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dc.contributor.authorLee, Yueh Lin
dc.contributor.authorGadre, milind Jayram
dc.contributor.authorShao-Horn, Yang
dc.contributor.authorMorgan, Dane
dc.date.accessioned2017-07-11T13:40:39Z
dc.date.available2017-07-11T13:40:39Z
dc.date.issued2015-07
dc.date.submitted2015-01
dc.identifier.issn1463-9076
dc.identifier.issn1463-9084
dc.identifier.urihttp://hdl.handle.net/1721.1/110618
dc.description.abstractIn this work, we performed density functional theory (DFT) calculations with inclusion of Hubbard U corrections for the transition metal d-electrons, to investigate stability and electrocatalytic activities of the oxygen evolution reaction (OER) and oxygen reduction reaction (ORR) for the ABO3 (A = La; B = Cr, Mn, Fe, Co, and Ni) (001) surfaces. We showed surface binding energies of relevant ORR/OER species are coupled strongly to surface polarity and local oxidation states, giving large (∼1 eV scale per adsorbate) differences in binding between (001) AO and BO2 surfaces, where the more oxidized BO2 bare surfaces in general exhibit weak coverage dependence, while the more reduced AO bare surfaces of the LaCrO3, LaMnO3, and LaFeO3 perovskites with lower d-electron filling show strong/moderate coverage dependences. We then predicted that surface coverage can play a key role in determining surface stability, and when coverage effects are included the AO and BO2(001) surfaces have either similar stability or the AO surface is more stable, as found for 1 monolayer HO* covered AO surfaces of LaCrO3 and LaFeO3 under ORR conditions and 1 monolayer O* covered LaNiO3 AO surface under OER conditions. For the (001) AO surfaces with strong coverage dependent surface adsorption, we predicted a decrease in ORR overpotential of 1–2 V with proper treatment of coverage effects as compared to those of the bare surface simulations. Our results indicated that the GGA+U method and proper treatment of coverage effects more accurately predict ORR and OER overpotentials relative to experimental values as compared to the GGA method and bare surfaces. The overall ORR activity trends vs. the LaBO3 series were predicted to be Co > Mn ≈ Ni > Fe > Cr.en_US
dc.description.sponsorshipUnited States. Department of Energy. Solid State Energy Conversion Allianc. Core Technology Program (Funding Opportunity No. DEFE0009435)en_US
dc.description.sponsorshipNational Science Foundation (U.S.). Software Intrastructure for Sustained Innovation (award No. 1148011)en_US
dc.description.sponsorshipSkoltech-MIT Center for Electrochemical Energyen_US
dc.description.sponsorshipOak Ridge National Laboratory. Center for Nanophase Materials Sciences (grant number CNMS2013-292)en_US
dc.language.isoen_US
dc.publisherRoyal Society of Chemistry (Great Britain)en_US
dc.relation.isversionofhttp://dx.doi.org/10.1039/c5cp02834een_US
dc.rightsCreative Commons Attribution-Noncommercial-Share Alikeen_US
dc.rights.urihttp://creativecommons.org/licenses/by-nc-sa/4.0/en_US
dc.sourceProf. Shao-Horn via Angie Locknaren_US
dc.titleAb initio GGA+U study of oxygen evolution and oxygen reduction electrocatalysis on the (001) surfaces of lanthanum transition metal perovskites LaBOen_US
dc.typeArticleen_US
dc.identifier.citationLee, Yueh-Lin, Milind J. Gadre, Yang Shao-Horn, and Dane Morgan. “Ab Initio GGA+U Study of Oxygen Evolution and Oxygen Reduction Electrocatalysis on the (001) Surfaces of Lanthanum Transition Metal Perovskites LaBO3 (B = Cr, Mn, Fe, Co and Ni).” Phys. Chem. Chem. Phys. 17, no. 33 (2015): 21643–21663.en_US
dc.contributor.departmentMassachusetts Institute of Technology. Department of Materials Science and Engineeringen_US
dc.contributor.departmentMassachusetts Institute of Technology. Department of Mechanical Engineeringen_US
dc.contributor.departmentMassachusetts Institute of Technology. Research Laboratory of Electronicsen_US
dc.contributor.approverShao-Horn, Yangen_US
dc.contributor.mitauthorLee, Yueh Lin
dc.contributor.mitauthorGadre, milind Jayram
dc.contributor.mitauthorShao-Horn, Yang
dc.contributor.mitauthorMorgan, Dane
dc.relation.journalPhys. Chem. Chem. Phys.en_US
dc.eprint.versionAuthor's final manuscripten_US
dc.type.urihttp://purl.org/eprint/type/JournalArticleen_US
eprint.statushttp://purl.org/eprint/status/PeerRevieweden_US
dspace.orderedauthorsLee, Yueh-Lin; Gadre, Milind J.; Shao-Horn, Yang; Morgan, Daneen_US
dspace.embargo.termsNen_US
dc.identifier.orcidhttps://orcid.org/0000-0003-2477-6412
mit.licenseOPEN_ACCESS_POLICYen_US


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