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DOE OSTI2020

Giant Domain Wall Conductivity in Self‐Assembled BiFeO 3 Nanocrystals

Abstract Ever‐increasing demand on electronic devices with ultrahigh‐density non‐volatile data storage has attracted great interest in novel ferroelectric memories based on conductive ferroelectric domain walls. Embedded in an insulating material, ferroelectric domain walls have the capability of being (re)created, displaced, erased, and altered in their spatial configurations and electronic characteristics. However, the domain wall conductivities are in most cases not yet sufficiently high to ensure the current density required to drive read‐out circuits operating at high speeds. In this work, a giant domain wall current (>10 µA) of a single charged domain wall is obtained through conductive atomic force microscopy with a bias field of 4 V. This is achieved in self‐assembled BiFeO 3 nanocrystals grown by sol‐gel method on Nb‐doped SrTiO 3 substrates. Local configurations of domains and domain wall types are studied using vector piezoresponse force microscopy and high‐resolution transmission electronic microscopy. The enhancement of the wall current is shown to be due to the formation of conducting pathways of charged defects accumulated along domain walls and traversing the nanocrystals. The diverse domain walls can be manipulated by electric field in a perpendicular architecture. The perpendicular array structure of BiFeO 3 nanocrystals should have great potentials for developing perpendicular nanoelectronic prototypes.

Liu, Lisha↗

DOE OSTI2022

Amorphizing noble metal chalcogenide catalysts at the single-layer limit towards hydrogen production

Rational design of noble metal catalysts with the potential to leverage efficiency is vital for industrial applications. Such an ultimate atom-utilization efficiency can be achieved when all noble metal atoms exclusively contribute to catalysis. In this work, we demonstrate the fabrication of a wafer-size amorphous PtSex film on a SiO 2 substate via a low-temperature amorphization strategy, which offers single-atom-layer Pt catalysts with high atom-utilization efficiency (~26 wt%). This amorphous PtSex (1.2 < x < 1.3) behaves as a fully activated surface, accessible to catalytic reactions, and features a nearly 100% current density relative to a pure Pt surface and reliable production of sustained high-flux hydrogen over a 2 inch wafer as a proof-of-concept. Furthermore, an electrolyser is demonstrated to generate a high current density of 1,000 mA cm –2 . Such an amorphization strategy is potentially extendable to other noble metals, including the Pd, Ir, Os, Rh and Ru elements, demonstrating the universality of single-atom-layer catalysts.

36 MATERIALS SCIENCE↗

DOE OSTI2015

Measurement of LHCD edge power deposition through modulation techniques on Alcator C-Mod

The efficiency of LHCD on Alcator C-Mod drops exponentially with line average density. At reactor relevant densities (> 1 · 1020 [m{sup −3}]) no measurable current is driven. While a number of causes have been suggested, no specific mechanism has been shown to be responsible for the loss of current drive at high density. Fast modulation of the LH power was used to isolate and quantify the LHCD deposition within the plasma. Measurements from these plasmas provide unique evidence for determining a root cause. Modulation of LH power in steady plasmas exhibited no correlated change in the core temperature. A correlated, prompt response in the edge suggests that the loss in efficiency is related to a edge absorption mechanism. This follows previous results which found the generation of n{sub ||}-independent SOL currents. Multiple Langmuir probe array measurements of the conducted heat conclude that the lost power is deposited near the last closed flux surface. The heat flux induced by LH waves onto the outer divertor is calculated. Changes in the neutral pressure, ionization and hard X-ray emission at high density highlight the importance of the active divertor in the loss of efficiency. Results of this study implicate a mechanism which may occur over multiple passes, leading to power absorption near the LCFS.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

NASA NTRS1984

Stability of Bromine Intercalated Graphite Fibers

Previous evidence suggested that bromine intercalation compounds of crystalline graphite spontaneously deintercalate when the bromine atmosphere is removed. However, results show that bromine intercalated P-100 graphite fibers are stable for long periods of time. They are stable under vacuum conditions, high humidity, and current densities up to 24,000 A/sq cm. They are thermally stable to 200 C, and at temperatures as high as 400 C still retain 80 percent of the conductivity gained by intercalation. At temperatures greater than 300 C, there is significant oxidative degradation of the fibers. The environmental stability shown by the bromine compound makes it a promising candidate for practical applications in aerospace technology.

