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At least 235 records · Page 13
All sourcesNASA NTRSDOE OSTI
DOE OSTI2025

Navigating thermal stability intricacies of high-nickel cathodes for high-energy lithium batteries

High-nickel oxide cathodes, LiNi x M 1−x O 2 (x ≥ 0.8), are preferred in automotive lithium batteries, but they face thermal instability challenges. Inconsistent literature reports and unstandardized testing protocols further complicate quantitative assessments of the thermal stability of these cathodes. Here, we present here a statistical thermal analysis based on the differential scanning calorimetry measurements of 15 representative cathode materials with different compositions, morphologies and states of charge. The findings reveal that each cathode has a critical state of charge that defines its safe operating limit, which is affected by the metal–oxygen bond strength and surface reactivity. The thermal runaway temperature is dictated by the layered Li 1−x NiO 2 to LiNi 2 O 4 spinel-like phase transition, which is thermodynamically determined by the metal–oxygen bond covalency and kinetically influenced by the cation mixing and particle size. Raman spectroscopy is used to predict the thermal runaway temperature on the basis of the linear relationship between them. Finally, we propose a thermal stability index to quantify cathode thermal stability as a guide for developing safer high-nickel cathodes.

batteries↗
DOE OSTI2024

Evidence for d -wave superconductivity of infinite-layer nickelates from low-energy electrodynamics

The discovery of superconductivity in infinite-layer nickelates established another category of unconventional superconductors that shares structural and electronic similarities with cuprates. However, key issues of the superconducting pairing symmetry, gap amplitude and superconducting fluctuations are yet to be addressed. Here we utilize static and ultrafast terahertz spectroscopy to address these. We demonstrate that the equilibrium terahertz conductivity and non-equilibrium terahertz responses of an optimally Sr-doped nickelate film (superconducting transition temperature of T c = 17 K) are in line with the electrodynamics of d-wave superconductivity in the dirty limit. The gap-to-T c ratio (2Δ/k B T c ) is found to be 3.4, indicating that the superconductivity falls in the weak coupling regime. In addition, we observed substantial superconducting fluctuations near T c that do not extend into the deep normal state as the optimally hole-doped cuprates do. In conclusion, our results support a d-wave system that closely resembles the electron-doped cuprates.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2026

Protonic nickelate device networks for spatiotemporal neuromorphic computing

Computation in biological neural circuits arises from the interplay of nonlinear temporal responses and spatially distributed dynamic network interactions. Replicating this richness in hardware has remained challenging, as most neuromorphic devices emulate only isolated neuron- or synapse-like functions. Here we introduce an integrated neuromorphic computing platform in which both nonlinear spatiotemporal processing and programmable memory are realized within a single perovskite nickelate material system. By engineering symmetric and asymmetric hydrogenated NdNiO 3 junction devices on the same wafer, we combine ultrafast, proton-mediated transient dynamics with stable multilevel resistance states. Networks of symmetric NdNiO 3 junctions exhibit emergent spatial interactions mediated by proton redistribution, while each node simultaneously provides short-term temporal memory, enabling nanosecond-scale operation with an energy cost of ~0.2 nJ per input. When interfaced with asymmetric output units serving as reconfigurable long-term weights, these networks allow both feature transformation and linear classification in the same material system. Leveraging these emergent interactions, the platform enables real-time pattern recognition and achieves high accuracy in spoken digit classification and early seizure detection, outperforming temporal-only or uncoupled architectures. These results position protonic nickelates as a compact, energy-efficient, CMOS-compatible platform that integrates processing and memory for scalable intelligent hardware.

