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DOE OSTI2022

Topological magnetic hysteresis in single crystals of CeAgSb 2 ferromagnet

Closed-topology magnetic domains are usually observed in thin films and in an applied magnetic field. In this work, we report the observation of rectangular cross-section tubular ferromagnetic domains in thick single crystals of CeAgSb 2 in zero applied field. Relatively low exchange energy, small net magnetic moment, and anisotropic in-plane crystal electric fields lower the domain wall energy and allow for the formation of the closed-topology patterns. The tubular domain structure irreversibly transforms into a dendritic pattern upon cycling the magnetic field. This transition between closed and open topologies results in a ‘topological magnetic hysteresis’— the actual hysteresis in magnetization, not due to the imperfections and pinning, but due to the difference in the pattern morphology. Similar physics was suggested before in pure type-I superconductors and is believed to be a generic feature of other nonlinear single (present case), or two-phase (type-I superconductor) systems where the effects similar to demagnetization (shape-dependent macroscopic variation of properties) lead to pattern formation.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2026

Magneto-optical study of Nb thin films for superconducting qubits

Abstract Among the recognized sources of decoherence in superconducting qubits, the spatial inhomogeneity of the superconducting state and the possible presence of magnetic-flux vortices remain comparatively underexplored. Niobium is commonly used as a structural material in transmon qubits that host Josephson junctions, and excess dissipation anywhere in the transmon can become a bottleneck that limits overall quantum performance. The metal/substrate interfacial layer may simultaneously host pair-breaking loss channels (e.g. two-level systems) and control thermal transport, thereby affecting dissipation and temperature stability. Here, we use quantitative magneto-optical imaging of the magnetic-flux distribution to characterize the homogeneity of the superconducting state and the critical current density, j c , in niobium films fabricated under different sputtering conditions. The imaging reveals distinct flux-penetration regimes, ranging from a nearly ideal Bean critical state to strongly nonuniform thermo-magnetic dendritic avalanches. By fitting the measured magnetic-induction profiles, we extract j c and try to correlate it with film physical properties and with measured qubit internal quality factors. Our results indicate that the Nb/Si interlayer can be a significant contributor to decoherence and should be considered an important factor that must be optimized.

Datta, Amlan [Ames National Laboratory; Iowa State↗

DOE OSTI2024

Endowing low fatigue for elastocaloric effect by refined hierarchical microcomposite in additive manufactured NiTiCuCo alloy

Abstract NiTiCu-based shape memory alloys have been considered as ideal materials for solid-state refrigeration due to their superb cycling stability for elastocaloric effect. However, the embrittlement and deterioration caused by secondary phase and coarse grains restrict their applications, and it is still challenging since the geometric components are required. Here, bulk NiTiCuCo parts with excellent forming quality were fabricated by laser powder bed fusion (LPBF) technique. The as-fabricated alloy exhibits refined three-phases hierarchical microcomposite formed based on the rapid cooling mode of LPBF, composed of intricate dendritic Ti 2 Ni–NiTi composite and nano Ti 2 Cu embedded inside the NiTi-matrix. This configuration endows far superior elastocaloric stability compared to the as-cast counterpart. The low fatigue stems from the strong elastic coupling between the interphases with reversible martensite transformation, revealed byin-situsynchrotron high-energy x-ray diffraction. The fabrication of NiTiCuCo alloy via LPBF fills the bill of complex geometric structures for elastocaloric NiTiCu alloys. The understanding of interphase micro-coupling could provide the guide for designing LPBF fabricated shape memory-based composites, enabling their applications for special demands on other functionalities.

Engineering↗

DOE OSTI2021

O-GlcNAc transferase Ogt regulates embryonic neuronal development through modulating Wnt/β-catenin signaling

Abstract Ogt-mediated O-GlcNAcylation is enriched in the nervous system and involves in neuronal development, brain function and neurological diseases. However, the roles of Ogt and O-GlcNAcylation in embryonic neurogenesis have remained largely unknown. Here, we show that Ogt is highly expressed in embryonic brain, and Ogt depletion reduces the proliferation of embryonic neural stem cells and migration of new born neurons. Ogt depletion in cultured hippocampal neurons impairs neuronal maturation, including reduced dendritic numbers and length, and immature development of spines. Mechanistically, Ogt depletion decreases the activity of Wnt/β-catenin signaling. Ectopic β-catenin rescues neuronal developmental deficits caused by Ogt depletion. Ogt also regulates human cortical neurogenesis in forebrain organoids derived from induced pluripotent stem cells. Our findings reveal the essential roles and mechanisms of Ogt-mediated O-GlcNAc modification in regulating mammalian neuronal development.

