2018
Water-Nucleophilic Attack Mechanism for the CuII(pyalk)2 Water-Oxidation Catalyst
Rudshteyn B, Fisher K, Lant H, Yang K, Mercado B, Brudvig G, Crabtree R, Batista V. Water-Nucleophilic Attack Mechanism for the CuII(pyalk)2 Water-Oxidation Catalyst. ACS Catalysis 2018, 8: 7952-7960. DOI: 10.1021/acscatal.8b02466.Peer-Reviewed Original ResearchKinetic isotope effectsWater nucleophilic attack mechanismWater oxidation catalystsWater nucleophilic attackD Kinetic Isotope EffectO bond formationUV-visible spectraDensity functional theoryElectrochemical stepWater oxidationElectrochemical analysisTurnover frequencyDerivative complexesBond formationRadical speciesRational designCis formFunctional theoryIsotope effectRate-limiting stepCatalystComplexesAttack mechanismMechanistic findingsDeprotonation
2016
Heterogenized Iridium Water-Oxidation Catalyst from a Silatrane Precursor
Materna K, Rudshteyn B, Brennan B, Kane M, Bloomfield A, Huang D, Shopov D, Batista V, Crabtree R, Brudvig G. Heterogenized Iridium Water-Oxidation Catalyst from a Silatrane Precursor. ACS Catalysis 2016, 6: 5371-5377. DOI: 10.1021/acscatal.6b01101.Peer-Reviewed Original ResearchIridium Water Oxidation CatalystsMetal oxide semiconductor surfacesWater oxidation catalystsExperimental IR spectraOxide semiconductor surfaceWater oxidationHeterogenized catalystTurnover frequencyIR spectraSilatrane precursorCovalent attachmentFunctional groupsTurnover numberM KNO3CatalystSemiconductor surfacesPrecatalystOverpotentialCatalysisComputational modelingOxidationPrecursorsKNO3SpectraSurface
2015
Behavior of the Ru-bda Water Oxidation Catalyst Covalently Anchored on Glassy Carbon Electrodes
Matheu R, Francàs L, Chernev P, Ertem M, Batista V, Haumann M, Sala X, Llobet A. Behavior of the Ru-bda Water Oxidation Catalyst Covalently Anchored on Glassy Carbon Electrodes. ACS Catalysis 2015, 5: 3422-3429. DOI: 10.1021/acscatal.5b00132.Peer-Reviewed Original ResearchWater oxidation catalystsX-ray absorption spectroscopyElectrode surfaceHybrid materialsGlassy carbonOxidation catalystHeterogeneous water oxidation catalystsGC electrode surfaceGlassy carbon electrodeRu-aqua complexesLow catalytic performanceOxidation of waterNew hybrid materialsGC electrodeElectrochemical reductionCarbon electrodeCovalent graftingActive catalystGood electrocatalystCatalytic performanceVoltammetric experimentsElectrochemical techniquesMetal oxidesAbsorption spectroscopyMolecular complexes
2014
Linker Rectifiers for Covalent Attachment of Transition‐Metal Catalysts to Metal‐Oxide Surfaces
Ding W, Negre CF, Palma JL, Durrell AC, Allen LJ, Young KJ, Milot RL, Schmuttenmaer CA, Brudvig GW, Crabtree RH, Batista VS. Linker Rectifiers for Covalent Attachment of Transition‐Metal Catalysts to Metal‐Oxide Surfaces. ChemPhysChem 2014, 15: 1138-1147. PMID: 24668518, DOI: 10.1002/cphc.201400063.Peer-Reviewed Original ResearchInterfacial electron transferElectron transferWater oxidation catalystsTransition metal catalystsElectron transfer propertiesBack electron transferMetal oxide surfacesElectron paramagnetic resonanceAcetylacetonate groupTerpyridyl groupsElectrode surfaceOxidation catalystMolecular linkersElectron reactionsAmide bondTiO2 surfaceParamagnetic resonanceCovalent attachmentAmide linkageTerahertz spectroscopic measurementsSpectroscopic measurementsElectron injectionTransfer propertiesLinkerCatalyst
2013
A Self‐Improved Water‐Oxidation Catalyst: Is One Site Really Enough?