Electrical and electronic engineering↗
DOE OSTI2021

Isotropic Pauli-limited superconductivity in the infinite-layer nickelate Nd 0.775 Sr 0.225 NiO 2

The recent observation of superconductivity in thin-film infinite-layer nickelates offers a different angle from which to investigate superconductivity in layered oxides. A wide range of candidate models have been proposed, which emphasize single- or multi-orbital electronic structure, Kondo or Hund’s coupling and analogies to cuprates. Further experimental characterization of the superconducting state is needed to develop a full understanding of the nickelates. Here we use magnetotransport measurements to probe the superconducting anisotropy in Nd 0.775 Sr 0.225 NiO 2 . Here, we find that the upper critical field is surprisingly isotropic at low temperatures despite the layered crystal structure. In a magnetic field, the superconductivity is strongly Pauli-limited, such that the paramagnetic effect dominates over orbital de-pairing. Underlying this isotropic response is a substantial anisotropy in the superconducting coherence length, which is at least four times longer in-plane than out-of-plane. A prominent low-temperature upturn in the upper critical field indicates the presence of an unconventional ground state.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2023

Resonant inelastic x-ray scattering data for Ruddlesden-Popper and reduced Ruddlesden-Popper nickelates

Abstract Ruddlesden-Popper and reduced Ruddlesden-Popper nickelates are intriguing candidates for mimicking the properties of high-temperature superconducting cuprates. The degree of similarity between these nickelates and cuprates has been the subject of considerable debate. Resonant inelastic x-ray scattering (RIXS) has played an important role in exploring their electronic and magnetic excitations, but these efforts have been stymied by inconsistencies between different samples and the lack of publicly available data for detailed comparison. To address this issue, we present open RIXS data on La 4 Ni 3 O 10 and La 4 Ni 3 O 8 .

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2020

Continuous liquid-phase synthesis of nickel phosphide nanoparticles in a helically coiled tube reactor

The continuous liquid phase synthesis of nickel phosphide (Ni 2 P) nanoparticles was studied in a helically coiled tube (HCT) reactor both in single-phase and two-phase slug flows. The reactants were nickel acetylacetonate and tri-n-octylphosphine (TOP) in a 1-octadecane solvent. For the single-phase mode, various parameters such as reaction temperature, residence time, TOP concentration, and P/Ni ratio were studied. It was found that lower temperatures of 320 and 340 °C resulted in the formation of mixed Ni 12 P 5 and Ni 2 P phases, while a higher temperature of 360 °C gave mostly Ni 2 P, with particle sizes increasing from 28 to 42 nm. Upon varying the contact time between 88 and 340 s at 360 °C, a likely sequence of reaction involved an amorphous phase that was transformed in parallel to Ni, Ni 12 P 5 , and Ni 2 P. When the flow in the HCT was changed to a two-phase slug flow by using N 2 to split the continuous liquid phase into small liquid columns, the product was nearly 100% Ni 2 P and the particle size was as small as 3–4 nm. This was attributed to the enhanced mass transfer in the small liquid columns of the slug flow that led to higher reaction rates. Finally, it is highlighted that the HCT operated in a slug flow is an efficient and continuous method for the fabrication of nanoparticles.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Nickel(ii) complexes based on dithiolate–polyamine binary ligand systems: crystal structures, hirshfeld surface analysis, theoretical study, and catalytic activity study on photocatalytic hydrogen generation

To ascertain the influence of binary ligand systems [1,1-dicyanoethylene-2,2-dithiolate (i-mnt -2 ) and polyamine {tetraen = tris(2-aminoethyl)amine, tren = diethylene triamine and opda = o-phenylenediamine}] on the coordination modes of the Ni(II) metal center and resulting supramolecular architectures, a series of nickel(II) thiolate complexes [Ni(tetraen)(i-mnt)](DMSO) (1), [Ni 2 (tren) 2 (i-mnt) 2 ] (2), and [Ni 2 (i-mnt) 2 (opda) 2 ] n (3) have been synthesized in high yield in one step in water and structurally characterized by single crystal X-ray crystallography and spectroscopic techniques. X-ray diffraction studies disclose the diverse i-mnt -2 coordination to the Ni +2 center in the presence of active polyamine ligands, forming a slightly distorted octahedral geometry (NiN 4 S 2 ) in 1, square planar (NiS 4 ) and distorted octahedral geometries (NiN 6 ) in the bimetallic co-crystallized aggregate of cationic [Ni(tren) 2 ] +2 and anionic [Ni(i-mnt) 2 ] -2 in 2, and a one dimensional (1D) polymeric chain along the [100] axis in 3, having consecutive square planar (NiS 4 ) and octahedral (NiN 6 ) coordination kernels. The N–H···O, N–H···S, N–H···N, N–H···S, N–H···N, and N–H···O type hydrogen bonds stabilize the supramolecular assemblies in 1, 2, and 3 respectively imparting interesting graph-set-motifs. The molecular Hirshfeld surface analyses (HS) and 2D fingerprint plots were utilized for decoding all types of non-covalent contacts in the crystal networks. Atomic HS analysis of the Ni +2 centers reveals significant Ni–N metal–ligand interactions compared to Ni–S interactions. We have also studied the unorthodox interactions observed in the solid state structures of 1–3 by QTAIM and NBO analyses. Moreover, all the complexes proved to be highly active water reduction co-catalysts (WRC) in a photo-catalytic hydrogen evolution process involving iridium photosensitizers, wherein 2 and 3 having a square planar arrangement around the nickel center(s) – were found to be the most active ones, achieving 1000 and 1119 turnover numbers (TON), respectively.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Thioester synthesis by a designed nickel enzyme models prebiotic energy conversion

