2021
Observation of a potential-dependent switch of water-oxidation mechanism on Co-oxide-based catalysts
Lang C, Li J, Yang K, Wang Y, He D, Thorne J, Croslow S, Dong Q, Zhao Y, Prostko G, Brudvig G, Batista V, Waegele M, Wang D. Observation of a potential-dependent switch of water-oxidation mechanism on Co-oxide-based catalysts. Chem 2021, 7: 2101-2117. DOI: 10.1016/j.chempr.2021.03.015.Peer-Reviewed Original ResearchWater oxidation mechanismWater oxidation reactionWater nucleophilic attack mechanismCo-based catalystsO bond formationNucleophilic attack mechanismKey elementary stepsHeterogeneous catalystsSalt electrolyteElectrode potentialApplied potentialBond formationLow driving forceO couplingElementary stepsMechanistic switchCatalystHigh driving forceDriving forceReactionAttack mechanismWater activityElectrolyteHereinPotential
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
Formate to Oxalate: A Crucial Step for the Conversion of Carbon Dioxide into Multi‐carbon Compounds
Lakkaraju P, Askerka M, Beyer H, Ryan C, Dobbins T, Bennett C, Kaczur J, Batista V. Formate to Oxalate: A Crucial Step for the Conversion of Carbon Dioxide into Multi‐carbon Compounds. ChemCatChem 2016, 8: 3453-3457. DOI: 10.1002/cctc.201600765.Peer-Reviewed Original ResearchMulti-carbon compoundsDensity functional theory calculationsSelective catalytic conversionIndustrial-scale synthesisFunctional theory calculationsChain reaction mechanismCatalytic performanceIon catalystAlkali formateIon catalysisConversion of formateBond formationCatalytic conversionQuantitative conversionIon intermediateReaction conditionsRaman spectroscopyTheory calculationsReaction mechanismCatalytic mechanismSodium hydrideOxalate saltsSodium formateFormateEfficient conversion
2015
Triplet Oxygen Evolution Catalyzed by a Biomimetic Oxomanganese Complex: Functional Role of the Carboxylate Buffer
Rivalta I, Yang K, Brudvig G, Batista V. Triplet Oxygen Evolution Catalyzed by a Biomimetic Oxomanganese Complex: Functional Role of the Carboxylate Buffer. ACS Catalysis 2015, 5: 2384-2390. DOI: 10.1021/acscatal.5b00048.Peer-Reviewed Original ResearchOxomanganese complexesTriplet oxygenOxygen evolutionWater splittingCatalytic oxygen evolutionO bond formationBiomimetic oxomanganese complexesNucleophilic water moleculeUnderlying reaction mechanismGreen plant chloroplastsPhotosynthetic oxygen evolutionWater ligandsCarboxylate ligandsInorganic coreMn complexesSuperoxo speciesNoninnocent roleCarboxylate groupsWater moleculesSubstrate waterBond formationSynthetic complexesCarboxylate buffersNucleophilic attackRedox potential