Gaier, J. R.↗

DOE OSTI2015

Enhanced Performance of Li|LiFePO4 Cells Using CsPF6 as an Electrolyte Additive

The practical application of lithium (Li) metal anode in rechargeable Li batteries is hindered by both the growth of Li dendrites and the low Coulombic efficiency (CE) during repeated charge/discharge cycles. Recently, we have discovered that CsPF6 as an electrolyte additive can significantly suppress Li dendrite growth and lead to highly compacted and well aligned Li nanorod structure during Li deposition on copper substrates. In this paper, the effect of CsPF6 additive on the performance of rechargeable Li metal batteries with lithium iron phosphate (LFP) cathode was further studied. Li|LFP coin cells with CsPF6 additive in electrolytes show well protected Li anode surface, decreased resistance, enhanced rate capability and extended cycling stability. In Li|LFP cells, the electrolyte with CsPF6 additive shows excellent long-term cycling stability (at least 500 cycles) at a charge current density of 0.5 mA cm-2 without internal short circuit. At high charge current densities, the effect of CsPF6 additive becomes less significant. Future work needs to be done to protect Li metal anode, especially at high charge current densities and for long cycle life.

Environmental Molecular Sciences Laboratory↗

DOE OSTI2024

Advanced silver sheathed 2212/Ag wire for high field magnets

Commercial High Temperature Superconductors (HTS) are all tape shaped (widths > 10 times thickness), because achieving useful current densities required them to be processed into this form, even though this also makes it more problematic to use them in some important coil types. Our product is based on 2212 (Bi2Sr2CaCu2O8) and it is the only HTS that can be processed into high current density wire forms that are similar to proven low temperature superconductors (LTS), while surpassing them in field generating and operating temperature capability. Required now are higher current density, lower cost and longer length 2212 wires to enable broad utilization where HTS tape usage is problematic. In Phase II we developed vital cost-lowering process technology elements and we test-processed longer wires with the standard commercial design as baseline and benchmark for our lower cost, higher quality and longer piece length wire advances. By initial application of Jc-boosting wire features, these wires exhibited significant performance increases. This Phase IIA program has now developed and qualified these technologies for lower cost, higher quality and longer piece length manufacturing in combination with current density-boosting wire features, paving the way to manufacturing capability that is essential for cost-effective commercial utilization of 2212 wire. Technical areas included automated, high uniformity powder packing, advanced drawing, annealing, lubricant cleaning and filament bundling, followed by integration of higher current density wire features and process variations.

17 WIND ENERGY↗

NASA NTRS1975

15 cm cusped magnetic field mercury ion thruster research

The importance of achieving a uniform current density in the exhaust beam of an electrostatic ion thruster is discussed in terms of thrust level and accelerator grid lifetime. A neutral residence time approach is used to propose a magnetic field geometry which should produce a highly uniform beam current density. The discharge chamber length to diameter ratio is shown to be an important optimization parameter and experimental evaluation of the cusped field thruster over a wide range of this parameter is presented. Beam profile measurements 5 cm downstream of the accelerator grid indicate a beam profile flatness parameter which is 25% greater than the SERT II value. Flatness parameters extrapolated to the plane of the accelerator grid are demonstrated to be as high as 0.9.

Beattie, J. R.↗

DOE OSTI2019

Coupling FeNi alloys and hollow nitrogen-enriched carbon frameworks leads to high-performance oxygen electrocatalysts for rechargeable zinc–air batteries

A dual-template strategy for facile preparation of a bifunctional oxygen electrocatalyst for high-performance rechargeable zinc–air batteries has been reported. Coupling FeNi alloys with hollow nitrogen-doped carbon frameworks concludes in exceptionally high electrocatalytic oxygen reduction and evolution activities. In 1 M KOH, the resulting new material exhibits a superior oxygen evolution activity with a low overpotential of 250 mV to deliver 10 mA cm -2 current density, at which the obtained oxygen reduction performance is also comparable to that of commercial Pt/C and the half-wave potential reaches as high as 0.87 V. As a result, the bifunctional oxygen electrocatalysis performance thus obtained (0.61 V, 1 M KOH) ranks among the best of non-precious oxygen electrocatalysts. Using this new catalyst as an air electrode, the as-prepared rechargeable Zn–air battery shows a high current density of 215 mA cm -2 at a voltage of 1.0 V, large peak power density (310 mW cm -2 ), high potential efficiency (64.7% at 10 mA cm -2 ) and prolonged operation durability. This method provides a means to control the surface features, thereby tuning the catalytic properties of the material, and may open up new possibilities for the rational design and synthesis of new materials for electrochemical applications.