López I, Ertem M, Maji S, Benet‐Buchholz J, Keidel A, Kuhlmann U, Hildebrandt P, Cramer C, Batista V, Llobet A. A Self‐Improved Water‐Oxidation Catalyst: Is One Site Really Enough? Angewandte Chemie International Edition 2013, 53: 205-209. PMID: 24259487, DOI: 10.1002/anie.201307509.Peer-Reviewed Original ResearchWater oxidation catalystsRobust water oxidation catalystsTransition metal complexesLarge turnover frequencyDFT computational analysisInterconnected catalytic cyclesMononuclear catalystsHomogeneous catalysisWater oxidationRobust catalystsTurnover frequencyEnergy conversion schemeCatalytic processCatalytic cycleMononuclear systemsCatalystDinuclear systemCatalysisComputational analysisOxidationSpectacular developmentHereinComplexesA Self‐Improved Water‐Oxidation Catalyst: Is One Site Really Enough?
López I, Ertem M, Maji S, Benet‐Buchholz J, Keidel A, Kuhlmann U, Hildebrandt P, Cramer C, Batista V, Llobet A. A Self‐Improved Water‐Oxidation Catalyst: Is One Site Really Enough? Angewandte Chemie 2013, 126: 209-213. DOI: 10.1002/ange.201307509.Peer-Reviewed Original ResearchWater oxidation catalystsRobust water oxidation catalystsTransition metal complexesLarge turnover frequencyDFT computational analysisInterconnected catalytic cyclesMononuclear catalystsHomogeneous catalysisWater oxidationRobust catalystsTurnover frequencyEnergy conversion schemeCatalytic processCatalytic cycleMononuclear systemsCatalystDinuclear systemCatalysisComputational analysisOxidationSpectacular developmentHereinComplexes
2010
Study of Proton Coupled Electron Transfer in a Biomimetic Dimanganese Water Oxidation Catalyst with Terminal Water Ligands
Wang T, Brudvig GW, Batista VS. Study of Proton Coupled Electron Transfer in a Biomimetic Dimanganese Water Oxidation Catalyst with Terminal Water Ligands. Journal Of Chemical Theory And Computation 2010, 6: 2395-2401. PMID: 20827389, PMCID: PMC2935188, DOI: 10.1021/ct1002658.Peer-Reviewed Original ResearchTerminal water ligandsWater ligandsOxomanganese complexesElectron transferRedox potentialProton Coupled Electron TransferWater oxidation catalystsCyclic voltammogram measurementsLewis base moietyOxidation of waterFree energy calculationsInorganic coreOxidation potentialOxidation statePrimary oxidantOxidation catalystMn centersBase moietyEnergy calculationsBiomimetic modelLigandsAnalogous conversionOxidationFree energyPhotosystem II
2009
Reversible Visible-Light Photooxidation of an Oxomanganese Water-Oxidation Catalyst Covalently Anchored to TiO2 Nanoparticles
Li G, Sproviero EM, McNamara WR, Snoeberger RC, Crabtree RH, Brudvig GW, Batista VS. Reversible Visible-Light Photooxidation of an Oxomanganese Water-Oxidation Catalyst Covalently Anchored to TiO2 Nanoparticles. The Journal Of Physical Chemistry B 2009, 114: 14214-14222. PMID: 19924873, DOI: 10.1021/jp908925z.Peer-Reviewed Original ResearchPolynuclear transition metal complexesWater oxidation catalystsTransition metal complexesArtificial photosynthetic assembliesVisible-light photoexcitationInterfacial electron transferOxidation chemistryPhotosynthetic assembliesWater oxidationHomogeneous catalystsElectron transferEPR spectroscopyCharge separationManganese compoundsAmide bondCovalent attachmentVisible lightTiO2 nanoparticlesPhotocatalytic devicesNanoparticlesElectron scavengerInexpensive materialsElectron acceptorOxidative conditionsStructural propertiesDeposition of an oxomanganese water oxidation catalyst on TiO 2 nanoparticles : computational modeling, assembly and characterization
Li G, Sproviero E, Snoeberger R, Iguchi N, Blakemore J, Crabtree R, Brudvig G, Batista V. Deposition of an oxomanganese water oxidation catalyst on TiO 2 nanoparticles : computational modeling, assembly and characterization. Energy & Environmental Science 2009, 2: 230-238. DOI: 10.1039/b818708h.Peer-Reviewed Original ResearchWater oxidation catalystsOxidation catalystTiO2 nanoparticlesUV-visible spectroscopyTiO 2 nanoparticlesMixed valence stateAmorphous TiO2 nanoparticlesWater ligandsElectrochemical studiesElectrochemical measurementsEPR spectroscopySurface complexesMimic photosynthesisDirect adsorptionSitu synthesisTiO2 surfaceSuccessful attachmentEPR dataNanoparticlesCatalystSolar cellsSpectroscopyComputational modelingAdsorptionEPR