Shen, Hui↗

DOE OSTI2021

Imaging the structural organization of chemical elements in growth cones of developing hippocampal neurons

Abstract During neurodevelopment, neurons form growth cones, F-actin rich extensions located at the distal end of the neurites. Growth cones allow dendrites and axons to build synaptic connections through a process of neurite guidance whose mechanisms have not been fully elucidated. Calcium is an important element in this process by inducing F-actin reorganization. We hypothesized that other biologically active elements might be involved in the growth cone-mediated neurite guidance mechanisms. We performed super resolution and confocal microscopy of F-actin, followed by synchrotron X-ray fluorescence microscopy of phosphorous, sulfur, chlorine, potassium, calcium, iron and zinc on growth cones from primary rat hippocampal neurons. We identified two main patterns of element organization. First, active growth cones presenting an asymmetric distribution of Ca co-localized with the cytoskeleton protein F-actin. In active growth cones, we found that the distributions of P, S, Cl, K, and Zn are correlated with Ca. This correlation is lost in the second pattern, quiescent growth cones, exhibiting a spread elemental distribution. These results suggest that Ca is not the only element required in the F-actin rich active regions of growth cones. In addition, highly concentrated Fe spots of submicrometer size were observed in calcium-rich areas of active growth cones. These results reveal the need for biological active elements in growth cones during neural development and may help explain why early life deficiencies of elements, such as Fe or Zn, induce learning and memory deficits in children.

60 APPLIED LIFE SCIENCES↗

DOE OSTI2023

Modelling and simulation of brinicle formation

Below the Arctic sea ice, under the right conditions, a flux of icy brine flows down into the sea. The icy brine has a much lower fusion point and is denser than normal seawater. As a result, it sinks while freezing everything around it, forming an ice channel called a brinicle (also known as ice stalactite). In this paper, we develop a mathematical model for this phenomenon, assuming cylindrical symmetry. The fluid is considered to be viscous and quasi-stationary. The heat and salt transport are weakly coupled to the fluid motion and are modelled with the corresponding conservation equations, accounting for diffusive and convective effects. Finite-element discretization is employed to solve the coupled system of partial differential equations. We find that the model can capture the general behaviour of the physical system and generate brinicle-like structures while also recovering dendrite composition, which is a physically expected feature aligned with previous experimental results. This represents, to our knowledge, the first complete model proposed that captures the global structure of the physical phenomenon even though it has some discrepancies, such as brine accumulation.

97 MATHEMATICS AND COMPUTING↗

DOE OSTI2022

In-situ visualization of the transition metal dissolution in layered cathodes

Transition metal dissolution in layered cathodes is one of the most intractable issues that deteriorates the battery performance and lifetime. It not only aggravates the structure degradation in cathode, but also damages the solid electrolyte interphase in anode and even induce the formation of lithium dendrites. In this work, we investigate the dissolution behaviors of polycrystalline and single-crystalline layered cathode via operando X-ray imaging techniques. The described cathode particle morphology appears to have a significant impact on the evolution of the dissolution dynamics. As a mitigation strategy, we reveal that doping with trace amount of Zr in the layered cathode could improve its robustness against the transition metal dissolution. Our finding provides valuable insights for designing the next-generation highly-stable layered battery cathodes.

25 ENERGY STORAGE↗

DOE OSTI2022

Computational Elucidation of Mechanical Degradation in NMC Cathodes: Impact on Cell Performance