The formation of carbon–carbon bonds from prebiotic precursors such as carbon dioxide represents the foundation of all primordial life processes. In extant organisms, this reaction is carried out by the carbon monoxide dehydrogenase (CODH)/acetyl coenzyme A synthase (ACS) enzyme, which performs the cornerstone reaction in the ancient Wood–Ljungdahl metabolic pathway to synthesize the key biological metabolite, acetyl-CoA. Despite its significance, a fundamental understanding of this transformation is lacking, hampering efforts to harness analogous chemistry. To address these knowledge gaps, we have designed an artificial metalloenzyme within the azurin protein scaffold as a structural, functional, and mechanistic model of ACS. We demonstrate the intermediacy of the Ni I species and requirement for ordered substrate binding in the bioorganometallic carbon–carbon bond-forming reaction from the one-carbon ACS substrates. The electronic and geometric structures of the nickel-acetyl intermediate have been characterized using time-resolved optical, electron paramagnetic resonance, and X-ray absorption spectroscopy in conjunction with quantum chemical calculations. Moreover, we demonstrate that the nickel-acetyl species is chemically competent for selective acyl transfer upon thiol addition to biosynthesize an activated thioester. Drawing an analogy to the native enzyme, a mechanism for thioester generation by this ACS model has been proposed. The fundamental insight into the enzymatic process provided by this rudimentary ACS model has implications for the evolution of primitive ACS-like proteins. Ultimately, these findings offer strategies for development of highly active catalysts for sustainable generation of liquid fuels from one-carbon substrates, with potential for broad applications across diverse fields ranging from energy storage to environmental remediation.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Entering the Nickel Age of Superconductivity.

After a 30-year quest, researchers found a nickel-based analog of copper oxide superconductors. The discovery motivates the search for other nickelates and should provide new insights into the origin of high-temperature superconductivity.

Norman, Michael R.↗
DOE OSTI2020

Theoretical investigation of superconductivity in trilayer square-planar nickelates

The discovery of superconductivity in Sr-doped NdNiO 2 is a crucial breakthrough in the long pursuit for nickel oxide materials with electronic and magnetic properties similar to those of the cuprates. NdNiO 2 is the infinite-layer member of a family of square-planar nickelates with general chemical formula R n +1 Ni n O 2 n +2 (R = La, Pr, Nd, n = 2, 3,...∞). In this Rapid Communication, we investigate superconductivity in the trilayer member of this series (R4Ni 3 O 8 ) using a combination of first-principles and $\textit{t–J}$ model calculations. R 4 Ni 3 O 8 compounds resemble cuprates more than RNiO 2 materials in that only Ni-d n 2 – y 2 bands cross the Fermi level, they exhibit a largely reduced charge transfer energy, and as a consequence superexchange interactions are significantly enhanced. In this work, we find that the superconducting instability in doped R 4 Ni 3 O 8 compounds is considerably stronger with a maximum gap about four times larger than that in Sr 0.2 Nd 0.8 NiO 2 .

