue layerElectrochemical oxidation of ammoniaOxidation of ammoniaElectrochemical oxidationSurface poisoningAqueous solventAmmonia oxidationOptimal operating conditionsAqueous solutionAmbient conditionsE appOperating conditionsAnodeFormation of nitriteOxidationOptimum selectionAmmoniaSolventNitrateNanoclustersDinitrogenElectrodeEcofriendly productsMapping the Oxygens in the Oxygen-Evolving Complex of Photosystem II by Their Nucleophilicity Using Quantum Descriptors
Amin M, Kaur D, Brudvig G, Brooks B. Mapping the Oxygens in the Oxygen-Evolving Complex of Photosystem II by Their Nucleophilicity Using Quantum Descriptors. Journal Of Chemical Theory And Computation 2024, 20: 1414-1422. PMID: 38306696, DOI: 10.1021/acs.jctc.3c00926.Peer-Reviewed Original ResearchConceptual density functional theoryOxygen-evolving complexQuantum descriptorsBridging oxygenSolar energy to chemical energyEnergy to chemical energyWater splitting reactionOxygen-evolving complex of photosystem IIReactivity of moleculesDensity functional theoryComplex of photosystem IIDual descriptorFukui functionsNucleophilic attackTerminal waterArtificial catalystsAtomic contributionsModel compoundsFunctional theoryReaction mechanismNucleophilesPhotosystem IIElectrophilesMn4Chemical energyManipulating Photoconduction in Cu–Pyrene 1‑D Coordination Nanosheets by Modulating Interlayer π–π Stacking
Nyakuchena J, Ostresh S, Streater D, Chiromo H, Wilkes J, Lindeman S, Wang D, Neu J, Brudvig G, Huang J. Manipulating Photoconduction in Cu–Pyrene 1‑D Coordination Nanosheets by Modulating Interlayer π–π Stacking. The Journal Of Physical Chemistry C 2024, 128: 315-320. DOI: 10.1021/acs.jpcc.3c07690.Peer-Reviewed Original ResearchOptical Pump THz Probe Spectroscopy on Metal-Organic Frameworks
Ostresh S, Nyakuchena J, Streater D, Wang D, Cody C, Hooper R, Zhang X, Reinhart B, Ma Q, He P, Brudvig G, Huang J, Neu J. Optical Pump THz Probe Spectroscopy on Metal-Organic Frameworks. 2024, fw4i.3. DOI: 10.1364/cleo_fs.2024.fw4i.3.Peer-Reviewed Original ResearchMetal-organic frameworksOptical pump-THz probePorous crystalline metal-organic frameworksCrystalline metal-organic frameworksCatalytic activity measurementsElectro-optical applicationsMetal centerProbe spectroscopyOptical pump-THz probe spectroscopyUltrafast photoconductivityPhotoconductivityTHz-probe spectroscopyPhotophysicsCatalysisChemical compositionTHz probeSpectroscopyMaterialsMetalChemical
2023
Infrared Spectroscopic Observation of Oxo- and Superoxo-Intermediates in the Water Oxidation Cycle of a Molecular Ir Catalyst
Zhang H, Chen B, Liu T, Brudvig G, Wang D, Waegele M. Infrared Spectroscopic Observation of Oxo- and Superoxo-Intermediates in the Water Oxidation Cycle of a Molecular Ir Catalyst. Journal Of The American Chemical Society 2023, 146: 878-883. PMID: 38154046, DOI: 10.1021/jacs.3c11206.Peer-Reviewed Original ResearchStructure of the antenna complex expressed during far-red light photoacclimation in Synechococcus sp. PCC 7335
Gisriel C, Shen G, Brudvig G, Bryant D. Structure of the antenna complex expressed during far-red light photoacclimation in Synechococcus sp. PCC 7335. Journal Of Biological Chemistry 2023, 300: 105590. PMID: 38141759, PMCID: PMC10810746, DOI: 10.1016/j.jbc.2023.105590.Peer-Reviewed Original ResearchComputing the Relative Affinity of Chlorophylls a and b to Light-Harvesting Complex II
Ranepura G, Mao J, Vermaas J, Wang J, Gisriel C, Wei R, Ortiz-Soto J, Uddin R, Amin M, Brudvig G, Gunner M. Computing the Relative Affinity of Chlorophylls a and b to Light-Harvesting Complex II. The Journal Of Physical Chemistry B 2023, 127: 10974-10986. PMID: 38097367, DOI: 10.1021/acs.jpcb.3c06273.Peer-Reviewed Original ResearchBridging 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 mechanismMolecular diversity and evolution of far-red light-acclimated photosystem I
Gisriel C, Bryant D, Brudvig G, Cardona T. Molecular diversity and evolution of far-red light-acclimated photosystem I. Frontiers In Plant Science 2023, 14: 1289199. PMID: 38053766, PMCID: PMC10694217, DOI: 10.3389/fpls.2023.1289199.Peer-Reviewed Original Research