Next-generation lithium ion batteries are expected to demonstrate superior energy and power density with longer cycle life for successful electrification of the automobile, aviation, and marine industries. Adoption of lithium metal anodes with solid electrolytes can help to achieve that goal given that the dendrite-related issues are solved eventually. Another possibility is to use Ni-rich high-capacity NMC cathode materials with liquid and/or solid electrolytes, which presently experiences rapid capacity fade while charged to higher voltages. Several mechanical and chemical degradation mechanisms are active within these NMC-based cathode particles. Recent experimental research activities attempted to correlate the mechanical damage with the capacity fade experienced by Ni-rich LiNi x Mn y Co z O 2 (x+y+z = 1) (NMC) cathodes. Here, a computational framework is developed in this study capable of quantifying the evolution of inter primary particle and cathode/electrolyte interfacial fracture experienced by the poly- and single-crystalline NMC cathodes during charge/discharge operation. Influences of mechanical degradation on the overall cell capacity, while operating with liquid and/or solid electrolytes, are successfully characterized. Decreasing the size of the cathode primary particles, or the size of the single-crystalline cathodes, can mitigate the overall mechanical degradation, and subsequent capacity fade, experienced by NMC cathodes. The developed theoretical methodology can help the engineers and scientists to better understand the mechanical degradation mechanism prevalent in Ni-rich NMC cathodes and build superior lithium ion-based energy storage devices for the application in next-generation devices.

25 ENERGY STORAGE↗

DOE OSTI2024

A High-Ceramic-Loading LATP–PVDF–Al 2 O 3 Composite Film for Lithium-Ion Batteries With Favorable Porous Microstructure and Enhanced Thermal Stability

A separator plays a crucial role in a Li-ion battery to carry liquid electrolytes while preventing short-circuiting between electrodes. Nevertheless, conventional commercial separators often exhibit poor wettability and are prone to shrink at elevated temperatures due to their limited thermal stability. Herein, we report a heat-resistant LATP–PVDF–Al 2 O 3 composite film with outstanding wetting performance. The thin film was prepared using ball mill mixing and tape-casting processes. Two solvents, NMP and glycerol, were applied to prepare the slurry, and a favorable microstructure in the film was created after drying. Here, the ionic conductivity of the film was tested at 1.39 mS cm –1 when paired with liquid electrolyte, almost double that of the commercial counterpart. The high ceramic loading of 70% improved both the thermal shrinkage resistance and dendrite inhibition of the membrane. When assembled in an NMC half-cell, the cycling capacity retentions of 92.8% and 92.1% are achieved after 50 cycles at 0.5 C and 1 C, demonstrating its capability to be used in Li-ion batteries.

25 ENERGY STORAGE↗

DOE OSTI2026

Identifying Bounds of Inorganic Content in Solventless Processing of Hybrid Solid Electrolytes

Solid-state lithium batteries require safe, robust electrolytes to enable higher energy densities and improved safety over conventional cells. Hybrid polymer–ceramic electrolytes are a promising solution, combining the processability of polymers with the high ionic conductivity and mechanical strength of inorganic fillers. In this work, we demonstrate a solventless, UV-curing method to produce hybrid solid electrolytes using a poly(ethylene glycol) dimethyl ether (PEGDME)-based photocurable matrix incorporating Li 1.5 Al 0.5 Ge 1.5 (PO 4 ) 3 (LAGP) or Li 7 La 3 Zr 2 O 12 (LLZO) ceramic electrolyte. Inorganic filler loadings up to ∼55 wt.% could be successfully incorporated via this process which was the highest inorganic content at which the slurry remains processable and cured into a uniform film. The resulting UV-cured composite electrolytes remain flexible and exhibit room-temperature ionic conductivities on the order of 10 −4 S·cm −1 , along with notably improved lithium-ion transference numbers compared to conventional polymer electrolytes. Similar performance and processing limits were observed for both LAGP and LLZO, indicating that ceramic filler chemistry does not significantly affect the UV-curing process or the electrolyte's ion transport properties in this regime. Eliminating solvents from fabrication not only simplifies processing and mitigates environmental concerns but also enables higher solid contents that enhance mechanical strength and help suppress lithium dendrite formation. In conclusion, this scalable approach thus paves the way for manufacturing robust composite solid electrolytes for next-generation solid-state batteries (SSBs).

Batteries↗

DOE OSTI2023

LiH formation and its impact on Li batteries revealed by cryogenic electron microscopy

Little is known about how evolved hydrogen affects the cycling of Li batteries. Hypotheses include the formation of LiH in the solid-electrolyte interphase (SEI) and dendritic growth of LiH. Here, we discover that LiH formation in Li batteries likely follows a different pathway: Hydrogen evolved during cycling reacts to nucleate and grow LiH within already deposited Li metal, consuming active Li. We provide the evidence that LiH formed in Li batteries electrically isolates active Li from the current collector that degrades battery capacity. We detect the coexistence of Li metal and LiH also on graphite and silicon anodes, showing that LiH forms in most Li battery anode chemistries. Last, we find that LiH has its own SEI layer that is chemically and structurally distinct from the SEI on Li metal. Our results highlight the formation mechanism and chemical origins of LiH, providing critical insight into how to prevent its formation.

