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At least 739 records · Page 41
All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

Gate-Controlled Anyon Generation and Detection in Kitaev Spin Liquids

Reliable manipulation of non-Abelian Ising anyons supported by Kitaev spin liquids may enable intrinsically fault-tolerant quantum computation. Here, we introduce a standalone scheme for both generating and detecting individual Ising anyons using tunable gate voltages in a heterostructure containing a non-Abelian Kitaev spin liquid and a monolayer semiconductor. In this study, the key ingredients of our setup are a Kondo coupling to stabilize an Ising anyon in the spin liquid around each electron in the semiconductor, and a large charging energy to allow control over the electron numbers in distinct gate-defined regions of the semiconductor. In particular, a single Ising anyon can be generated at a disk-shaped region by gate tuning its electron number to one, while it can be interferometrically detected by measuring the electrical conductance of a ring-shaped region around it whose electron number is allowed to fluctuate between zero and one. We provide concrete experimental guidelines for implementing our proposal in promising candidate materials like α-RuCl 3 .

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2023

2 kV, 0.7 mΩ•cm2 Vertical Ga2O3 Superjunction Schottky Rectifier with Dynamic Robustness

We report the first experimental demonstration of a vertical superjunction device in ultra-wide bandgap (UWBG) Ga 2 O 3 . The device features 1.8 μm wide, 2×10 17 cm -3 doped n-Ga 2 O 3 pillars wrapped by the charge-balanced p-type nickel oxide (NiO). The sidewall NiO is sputtered through a novel self-align process. Benefited from the high doping in Ga 2 O 3 , the superjunction Schottky barrier diode (SJ-SBD) achieves a ultra-low specific on-resistance (R ON,SP ) of 0.7 mΩ•cm 2 with a low turn-on voltage of 1 V and high breakdown voltage (BV) of 2000 V. The R ON,SP ~BV trade-off is among the best in all WBG and UWBG power SBDs. The device also shows good thermal stability with BV > 1.8 kV at 175 °C. In the unclamped inductive switching tests, the device shows a dynamic BV of 2.2 kV and no degradation under 1.7 kV repetitive switching, verifying the fast acceptor depletion in NiO under dynamic switching. Such high-temperature and switching robustness are reported for the first time in a heterogeneous superjunction. These results show the great potential of UWBG superjunction power devices.

Qin, Yuan↗
DOE OSTI2024

Thermodynamic, Kinetic, and Transport Contributions to Hydrogen Evolution Activity and Electrolyte-Stability Windows for Water-in-Salt Electrolytes

Concentrated water-in-salt electrolytes (WiSEs) are used in aqueous batteries and to control electrochemical reactions for fuel production. The hydrogen evolution reaction is a parasitic reaction at the negative electrode that limits cell voltage in WiSE batteries and leads to self-discharge, and affects selectivity for electrosynthesis. Mitigating and modulating these processes is hampered by a limited fundamental understanding of HER kinetics in WiSEs. Here, in this study, we quantitatively assess how thermodynamics, kinetics, and interface layers control the apparent HER activities in 20 m LiTFSI. When the LiTFSI concentration is increased from 1 to 20 m, an increase in proton activity causes a positive shift in the HER equilibrium potential of 71 mV. The exchange current density, i o , derived from the HER branch for 20 m LiTFSI in 98% purity (0.56 ± 0.05 μA/cm Pt 2 ), however, is 8 times lower than for 20 m LiTFSI in 99.95% (4.7 ± 0.2 μA/cm Pt 2 ) and 32 times lower than for 1 m LiTFSI in 98% purity (18 ± 1 μA/cm Pt 2 ), demonstrating that the WiSE's impurities and concentration are both central in significantly suppressing HER kinetics. The ability and applicability of the reported methods are extended by examining additional WiSEs formulations made of acetates and nitrates.

25 ENERGY STORAGE↗
DOE OSTI2025

Large-signal Stability Analysis of Grid-forming Inverters with Equivalent-circuit Models

Here, this paper proposes an energy function-based direct method for large-signal stability assessment of grid-forming (GFM) inverters leveraging an equivalent-circuit representation of all involved control- and physical-layer dynamics. Three different primary controls, a standard inner-current outer-voltage cascaded-control architecture, output LCL filter, and reference-current saturation limiting are featured in the modeling and analysis framework. A composite energy function for the GFM inverter is obtained by summing up individual energy contributions gleaned from the circuit representation. The approach can readily be generalized to different primary controls, output-filter arrangements, and current limiters since it is based on a circuit-theoretic foundation. Numerical simulations validate the efficacy of the approach in estimating the critical clearing time following a large-signal disturbance.