25 ENERGY STORAGE↗

DOE OSTI2023

Improving Durability of Fuel Cells with Platinum-rich Alloy Cathode Catalysts

Pt 3 Co-alloy based nanoparticle catalysts are very active for oxygen reduction reaction (ORR) thereby enabling high performance of proton exchange membrane fuel cells (PEMFC) for automotive propulsion. However, these catalyst materials degrade due to a combination of electrochemical surface area (ECSA) loss and dissolution of cobalt-alloying element from the nanoparticles. Dissolution of cobalt has a two-fold impact on the durability of fuel cells—i) a loss in the low-current density kinetic region due to a decrease in specific activity and ii) a loss in the high-current density transport region due to Co 2+ contamination of the ionomer phase. Cobalt dissolution-contamination needs to be mitigated as it limits fuel cell performance and lifetime for heavy-duty automotive applications. In this article, we study the use of PtCo-alloy catalysts with Pt-rich compositions using catalyst-specific accelerated stress test measurement in membrane electrode assemblies to decrease the amount of dissolved Co and mitigate its subsequent contamination effects. We demonstrate Pt 5 Co and Pt 7 Co compositions to enable significant improvements in durability (∼50 mV and ∼100 mV with respect to Pt 3 Co after 30,000 voltage cycles) with a minor but acceptable compromise in the initial specific activity of the catalyst.

08 HYDROGEN↗

NASA NTRS1982

Design, construction and long life endurance testing of cathode assemblies for use in microwave high-power transmitting tubes

The ability of state of the art cathode types to produce current densities of 2A/sq cm, respectively, over a minimum designed life of 30,000 hours of continuous operation without failures was demonstrated. The performance of the state of the art cathode types was evaluated by endurance testing while operating under identical electrical geometrical, and vacuum conditions that realistically duplicate the operating conditions present in a transmitter tube. Although there has been considerable life testing done on high current density types of cathodes, these have beem primarily limited to diodes. A diode and high power microwave tube are grossly different devices. A comparison of these two devices is provided. A diode and high power microwave tube are quite different; one could therefore assume different internal environments, especially in the cathode region. Therefore, in order to establish life capabilities of the cathodes just mentioned, they should be tested in a vehicle which has an internal environment similar to that of a high power microwave tube.

Gorshe, R.↗

DOE OSTI2024

Synergizing Fe 2 O 3 Nanoparticles on Single Atom Fe‐N‐C for Nitrate Reduction to Ammonia at Industrial Current Densities

The electrochemical reduction of nitrates (NO 3 − ) enables a pathway for the carbon neutral synthesis of ammonia (NH 3 ), via the nitrate reduction reaction (NO 3 RR), which has been demonstrated at high selectivity. However, to make NH 3 synthesis cost-competitive with current technologies, high NH 3 partial current densities (j NH3 ) must be achieved to reduce the levelized cost of NH 3 . Here, the high NO 3 RR activity of Fe-based materials is leveraged to synthesize a novel active particle-active support system with Fe 2 O 3 nanoparticles supported on atomically dispersed Fe–N–C. The optimized 3×Fe 2 O 3 /Fe–N–C catalyst demonstrates an ultrahigh NO 3 RR activity, reaching a maximum j NH3 of 1.95 A cm −2 at a Faradaic efficiency (FE) for NH 3 of 100% and an NH 3 yield rate over 9 mmol hr −1 cm −2 . Operando XANES and post-mortem XPS reveal the importance of a pre-reduction activation step, reducing the surface Fe 2 O 3 (Fe 3+ ) to highly active Fe 0 sites, which are maintained during electrolysis. Durability studies demonstrate the robustness of both the Fe 2 O 3 particles and Fe–N x sites at highly cathodic potentials, maintaining a current of −1.3 A cm −2 over 24 hours. This work exhibits an effective and durable active particle-active support system enhancing the performance of the NO 3 RR, enabling industrially relevant current densities and near 100% selectivity.

active support↗

DOE OSTI2017

Transforming from planar to three-dimensional lithium with flowable interphase for solid lithium metal batteries