25 ENERGY STORAGE↗

DOE OSTI2023

Lithium-compatible and air-stable vacancy-rich Li 9 N 2 Cl 3 for high–areal capacity, long-cycling all–solid-state lithium metal batteries

Attaining substantial areal capacity (>3 mAh/cm 2 ) and extended cycle longevity in all–solid-state lithium metal batteries necessitates the implementation of solid-state electrolytes (SSEs) capable of withstanding elevated critical current densities and capacities. In this study, we report a high-performing vacancy-rich Li 9 N 2 Cl 3 SSE demonstrating excellent lithium compatibility and atmospheric stability and enabling high–areal capacity, long-lasting all–solid-state lithium metal batteries. The Li 9 N 2 Cl 3 facilitates efficient lithium-ion transport due to its disordered lattice structure and presence of vacancies. Notably, it resists dendrite formation at 10 mA/cm 2 and 10 mAh/cm 2 due to its intrinsic lithium metal stability. Furthermore, it exhibits robust dry-air stability. Incorporating this SSE in Ni-rich LiNi 0.83 Co 0.11 Mn 0.06 O 2 cathode-based all–solid-state batteries, we achieve substantial cycling stability (90.35% capacity retention over 1500 cycles at 0.5 C) and high areal capacity (4.8 mAh/cm 2 in pouch cells). These findings pave the way for lithium metal batteries to meet electric vehicle performance demands.

25 ENERGY STORAGE↗

DOE OSTI2021

Solvation sheath reorganization enables divalent metal batteries with fast interfacial charge transfer kinetics

Efficient, rechargeable Mg and Ca batteries Divalent rechargeable metal batteries such as those based on magnesium and calcium are of interest because of the abundance of these elements and their lower tendency to form dendrites, but practical demonstrations are lacking. Hou et al . used methoxyethyl amine chelants in which the ligands attach to the metal atom in more than one place, modulating the solvation structure of the metal ions to enable a facile charge-transfer reaction (see the Perspective by Zuo and Yin). In full battery cells, these components lead to high efficiency and energy density. Theoretical calculations were used to understand the solvation structures. —MSL

Science & Technology - Other Topics↗

DOE OSTI2025

Cracking the failure of lithium batteries

Lithium batteries that use a solid electrolyte have the potential to improve safety and increase the amount of stored energy . This makes solid-state electrochemical cells a promising option for electric vehicles and wearable devices. However, nonuniform plating or stripping of lithium at the interface between an anode (negative electrode) and the electrolyte during charging and discharging leads to growth of detrimental lithium filaments (dendrites) that short-circuit the battery cell. This problem even occurs when the battery operates at small currents. The underlying mechanism of this failure is not well understood. On page 311 of this issue, Wang et al. (1) report that structural defects accumulate in the lithium metal anode under repeated charging and discharging at a small current. This is similar to mechanical fatigue that is observed over longer periods of intermittent straining of a material. Here, the observation could guide the design of lithium batteries with increased life span.

25 ENERGY STORAGE↗

DOE OSTI2021

Comparative Molecular and Immunoregulatory Analysis of Extracellular Vesicles from Candida albicans and Candida auris

Candida auris is a recently described multidrug-resistant pathogenic fungus that is increasingly responsible for health care-associated outbreaks across the world. Bloodstream infections of this fungus cause death in up to 70% of cases. Aggravating this scenario, the disease-promoting mechanisms of C. auris are poorly understood. Fungi release extracellular vesicles (EVs) that carry a broad range of molecules, including proteins, lipids, carbohydrates, pigments, and RNA, many of which are virulence factors. Here, we carried out a comparative molecular characterization of C. auris and Candida albicans EVs and evaluated their capacity to modulate effector mechanisms of host immune defense. Using proteomics, lipidomics, and transcriptomics, we found that C. auris released EVs with payloads that were significantly different from those of EVs released by C. albicans. EVs released by C. auris potentiated the adhesion of this yeast to an epithelial cell monolayer, while EVs from C. albicans had no effect. C. albicans EVs primed macrophages for enhanced intracellular yeast killing, whereas C. auris EVs promoted survival of the fungal cells. Moreover, EVs from both C. auris and C. albicans induced the activation of bone marrow-derived dendritic cells. Together, our findings show distinct profiles and properties of EVs released by C. auris and by C. albicans and highlight the potential contribution of C. auris EVs to the pathogenesis of this emerging pathogen.

