Oxygen electrochemistry plays a key role in renewable energy technologies such as fuel cells and electrolyzers, but the slow kinetics of the oxygen evolution reaction (OER) limit the performance and commercialization of such devices. Here we report an iridium oxide/strontium iridium oxide (IrO/SrIrO) catalyst formed during electrochemical testing by strontium leaching from surface layers of thin films of SrIrO This catalyst has demonstrated specific activity at 10 milliamps per square centimeter of oxide catalyst (OER current normalized to catalyst surface area), with only 270 to 290 millivolts of overpotential for 30 hours of continuous testing in acidic electrolyte. Density functional theory calculations suggest the formation of highly active surface layers during strontium leaching with IrO or anatase IrO motifs. The IrO/SrIrO catalyst outperforms known IrO and ruthenium oxide (RuO) systems, the only other OER catalysts that have reasonable activity in acidic electrolyte.
The ability to create and manipulate materials in two-dimensional (2D) form has repeatedly had transformative impact on science and technology. In parallel with the exfoliation and stacking of intrinsically layered crystals, atomic-scale thin film growth of complex materials has enabled the creation of artificial 2D heterostructures with novel functionality and emergent phenomena, as seen in perovskite heterostructures. However, separation of these layers from the growth substrate has proved challenging, limiting the manipulation capabilities of these heterostructures with respect to exfoliated materials. Here we present a general method to create freestanding perovskite membranes. The key is the epitaxial growth of water-soluble Sr AlO on perovskite substrates, followed by in situ growth of films and heterostructures. Millimetre-size single-crystalline membranes are produced by etching the SrAl O layer in water, providing the opportunity to transfer them to arbitrary substrates and integrate them with heterostructures of semiconductors and layered compounds.
The search for oxide materials with physical properties similar to the cuprate high Tc superconductors, but based on alternative transition metals such as nickel, has grown and evolved over time [1][2][3][4][5][6][7][8][9][10]. The recent discovery of superconductivity in doped infinite-layer nickelates RNiO2 (R = rare-earth element) [11,12] further strengthens these efforts. With a crystal structure similar to the infinite-layer cupratestransition metal oxide layers separated by a rare-earth spacer layerformal valence counting suggests that these materials have monovalent Ni 1+ cations with the same 3d electron count as Cu 2+ in the cuprates. Here, we use x-ray spectroscopy in concert with density functional theory to show that the electronic structure of RNiO2 (R = La, Nd), while similar to the cuprates, includes significant distinctions. Unlike cuprates with insulating spacer layers between the CuO2 planes, the rare-earth spacer layer in the infinite-layer nickelate supports a weaklyinteracting three-dimensional 5d metallic state. This three-dimensional metallic state hybridizes with a quasi-two-dimensional, strongly correlated state with 3dx 2 -y 2 symmetry in the NiO2 layers. Thus, the infinite-layer nickelate can be regarded as a sibling of the rare earth intermetallics [13-15], well-known for heavy Fermion behavior, where the NiO2 correlated layers play an analogous role to the 4f states in rare-earth heavy Fermion compounds. This unique Kondo-or Anderson-lattice-like "oxide-intermetallic" replaces the Mott insulator as the reference state from which superconductivity emerges upon doping.While the mechanism of superconductivity in the cuprates remains a subject of intense research, early on it was suggested that the conditions required for realizing high Tc superconductivity are rooted in the physics of a two-dimensional electron system subject to strong local repulsion [16,17]. This describes the Mott (charge-transfer) insulators in the stoichiometric parent compounds, characterized by spin ½ Heisenberg antiferromagnetism, from which superconductivity emerges upon doping. A long-standing question regards whether these "cuprate-Mott" conditions can be realized in other oxides; and extensive efforts to synthesize and engineer nickel oxides (nickelates) have promised such a realization [1-10]. Infinite-layer NdNiO2 became the first such nickelate superconductor following the recent discovery of superconductivity in Srdoped samples [11]. The undoped parent compound, produced by removing the apical oxygen atoms from the perovskite nickelate NdNiO3 using a metal hydride-based soft chemistry reduction process [10,[18][19][20], appears to be a close sibling of the cuprates-it is isostructural to the infinitelayer cuprates with monovalent Ni 1+ cations and possesses the same 3d 9 electron count as that of Cu 2+ cations in undoped cuprates. Yet, as we will reveal, the electronic structure of the undoped RNiO2 (R = La and Nd) remains distinct from the Mott, or charge-transfer, compounds of undoped cuprates, and even...
All the iron-based superconductors identified to date share a square lattice composed of Fe atoms as a common feature, despite having different crystal structures. In copper-based materials, the superconducting phase emerges not only in square lattice structures but also in ladder structures. Yet iron-based superconductors without a square lattice motif have not been found despite being actively sought out. Here, we report the discovery of pressure-induced superconductivity in the iron-based spin-ladder material BaFe 2 S 3 , a Mott insulator with striped-type magnetic ordering below ~120 K. On the application of pressure this compound exhibits a metal-insulator transition at about 11 GPa, followed by the appearance of superconductivity below T c = 14 K, right after the onset of the metallic phase. Our findings indicate that iron-based ladder compounds represent promising material platforms, in particular for studying the fundamentals of iron-based superconductivity.The discovery of iron-based superconductors had a significant impact on condensed matter physics and led to extensive study of the interplay between crystal structure, magnetism and superconductivity 1 . All the iron-based superconducting materials discovered to date share the same structural motif: a two-dimensional square lattice formed by edge-shared FeX 4 tetrahedra (X = Se, P and As). The Fe atoms are nominally divalent in most of the parent materials. These parent compounds undergo a magnetic transition at low temperatures, typically exhibiting striped-type ordering.Superconductivity appears when the magnetic order is fully suppressed by the application of pressure or by the addition of doping carriers through chemical Purpose of this studyThe application of pressure is often a useful means of changing the electronic structure of a compound so as to induce a metallic state without simultaneously introducing any degree of disorder 17 . In this study, we investigated in detail the magnetic properties of a sulphur-analogue of the Fe-based ladder materials, BaFe 2 S 3 (space group: orthorhombic, Cmcm) 18,19 , and undertook experimental trials in which this compound was subjected to high pressures to obtain the metallic state. The electronic properties of this material depend on the manner in which the samples are synthesized, and thus we present data for sample 1 describing magnetic properties, and data for a range of samples 1 to 6 describing high-pressure effects. The details of the sample preparation process are given in the Method section. Electronic properties under ambient pressureFigure 2a displays the temperature dependence of the electrical resistivity (ρ) of BaFe 2 S 3 along the leg direction under ambient pressure. The observed insulating behaviour, which occurs despite the expected metallic behaviour in an unfilled 3d manifold, is caused by the Coulomb repulsion between Fe 3d electrons, which becomes prominent in a quasi-one-dimensional ladder structure. Figure 2b shows the magnetic susceptibility (χ) at 5 T along the three orthorhombic...
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