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Structure, electrical conductivity and oxygen transport properties of Ruddlesden–Popper phases Lnn+1NinO3n+1 (Ln = La, Pr and Nd; n = 1, 2 and 3)

hal.structure.identifierInstitute for Nanotechnology [MESA+]
dc.contributor.authorSONG, Jia
hal.structure.identifierHelmholtz-Zentrum Berlin für Materialien und Energie GmbH = Helmholtz Centre Berlin for Materials and Energy = Centre Helmholtz de Berlin pour les matériaux et l'énergie [HZB]
dc.contributor.authorNING, De
hal.structure.identifierInstitute for Nanotechnology [MESA+]
dc.contributor.authorBOUKAMP, Bernard
hal.structure.identifierInstitut de Chimie de la Matière Condensée de Bordeaux [ICMCB]
dc.contributor.authorBASSAT, Jean-Marc.
hal.structure.identifierInstitute for Nanotechnology [MESA+]
hal.structure.identifierCAS Key Laboratory of Materials for Energy Conversion
hal.structure.identifierInstitute of Energy and Climate Research: Materials Synthesis and Processing [IEK-1]
dc.contributor.authorBOUWMEESTER, Henny J. M.
dc.date.issued2020-11-03
dc.identifier.issn2050-7488
dc.description.abstractEnLayered Ruddlesden–Popper (RP) lanthanide nickelates, Lnn+1NinO3n+1 (Ln = La, Pr and Nd; n = 1, 2 and 3), are considered potential cathode materials in solid oxide fuel cells. In this study, the thermal evolution of the structure, oxygen nonstoichiometry, electrical conductivity and oxygen transport properties of La2NiO4+δ, Nd2NiO4+δ, La3Ni2O7−δ, La4Ni3O10−δ, Pr4Ni3O10−δ and Nd4Ni3O10−δ are investigated. Phase transitions involving a disruption of the cooperative tilting of the perovskite layers in the low-temperature structure thereby transforming it to a more symmetric structure are observed in several of the materials upon heating in air. Pr4Ni3O10−δ and Nd4Ni3O10−δ show no phase transition from room temperature up to 1000 °C. High density ceramics (>96%) are obtained after sintering at 1300 °C and (for n = 2 and n = 3 members) post-sintering annealing at reduced temperatures. Data for the electrical conductivity measurements on these specimens indicate itinerant behaviour of the charge carriers in the RP nickelates. The increase in p-type conductivity with the order n of the RP phase is interpreted as arising from the concomitant increase in the formal valence of Ni. The observations can be interpreted in terms of a simple energy band scheme, showing that electron holes are formed in the σx2−y2↑ band upon increasing the oxidation state of Ni. Electrical conductivity relaxation measurements reveal remarkable similarities between the surface exchange coefficients (kchem) of the different RP phases despite the differences in the order parameter n and the nature of the lanthanide ion. Calculation of the oxygen self-diffusion coefficients (Ds) from the experimental values of the chemical diffusion coefficients (Dchem), using the corresponding data of oxygen non-stoichiometry from thermogravimetry measurements, shows that these are strongly determined by the order parameter n. The value of Ds decreases almost one order of magnitude on going from the n = 1 members La2NiO4+δ and Nd2NiO4+δ to the n = 2 member La3Ni2O7−δ, and again one order of magnitude on going to the n = 3 members La4Ni3O10−δ, Pr4Ni3O10−δ and Nd4Ni3O10−δ. The results confirm that oxygen-ion transport in the investigated RP nickelates predominantly occurs via an interstitialcy mechanism within the rock-salt layer of the structures.
dc.language.isoen
dc.publisherRoyal Society of Chemistry
dc.subject.en25:05 PM
dc.subject.enThis article is licensed under a Creative Commons Attribution-NonCommercial 3
dc.subject.en0 Unported Licence View Article Online
dc.title.enStructure, electrical conductivity and oxygen transport properties of Ruddlesden–Popper phases Lnn+1NinO3n+1 (Ln = La, Pr and Nd; n = 1, 2 and 3)
dc.typeArticle de revue
dc.identifier.doi10.1039/D0TA06731H
dc.subject.halChimie/Matériaux
bordeaux.journalJournal of Materials Chemistry A
bordeaux.page22206-22221
bordeaux.volume8
bordeaux.issue42
bordeaux.peerReviewedoui
hal.identifierhal-03028446
hal.version1
hal.popularnon
hal.audienceInternationale
hal.origin.linkhttps://hal.archives-ouvertes.fr//hal-03028446v1
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