59 BASIC BIOLOGICAL SCIENCES↗

DOE OSTI2020

Improved Stability and Cyclability of Ceramic Solid Electrolyte by Coating Polymer

Rechargeable all-solid-state lithium (Li) metal batteries show better safety and energy density compared to commercial Li-ion batteries using liquid electrolyte. As the key component of Li metal batteries, ceramic solid-state electrolyte has attracted great interest because of its high ion conductivity and great potential in interfacing with Li metal. Ceramic electrolyte has a more stable interface with Li metal than liquid electrolyte, but chemical reaction and Li dendrite growth at the electrolyte/Li interface are still significant, which causes device degradation and failure by cycling of Li plating and stripping. Unlike ceramic electrolyte, polymer electrolyte has a relatively stable interface with Li metal and better mechanical flexibility. Therefore, we introduced a polymer electrolyte coating to protect the ceramic electrolyte from direct contact with Li metal. The galvanotactic cycling Li plating/striping data on the devices with (without) the coating illustrates increased (decreased) overall conductivity and cyclability of the test cell by the cycling. Nanometer-scale ionic-transport imaging, based on atomic force microscopy, shows that cycling degrades the ceramic-only electrolyte by partially blocking ionic transport in areas; in contrast, cycling on the polymer-coated electrolyte improves ionic conductivity. Compared with the ceramic-only electrolyte, this novel polymer electrolyte coating on ceramic electrolyte shows less degradation when in contact with Li metal.

25 ENERGY STORAGE↗

DOE OSTI2020

Mechano-Electrochemical Interaction in Solid-State Lithium Batteries

A solid-state lithium (Li) battery primarily consists of Li metal anode, solid electrolyte separator, and cathode. The asymmetric volume changes, originating from ion transport and interfacial Li growth during plating, lead to significant stresses in the layered architecture. In this study, we develop a coupled mechanics-electrochemistry formalism for polymer electrolyte based solid-state batteries, in particular, focusing on the stress effect on electrochemical performance. By means of a coupling coefficient, it is found that stress-assisted ion transport in the electrolyte results in a delayed Sand’s time and increased critical current density of unstable electrodeposition, and consequently, alleviates the propensity of dendrite formation. Stress at the Li metal-electrolyte interface affects the electrochemical reaction kinetics, and the influences from the deviatoric stress and hydrostatic pressure vary with Li plating time. In addition, a low restraint stiffness to the layered structure could elastically buffer the volumetric changes and thus reduce the stress during Li plating. This fundamental study provides guidance for the design of solid-state batteries, aimed at stable electrodeposition and mechanical integrity.

25 ENERGY STORAGE↗

DOE OSTI2020

Model-Instructed Design of Novel Charging Protocols for the Extreme Fast Charging of Lithium-Ion Batteries Without Lithium Plating

Relatively long recharge time of high-energy density lithium-ion batteries (LIBs) is one of the major obstacles to the widespread deployment of electric vehicles (EVs). Excessive fast charge of LIBs can cause severe safety issues, the most significant of which is lithium plating. In addition to the consumption of cyclable lithium, dendrite-like lithium plating can cause short-circuiting within the cell, which could lead to catastrophic failure. In addition to the developments of advanced electrolytes, active materials and electrodes, the fast charging capability of LIBs can be improved by using optimized charging protocol. In this paper, the Pseudo2D battery model is first used to screen some conventional charging protocols proposed for fast charging, including the constant-current constant-voltage charging (CCCV), constant-power constant-voltage charging (CPCV), multi-stage constant-current charging, and pulse current charging. A semi-optimal charging protocol is then developed by automatically modifying the charge current such that the cell is charged at close-to-maximum current without lithium plating. Based on the features of the semi-optimal protocol, two practical novel fast charging protocols are proposed which allow charging the cell at a higher rate without lithium plating. Through simulation, we show that the no-plating capacity after 10 min charge can be improved by up to ~10.7% compared to CCCV charging for a 2.5 mAh cm -2 cell and ~18.8% for a 4 mAh cm -2 cell, when the proposed charging protocols are used.

25 ENERGY STORAGE↗