Solid-state lithium (Li) metal batteries are prominent among next-generation energy storage technologies due to their significantly high energy density and reduced safety risks. Previously, solid electrolytes have been intensively studied and several materials with high ionic conductivity have been identified. However, there are still at least three obstacles before making the Li metal foil-based solid-state systems viable, namely, high interfacial resistance at the Li/electrolyte interface, low areal capacity, and poor power output. The problems are addressed by incorporating a flowable interfacial layer and three-dimensional Li into the system. The flowable interfacial layer can accommodate the interfacial fluctuation and guarantee excellent adhesion at all time, whereas the three-dimensional Li significantly reduces the interfacial fluctuation from the whole electrode level (tens of micrometers) to local scale (submicrometer) and also decreases the effective current density for high-capacity and high-power operations. As a consequence, both symmetric and full-cell configurations can achieve greatly improved electrochemical performances in comparison to the conventional Li foil, which are among the best reported values in the literature. Noticeably, solid-state full cells paired with high–mass loading LiFePO4 exhibited, at 80°C, a satisfactory specific capacity even at a rate of 5 C (110 mA·hour g -1 ) and a capacity retention of 93.6% after 300 cycles at a current density of 3 mA cm -2 using a composite solid electrolyte middle layer. In addition, when a ceramic electrolyte middle layer was adopted, stable cycling with greatly improved capacity could even be realized at room temperature.

25 ENERGY STORAGE↗

DOE OSTI2017

Time and space resolved current density mapping in three dimensions using magnetic field probe array in a high voltage coaxial gap

We present an experimental analysis of the symmetry of current density in a coaxial geometry, diagnosed using a magnetic field probe array and calculations of the Fowler-Nordheim enhancement factor. Data were collected on the coaxial gap breakdown device (240 A, 25 kV, 150 ns, ~0.1 Hz), and data from experiments using 2 different gap sizes and different penetration depths are compared over runs comprising 50 shots for each case. The magnetic field probe array quantifies the distribution of current density at three axial locations, on either sides of a vacuum breakdown, and tracks the evolution with time and space. The results show asymmetries in current density, which can be influenced by changes in the gap size and the penetration depth (of the center electrode into the outer electrode). For smaller gap sizes (400 μm), symmetric current profiles were not observed, and the change in the penetration depth changes both the symmetric behavior of the current density and the enhancement factor. For larger gaps (900 μm), current densities were typically more uniform and less influenced by the penetration depth, which is reflected in the enhancement factor values. Furthermore it is possible that the change in inductance caused by the localization of current densities plays a role in the observed behavior.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

NASA NTRS2018

Shrouded CMC Rotor Blades for High Pressure Turbine Applications

The density of Ceramic Matrix Compos-ite(CMC) materials is approximately 1/3 the density of metals currently used for High Pressure Turbine(HPT) blades. A lower density, and consequently lower centrifugal stresses, increases the feasibility of shrouding HPT blades. Shrouding HPT blades improves aerodynamic eciency, especially for low aspect ratio turbine blades. This paper explores aerodynamic and structural issues associated with shrouding HPT rotor blades. Detailed Navier-Stokes analysis of a rotor blade showed that shrouding improved blade row aerodynamic eciency by 1.3%, when the clearance was 2% of the blade span. Recessed casings were used. Without a shroud the depth of the recess equaled the clearance. With a shroud the recess depth increased by the shroud thickness, which included a knife seal. There was good agreement between the predicted stage eciency for the unshrouded blades and the experimentally measured efficiency. Structural analysis showed a strong interaction between stresses in the shroud and peak stresses at the hub of the blade. A thin shroud of uniform thickness only moderately increased maximum blade stress, but there were very high stresses in the shroud itself. Increasing shroud thickness reduced stresses in the shroud, but increased blade stresses near the hub. A single knife seal added to the thin shroud noticeably decreased maximum shroud stress, without increasing maximum blade stress. Maximum stresses due to pressure loads and combined pressure and centrifugal loads were nearly the same as the maximum stresses for individual pressure or cen-trifugal loads. Stresses due to a 100K temperature

Ceramic Matrix Composite↗

DOE OSTI2026

Electronegativity-Guided Site Differentiation in High-Entropy Alloy for pH-universal Hydrogen Evolution Reactions

