High Pressure Synthesis of SrFe&lt;sub&gt;1−&lt;/sub&gt;&lt;i&gt;&lt;sub&gt;x&lt;/sub&gt;&lt;/i&gt;Ni&lt;i&gt;&lt;sub&gt;x&lt;/sub&gt;&lt;/i&gt;O&lt;sub&gt;3&lt;/sub&gt;

Seki, Hayato; Saito, Takashi; Shimakawa, Yuichi

doi:10.2497/jjspm.63.609

Cited by 6 publications

(4 citation statements)

References 17 publications

(6 reference statements)

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“…The c value for the n = 8 SL is close to that of the pure LFO film. Inasmuch as the c value of the SL decreases with increasing SNO mole fraction and approaches to that of bulk SNO reported by H. Seki et al., [ 31 ] our results indicate that we can stabilize perovskite SNO in these SNO 1 /LFO n SLs. All SLs were found to be coherently strained to the LSAT substrates according to reciprocal space maps (RSMs) (Figure S3d, Supporting Information).…”

Section: Figuresupporting

confidence: 81%

“…This is the most likely reason that no stable SrFe 1− x Ni x O 3 structures with x > 0.5 have been reported in the literature. [ 31 ] However, we show that all‐perovskite‐structured superlattices can be stabilized when the SNO layer thickness is limited to 1 u.c ( m = 1). The structural diagram for a generic (SNO 1 /LFO n ) k SL deposited on a buffer layer of 10 u.c.…”

Section: Figurementioning

confidence: 89%

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Hole‐Trapping‐Induced Stabilization of Ni^4 + in SrNiO₃/LaFeO₃ Superlattices

et al. 2020

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Creating new functionality in materials containing transition metals is predicated on the ability to control the associated charge states. For a given transition metal, there is an upper limit on valence that is not exceeded under normal conditions. Here, it is demonstrated that this limit of 3+ for Ni and Fe can be exceeded via synthesis of (SrNiO3)m/(LaFeO3)n superlattices by tuning n and m. The Goldschmidt tolerance constraints are lifted, and SrNi4+O3 with holes on adjacent O anions is stabilized as a perovskite at the single‐unit‐cell level (m = 1). Holding m = 1, spectroscopy reveals that the n = 1 superlattice contains Ni3+ and Fe4+, whereas Ni4+ and Fe3+ are observed in the n = 5 superlattice. It is revealed that the B‐site cation valences can be tuned by controlling the magnitude of the FeO6 octahedral rotations, which, in turn, determine the energy balance between Ni3+/Fe4+ and Ni4+/Fe3+, thus controlling emergent electrical properties such as the band alignment and resulting hole confinement. This approach can be extended to other systems for synthesizing novel, metastable layered structures with new functionalities.

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Section: Figuresupporting

confidence: 81%

Section: Figurementioning

confidence: 89%

Hole‐Trapping‐Induced Stabilization of Ni^4 + in SrNiO₃/LaFeO₃ Superlattices

et al. 2020

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“…Unfortunately, this prediction is hard to validate experimentally as SrNiO 3 adopts a non-perovskite structure based on a hexagonal close packing of Sr and O atoms 19 . In addition, it is known that the substitution of Sr into LaNiO 3 is limited to ~5–20% after which phase impurities appear that result in poor catalytic activity 20,21 .…”

Section: Introductionmentioning

confidence: 99%

Exceptional electrocatalytic oxygen evolution via tunable charge transfer interactions in La0.5Sr1.5Ni1−xFexO4±δ Ruddlesden-Popper oxides

Forslund¹,

Hardin²,

Xi³

et al. 2018

Nat Commun

185

130

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The electrolysis of water is of global importance to store renewable energy and the methodical design of next-generation oxygen evolution catalysts requires a greater understanding of the structural and electronic contributions that give rise to increased activities. Herein, we report a series of Ruddlesden–Popper La0.5Sr1.5Ni1−xFexO4±δ oxides that promote charge transfer via cross-gap hybridization to enhance electrocatalytic water splitting. Using selective substitution of lanthanum with strontium and nickel with iron to tune the extent to which transition metal and oxygen valence bands hybridize, we demonstrate remarkable catalytic activity of 10 mA cm−2 at a 360 mV overpotential and mass activity of 1930 mA mg−1ox at 1.63 V via a mechanism that utilizes lattice oxygen. This work demonstrates that Ruddlesden–Popper materials can be utilized as active catalysts for oxygen evolution through rational design of structural and electronic configurations that are unattainable in many other crystalline metal oxide phases.