24 POWER TRANSMISSION AND DISTRIBUTION↗
DOE OSTI2021

Doping- and Strain-Dependent Electrolyte-Gate-Induced Perovskite to Brownmillerite Transformation in Epitaxial La 1– x Sr x CoO 3–δ Films

Much recent attention has focused on the voltage-driven reversible topotactic transformation between the ferromagnetic metallic perovskite (P) SrCoO 3-δ and oxygen-vacancy-ordered antiferromagnetic insulating brownmillerite (BM) SrCoO 2.5 . This is emerging as a paradigmatic example of the power of electrochemical gating (using, e.g., ionic liquids/gels), the wide modulation of electronic, magnetic, and optical properties generating clear application potential. SrCoO 3 films are challenging with respect to stability, however, and there has been little exploration of alternate compositions. Here, we present the first study of ion-gel-gating-induced P. BM transformations across almost the entire La 1-x SrxCoO 3 phase diagram (0 ≤ x ≤ 0.70), under both tensile and compressive epitaxial strain. Electronic transport, magnetometry, and operando synchrotron X-ray diffraction establish that voltage-induced P → BM transformations are possible at essentially all x, including x ≤ 0.50, where both P and BM phases are highly stable. Under small compressive strain, the transformation threshold voltage decreases from approximately +2.7 V at x = 0 to negligible at x = 0.70. Both larger compressive strain and tensile strain induce further threshold voltage lowering, particularly at low x. The P → BM threshold voltage is thus tunable, via both composition and strain. At x = 0.50, voltage-controlled ferromagnetism, transport, and optical transmittance are then demonstrated, achieving Curie temperature and resistivity modulations of similar to 220 K and at least 5 orders of magnitude, respectively, and enabling estimation of the voltage-dependent Co valence. The results are analyzed in the context of doping- and strain-dependent oxygen vacancy formation energies and diffusion coefficients, establishing that it is thermodynamic factors, not kinetics, that underpin the decrease in the threshold voltage with x, that is, with increasing formal Co valence. These findings substantially advance the practical and mechanistic understanding of this voltage-driven transformation, with fundamental and technological implications.

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

Stabilized Lithium, Manganese-Rich Layered Cathode Materials Enabled by Integrating Co-Doping and Nanocoating

While lithium, manganese-rich (LMR) layered oxide cathode materials offer high energy density (>900 Wh kg –1 ) and low cost, LMR is susceptible to continuous capacity and voltage decay from the oxygen migration and side reaction with aqueous electrolyte at high voltage. Herein, the integration of Na/F co-doping (CD) and AlF 3 coating on LMR is achieved without the need of complex atomic layer deposition. Akin to pristine and CD samples, CD with 1 wt % AlF 3 (CD-1.0 wt %) shows excellent electrochemical performance with the capacity and voltage retentions of 93 and 91% after 150 cycles at 0.5C, respectively, and increased ionic conductivity. Spectroscopic analysis indicates that the coating mainly influences the Co distribution, where Co is enriched on the surface, and partial diffusion of Al 3+ ions toward the bulk, leading to a slight change of transition-metal (TM) valence states at the nanometer scale and the formation of a stable Li x (CoAl)O y phase. Post-cycling analysis reveals that CD-1.0 wt % can alleviate the formation of rock-salt structure and Mn dissolution. Besides, little to no metal segregation is detected for the cycled CD-1.0 wt % sample. This finding presents the first instance to apply co-doping and AlF 3 coating as a new strategy to enhance the structural homogeneity and takes another step toward their commercial viability.

25 ENERGY STORAGE↗
DOE OSTI2023

Tuning the thermal activation atmosphere breaks the activity–stability trade-off of Fe–N–C oxygen reduction fuel cell catalysts

Fe–N–C catalysts are the most promising platinum group metal-free oxygen-reduction catalysts, but they suffer from a low density of active metal sites and the so-called activity–stability trade-off. Here we report an Fe–N–C catalyst prepared by adding an optimal amount of H 2 to the traditional inert atmosphere during the thermal activation. The presence of H 2 significantly increases the total density of FeN 4 sites, suppressing the unstable pyrrolic-N-coordinated S1 sites and favouring the stable pyridinic-N-coordinated S2 sites with shortened Fe–N bond lengths. Here, we propose that the intrinsically stable S2 sites are probably arranged in well-graphitized carbon layers, and the S1 sites exist in less-graphitized carbon. H 2 could remove unstable S1 sites and retain stable S2 sites during the pyrolysis to break the challenging activity–stability trade-off. The Fe–N–C catalyst in membrane electrode assemblies maintains a current density of 67 mA cm -2 at 0.8 V (H 2 –air) after 30,000 voltage cycles (0.60 to 0.95 V under H 2 –air), achieving encouraging durability and performance simultaneously.