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2020

Similarities and differences between nickelate and cuprate films grown on a SrTiO 3 substrate

The recent discovery of superconductivity in Sr-doped NdNiO 2 films grown on SrTiO 3 started a novel field within unconventional superconductivity. Therefore, to understand the similarities and differences between nickelate and cuprate layers on the same SrTiO 3 substrate, here based on the density functional theory we have systematically investigated the structural, electronic, and magnetic properties of NdNiO 2 / SrTiO 3 and CaCuO 2 / SrTiO 3 systems. Our results revealed a strong lattice reconstruction in the case of NdNiO 2 / SrTiO 3 , resulting in a polar film, with the surface and interfacial NiO 2 layers presenting opposite displacements. To avoid the “polar catastrophe,” the NiO 2 surface to the vacuum reconstructs as well. However, for CaCuO 2 / SrTiO 3 , the distortions of those same two CuO 2 layers were in the same direction. In addition, we found this distortion to be approximately independent of the studied range of film thickness for the nickelate films. Furthermore, we also observed a two-dimensional electron gas at the interface between NdNiO 2 and SrTiO 3 , caused by the polar discontinuity, in agreement with recent literature. For NdNiO 2 / SrTiO 3 the two-dimensional electron gas extends over several layers, while for CaCuO 2 / SrTiO 3 this electronic rearrangement is very localized at the interface between CaCuO 2 and SrTiO 3 . The electronic reconstruction found at the interface involves a strong occupation of the Ti 3 d x y state. In both cases, there is a significant electronic charge transfer from the surface Ni or Cu layers to the Ti interface layer. The interfacial Ni and Cu layers are hole and electron doped, respectively. By introducing magnetism and electronic correlation, we observed that the d 3 z 2 - r 2 orbital of Ni becomes itinerant while the same orbital for Cu remains doubly occupied, establishing a clear two- vs one-orbital active framework for the description of these systems. Furthermore, we also observed a strong magnetic reconstruction at the NdNiO 2 surface to vacuum layer where magnetism is basically suppressed.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2020

High oxygen pressure floating zone growth and crystal structure of the metallic nickelates R4Ni3O10 ( R=La,Pr )

Single crystals of the metallic Ruddlesden-Popper trilayer nickelates R 4 Ni 3 O 10 ( R = La , Pr ) were successfully grown using an optical-image floating zone furnace under oxygen pressure ( p O 2 ) of 20 bar for La 4 Ni 3 O 10 and 140 bar for Pr 4 Ni 3 O 10 . Furthermore, a combination of synchrotron and laboratory x-ray single-crystal diffraction, high-resolution synchrotron x-ray powder diffraction and measurements of physical properties revealed that R 4 Ni 3 O 10 ( R = La , Pr ) crystallizes in the monoclinic P 2 1 / a ( Z = 2 ) space group at room temperature, and that a metastable orthorhombic phase ( Bmab ) can be trapped by postgrowth rapid cooling. Both La 4 Ni 3 O 10 and Pr 4 Ni 3 O 10 crystals undergo a metal-to-metal transition (MMT) below room temperature. In the case of Pr 4 Ni 3 O 10 , the MMT is found at 157.6 K. For La 4 Ni 3 O 10 , the MMT depends on the lattice symmetry: 147.5 K for Bmab vs 138.6 K for P 2 1 / a . Lattice anomalies were found at the MMT that, when considered together with the pronounced dependence of the transition temperature on subtle structural differences between Bmab and P 2 1 / a phases, demonstrate a not insignificant coupling between electronic and lattice degrees of freedom in these trilayer nickelates.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Scanning SQUID study of ferromagnetism and superconductivity in infinite-layer nickelates