Enhancing the intrinsic activity of transition metal catalysts for the hydrogen evolution reaction (HER) remains a critical challenge in sustainable energy conversion. Herein, we report an electronegativity-guided site differentiation strategy in a single-phase CoNiCuMoW high-entropy alloy (HEA) via electrodeposition by incorporating high-electronegativity 4d/5d orbital transition metals (Mo, W) into the face-centered cubic (fcc) matrix (CoNiCu). The as-synthesized HEA demonstrates exceptional HER performance in all pH conditions, delivering an outstanding overpotential of 65 mV (alkaline), 28 mV (acidic), and 155 mV (neutral) at a current density of 100 mA cm−2, showing performance comparable to commercial Pt/C and has excellent long-term stability at high current density (1 A cm−2, 1000 h). X-Ray absorption spectroscopy (XAS) and density functional theory (DFT) calculations reveal that the incorporation of Mo/W simultaneously alters the local coordination environment and induces element-dependent charge redistribution, accompanied by a system-level d-band center downshift, thereby optimizing the hydrogen binding strength across multimetallic sites. Meanwhile, oxophilic Mo/W sites lower the water dissociation energy barrier. These synergistic effects collectively enable efficient and durable pH-universal HER performance.

Wu, Yutong↗

DOE OSTI2020

Ultra‐Steep Slope Impact Ionization Transistors Based on Graphene/InAs Heterostructures

With the continued scaling of transistors, there is a growing trend for developing steep slope transistors with subthreshold swing (SS) below Boltzmann limitation ( k T/ q ). To this end, impact ionization metal oxide semiconductor (I‐MOS) transistors are attractive for a unique combination of high ON‐state current density, small hysteresis, and ultra‐steep SS slope. However, the performance of I‐MOS is generally limited by the relatively thick depletion region and large operation voltage required for the activation of impact ionization (typically >5 V). Herein, a high‐performance I‐MOS is constructed by van der Waals integrating single‐crystal InAs film with graphene. Due to the low bandgap of InAs as well as the semi‐metallic nature of graphene, the InAs/graphene I‐MOS demonstrates a low operation voltage of 1.5 V, high ON‐state current of 230 μA μm −1 , steep SS <0.6 mV dec −1 , and large ON–OFF ratio >10 6 at temperature below 200 K. Furthermore, a negative transconductance and steep current oscillation is observed in the subthreshold regime, and a device working mechanism is proposed for this novel phenomenon. This study not only pushes the performance limit of I‐MOS but also defines a general pathway to van der Waals heterostructures between conventional III–V compound semiconductors and novel 2D materials for unconventional device functions.

Liu, Yuan↗

DOE OSTI2020

Ultralight and fire-extinguishing current collectors for high-energy and high-safety lithium-ion batteries

Inactive components and safety hazards are two critical challenges in realizing high-energy lithium-ion batteries. Metal foil current collectors with high density are typically an integrated part of lithium-ion batteries yet deliver no capacity. Meanwhile, high-energy batteries can entail increased fire safety issues. Here we report a composite current collector design that simultaneously minimizes the ‘dead weight’ within the cell and improves fire safety. An ultralight polyimide-based current collector (9 μm thick, specific mass 1.54 mg cm-2) is prepared by sandwiching a polyimide embedded with triphenyl phosphate flame retardant between two superthin Cu layers (~500 nm). Compared to lithium-ion batteries assembled with the thinnest commercial metal foil current collectors (~6 µm), batteries equipped with our composite current collectors can realize a 16-26% improvement in specific energy and rapidly self-extinguish fires under extreme conditions such as short circuits and thermal runaway.

25 ENERGY STORAGE↗

DOE OSTI2016

Enhanced Electrical Resistivity and Properties via Ion Bombardment of Ferroelectric Thin Films

140 nm PbTiO 3 /20 nm SrRuO 3 thin-film heterostructures were grown on SrTiO 3 (001) single-crystal substrates via pulsed-laser deposition. In order to study the properties of these films, symmetric SrRuO 3 capacitor structures were fabricated using established techniques and dramatic differences were observed in the leakage characteristics of the heterostructures. The high-pressure O 2 and O 2 /Ar heterostructures reveal more than 2 orders of magnitude higher leakage current densities as compared to the low-pressure O 2 heterostructures. In turn, the high leakage current density of the heterostructures grown in high pressures precludes measurement of closed, saturated ferroelectric hysteresis loops, while nearly-square, fully saturated and closed hysteresis loops can be measured for the low-pressure O 2 heterostructures. The defects responsible for poor transport and ferroelectric properties in PbTiO 3 thin films are identified to be isolated point defects such as Pb 3+ centers and lead vacancies, which contribute to hole conduction. Introduction of bombardment-induced defects is shown to be an effective way to quench these trap states by turning them into deep lying defect complexes and clusters which, in turn, leads to a dramatic reduction of leakage current by up to 5 orders of magnitude and improvement of ferroelectric device performance.

36 MATERIALS SCIENCE↗