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“…The large ionic radii of divalent Sr and Ba lead to Goldschmidt tolerance factors exceeding 1, which explains the stability of the hexagonal SrNiO 3 and BaNiO 3 compounds compared to the cubic perovskite structure. However, cubic perovskite-structured compounds have been stabilized if there is only partial substitution of Ni, such as in cubic SrFe 1−x Ni x O 3 with x = 0−0.5 [30,31]. Recently, a single unit cell layer of epitaxial cubic perovskite SrNiO 3 was stabilized by charge redistribution in a SrNiO 3 /(LaFeO 3 ) n superlattice synthesized by molecular beam epitaxy [32], but another recent study to synthesize epitaxial cubic SrNiO 3 yielded phase separation into Sr 2 NiO 3 and SrNi 2 O 3 [33].…”

Section: Introductionmentioning

confidence: 99%

First-principles calculation of oxygen vacancy effects on the magnetic properties of the perovskite SrNiO3

Cho

Klyukin

Ning

et al. 2021

Phys. Rev. Materials

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Nickelates have been studied extensively due to their intriguing physical properties, but less attention has been paid to the properties of divalent A-site cation perovskite nickelates with a formal valence state of 4+ for Ni.Here, we study the electronic and magnetic properties of perovskite SrNiO 3−δ with an oxygen deficiency δ up to 0.375 using density functional theory. Because of the strong covalency and negative charge transfer energetics, the structure is predicted to exhibit ligand holes L, with Ni present as d 8 L 2 or d 7 L and significant magnetic moment at the oxygen sites. The ground state for δ = 0-0.375 consists of ferromagnetically ordered Ni with the Ni and O moments coupled antiferromagnetically, and the removal of oxygen increases the net magnetization. These behaviors are also predicted for other A-site cations such as Ca and Ba. This work demonstrates the importance of ligand holes in oxides with formally high valence Ni, including their influence on the magnetic properties, and motivates further experimental study of the electronic and magnetic properties of nickelates with divalent A-site cations.

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High Pressure Synthesis of SrFe<sub>1−</sub><i><sub>x</sub></i>Ni<i><sub>x</sub></i>O<sub>3</sub>

Cited by 6 publications

References 17 publications

Hole‐Trapping‐Induced Stabilization of Ni^4 + in SrNiO₃/LaFeO₃ Superlattices

Hole‐Trapping‐Induced Stabilization of Ni^4 + in SrNiO₃/LaFeO₃ Superlattices

Exceptional electrocatalytic oxygen evolution via tunable charge transfer interactions in La0.5Sr1.5Ni1−xFexO4±δ Ruddlesden-Popper oxides

First-principles calculation of oxygen vacancy effects on the magnetic properties of the perovskite SrNiO3

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High Pressure Synthesis of SrFe<sub>1−</sub><i><sub>x</sub></i>Ni<i><sub>x</sub></i>O<sub>3</sub>

Cited by 6 publications

References 17 publications

Hole‐Trapping‐Induced Stabilization of Ni4 + in SrNiO3/LaFeO3 Superlattices

Hole‐Trapping‐Induced Stabilization of Ni4 + in SrNiO3/LaFeO3 Superlattices

Exceptional electrocatalytic oxygen evolution via tunable charge transfer interactions in La0.5Sr1.5Ni1−xFexO4±δ Ruddlesden-Popper oxides

First-principles calculation of oxygen vacancy effects on the magnetic properties of the perovskite SrNiO3

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Hole‐Trapping‐Induced Stabilization of Ni^4 + in SrNiO₃/LaFeO₃ Superlattices

Hole‐Trapping‐Induced Stabilization of Ni^4 + in SrNiO₃/LaFeO₃ Superlattices