Infinite-layer nickelates R 1-x Sr x NiO 2 (R = La, Pr, Nd) are a class of superconductors with structural similarities to cuprates. Although long-range antiferromagnetic order has not been observed for these materials, magnetic effects such as antiferromagnetic spin fluctuations and spin-glass behavior have been reported. Different experiments have drawn different conclusions about whether the pairing symmetry is s or d wave. In this paper, we applied a scanning superconducting quantum interference device (SQUID) to probe the magnetic behavior of film samples of three infinite-layer nickelates (La 0.85 Sr 0.15 NiO 2 , Pr 0.8 Sr 0.2 NiO 2 , and Nd 0.775 Sr 0.225 NiO 2 ) grown on SrTiO 3 (STO), each with a nominal thickness of 20 unit cells. In all three films, we observed a ferromagnetic background. We also measured the magnetic susceptibility above the superconducting critical temperature in Pr 0.8 Sr 0.2 NiO 2 and La 0.85 Sr 0.15 NiO 2 and identified a non-Curie-Weiss dynamic susceptibility. Both magnetic features are likely due to NiO x nanoparticles. We investigated superconductivity in Pr 0.8 Sr 0.2 NiO 2 and Nd 0.775 Sr 0.225 NiO 2 , which exhibited inhomogeneous diamagnetic screening. The superfluid density inferred from the diamagnetic susceptibility in relatively homogeneous regions shows T-linear behavior in both samples. Finally, we observed superconducting vortices in Nd 0.775 Sr 0.225 NiO 2 . We determined a Pearl length of 330 µm for Nd 0.775 Sr 0.225 NiO 2 at 300 mK, both from the strength of the diamagnetism and from the size and shape of the vortices. These results highlight the importance of considering NiO x particles when interpreting experimental results for these films.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2025

Electronic effects in radiation-induced collision cascades in nickel

The accurate treatment of electronic effects in multi-million-atom simulations of radiation-induced collision cascades is crucial for reliable predictions of primary radiation damage. In this work, we explore the fidelity of a recently developed two-temperature molecular dynamics model implementing an electron density-dependent coupling of electronic and atomic subsystems for cascade simulations in nickel. We show that the parameter-free model realistically captures the instantaneous energy losses during all stages of the highly nonequilibrium cascade process. Our simulations predict two distinct coupling regimes, corresponding to the rapid energy losses through electronic stopping in the early stages of the cascade and to the slow equilibration through the electron-phonon coupling mechanism in the later stages, without the use of separate models or coupling terms. The intermediate stage of the cascade dynamics displays a complex energy transfer between the subsystems, which cannot be interpreted by comparison to either electronic stopping or electron-phonon coupling theories. We therefore compare the predicted atomic mixing, which is sensitive to the energy losses during the intermediate cascade stage, with experimental ion beam mixing measurements. We find good agreement with the experiments, validating the coupling model for the intermediate stage of the cascade. Predictions of final defect numbers and cluster sizes are found in line with the results from conventional electronic stopping-based methods, while significantly reducing the theoretical uncertainty in the outcomes of conventional models stemming from arbitrary choices of thresholds for different coupling terms. Our results represent a notable improvement in cascade damage predictions in nickel, providing validation of the electron density-dependent coupling model for radiation damage simulations in general. The results lead us to propose an interpretation of the electronic energy losses in the intermediate regime of velocities, where we find an effectively nonlinear dissipation.

Crystal defects↗
DOE OSTI2025

Softening of dd excitation in the resonant inelastic x-ray scattering spectra as a signature of Hund's coupling in nickelates

We investigate the effects of Hund's coupling on the resonant x-ray absorption spectra of the recently discovered family of layered nickelate superconductors. We contrast two scenarios depending on the relative strength of the ratio of the effective Hund's coupling ( J H ) to the crystal fields ( Δ ) in these systems. We carry out the cluster and DFT + DMFT simulations of the RIXS signal at the Ni L edge for different values of Hund's coupling. We find the latter dominates for the parent compound while the former becomes important for sufficiently large doping. Our results are consistent with the observations of a softening of a RIXS peak as a function of doping by Rossi [], only when the Hund coupling is sizable. To interpret the results, we separate the theoretical RIXS signal into spin conserving and nonspin conserving channels and conclude that the infinite layer nickelates are in a regime where Δ and J compete effectively and suggest further experimental tests of the theory. Published by the American Physical Society 2025

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2025

Magnetic correlations and pairing tendencies of the hybrid stacking nickelate superlattice La 7 Ni 5 O 17 (La 3 ⁢Ni 2 ⁢O 7 /La 4 Ni 3 ⁢O 10 ) under pressure

Motivated by the recent rapid progress in high-𝑇 𝑐 nickelate superconductors, we comprehensively study the physical properties of the alternating bilayer trilayer stacking nickelate La 7 ⁢Ni 5 ⁢O 17 . The high-symmetry phase of this material, without the tilting of oxygen octahedra, is not stable at ambient conditions but becomes stable under high pressure, where a small hole pocket 𝛾 0 , composed of the 𝑑 3⁢𝑧 2 −𝑟 2 states in the trilayer sublattice, appears. Here, this pocket was identified in our previous work for trilayer La 4 ⁢Ni 3 ⁢O 10 as important to develop superconductivity. Moreover, using random-phase approximation calculations, we find a leading 𝑠 ± pairing state for the high-symmetry phase under pressure with similar pairing strength as that obtained previously for the bilayer La 3⁢ Ni 2 ⁢O 7 compound, suggesting a similar or higher superconducting transition temperature 𝑇 𝑐 , at the random-phase approximation level. In addition, we find that the dominant magnetic fluctuations in the system driving this pairing state have antiferromagnetic structure both in-plane and between the planes of the top and bottom trilayer and bilayer sublattices, while the middle trilayer is magnetically decoupled.

Zhang, Yang [Univ. of Tennessee, Knoxville, TN (Un↗
DOE OSTI2023

Influence of Single-Crystalline Morphology on the Electrochemical Behavior of High-Nickel Layered Oxide Cathodes

High-Nickel layered oxides are being pursued for their high specific capacities. With increasing nickel content, the layered oxides also suffer from structural and morphological instabilities, which degrade the electrochemical performance. Single-crystalline morphology presents an attractive solution to these problems, simultaneously reducing surface area available for parasitic reactions and preventing electrolyte penetration into the bulk with the removal of grain boundaries. Single-crystal cathodes have already shown promising results with NMC composition cathodes, but there are still gaps in the fundamental understanding of how single-crystalline morphology alters electrochemical behavior. We attempt to fill some of these gaps by studying in detail the electrochemical operation of polycrystalline and single-crystalline LiNiO 2 (LNO). Single-crystal LNO is prepared through a molten salt method yielding high-quality, distinct crystals with comparable lattice chemistry to polycrystalline LNO. The single-crystal LNO achieves far greater stability during long-term cycling, reaching 500 cycles with 82.5% capacity retention. Interestingly, the single-crystalline LNO also displays superior rate performance, delivering 157 mA h g −1 at 10C discharge rate. Investigation of the phase evolution behavior during cycling strongly suggests that the absence of grain boundaries in single-crystalline LNO is responsible for the superior performance.

25 ENERGY STORAGE↗
DOE OSTI2025

Recent Developments in Lithium-Manganese-Nickel Oxide Electrochemistry: The Alchemy of LiMn 0.5 Ni 0.5 O 2

Efforts have been underway for some time at Argonne National Laboratory to design structurally integrated and stabilized lithium-manganese-nickel-oxide cathode materials. The goal has been to find a cobalt-free, high-capacity cathode for a Li-ion battery that is competitive, both cost- and energy-wise, with lithium-nickel-manganese-cobalt-oxide (NMC) and lithium-iron-phosphate (LFP) products. This brief synopsis highlights the remarkable alchemy of LiMn 0.5 Ni 0.5 O 2 resulting from its well-known, slightly disordered layered structure and the recently discovered lithiated spinel phase and totally disordered rock-salt configurations. All three arrangements share a structurally compatible cubic-close-packed oxygen array. The lithiated spinel and layered components provide an intersecting network of two- and three-dimensional channels that facilitate Li + -ion transport, while a minor amount of an extensively disordered rock-salt component likely serves to enhance the structural and electrochemical stability of the electrode. The synopsis also encompasses the historical development of lithiated spinel electrode materials and structurally integrated systems.

Thackeray, Michael M. [Argonne National Laboratory↗