25 ENERGY STORAGE↗
DOE OSTI2020

Voltage bias stress effects in metal halide perovskites are strongly dependent on morphology and ion migration pathways

The solar-to-power power conversion efficiencies (PCEs) of metal halide perovskites (MHP) have improved over the last decade using a wide variety of methods, including composition manipulation, dopant introduction, and interfacial buffers. These methods, however, have taken little regard for the electronic and interfacial effects such alterations may cause within devices under voltage bias stress – a condition required for most device operation. We investigate how halide and cation substitution in MHP structures [specifically, CH 3 NH 3 PbI 2.87 Cl 0.13 and Cs 0.1 (MA 0.17 FA 0.83 ) 0.9 Pb(I 0.83 Br 0.17 ) 3 ] effects the current behavior of devices while under a range of voltage bias stress in both light and dark conditions. Additionally, conducting in depth investigations into the electronic and morphological differences between these two MHP devices, we confirmed their unique voltage bias stress effects are due to intrinsic behavior within the perovskite structure. Importantly, we also determined how crystallite orientation can influence ion migration and therefore alter charge transport and current stability in MHP photovoltaic devices.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Portable Soft X-Ray Diagnostics for Transformative Fusion-Energy Concepts (Final Scientific/Technical Report)

A time-gated extreme-ultraviolet spectrometer was fielded on a transformative fusion-energy device, FuZE-Q at Zap Energy, Inc. (ZEI), a sheared-flow-stabilized z-pinch. Plasma emission spectra were collected in the 5–40 nm wavelength (30–250 eV) range. This was the first time a direct-vacuum-coupled, high-voltage, deposition-sensitive diagnostic was fielded on this type of dense-plasma fusion device. To overcome the special challenges of such a coupling, a unique, highly effective implementation was developed, with fast (10-ns risetime) pulsed high-voltage electronics and a multi-stage differential pumping system. This enabled the UNR spectrometer to collect three independently timed spectra per FuZE-Q shot while also protecting sensitive internal components. Analysis of line emission identified oxygen (N-, C-, B-, Be-, Li-, and He-like O), peaking in intensity shortly after maximum current (>500 kA). Spectral databases and collisional-radiative modeling have been used to identify impurities and estimate edge-plasma temperatures.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2022

Time Delay of Wide Area Damping Control in Urban Power Grid: Model-Based Analysis and Data-Driven Compensation

Due to the rapid development of economies, large urban cities consume an increasing amount of energy and have a higher requirement for power quality. Voltage source converter based high voltage direct current (VSC-HVDC) is a promising device to transmit clean power from remote regions to urban power systems, while also providing wide area damping control (WADC) for frequency stabilization. However, the time-delay naturally existing in the VSC-HVDC system may degrade the performance of WADC and even result in instability. To address this issue, this paper develops a time-delay correction control strategy for VSC-HVDC damping control in urban power grids. First, a small signal model of WADC is built to analyze the negative impacts of time delay. Then, a data-driven approach is proposed to compensate for the inherent time delay in VSC-HVDC damping control. The extensive training data will be generated under various disturbances. After offline training, the long short-term memory network (LSTM) can be implemented online to predict the actual frequency deviation based on real-time measurements. Finally, the proposed method is validated through MATLAB-Simulink in a two-area four-machine system. The results indicate that the data-driven compensation has a strong generalization ability for random delay time constants and can improve the performance of WADC significantly.

24 POWER TRANSMISSION AND DISTRIBUTION↗
DOE OSTI2022

Mechanistic Elucidation of Electronically Conductive PEDOT:PSS Tailored Binder for a Potassium‐Ion Battery Graphite Anode: Electrochemical, Mechanical, and Thermal Safety Aspects

Potassium-ion batteries (KIBs) are considered more appropriate for grid-scale storage than lithium-ion batteries (LIBs) due to similar operating chemistry, abundant precursors, and compatibility with low-cost graphite anodes. However, a larger ion reduces rate capabilities and exacerbates capacity fading from volumetric expansion. In this report, conductive polymer, poly(3,4-ethylenedioxythiophene) polystyrene sulfonate (PEDOT:PSS), is substituted for standard insulating polyvinylidene fluoride (PVDF). Half-cells using carbon black (CB) in continuously conductive PEDOT:PSS/CB binder outperforms PVDF/CB by mitigating electrically isolated “dead” graphite, improving 100 cycle capacity retention at C/10 from 63 to 80%. Enhanced electrical contact with PEDOT:PSS/CB also reduces ion impedance and improves rate capabilities. Without CB however, PEDOT:PSS binder performs poorly in electrochemical studies despite promising ex situ electronic conductivity. This discrepancy is mechanistically elucidated through identification of redox activity between PEDOT:PSS and K + which results in high impedances in the anode operating voltage window. Additionally, the impact of conducting binder on mechanical properties and thermal safety of the anode is investigated. Brittleness and poor wettability of PEDOT:PSS are identified as issues, but greater stability against reactive KC 8 reduces overall heat generation. Binder substitution offers a promising means of mitigating issues with current KIB anodes regardless of active material, and the work herein addresses issues towards further improvement.

electrochemical impedance spectroscopy↗
DOE OSTI2024

Crack‐Free Single‐Crystalline LiNiO 2 for High Energy Density All‐Solid‐State Batteries

Abstract Single‐crystalline layered oxide (LiNi 1‐ x ‐ y Mn x Co y O 2 ) cathodes have been found to exhibit exceptional electrochemical properties when coupled with various inorganic solid electrolytes (ISEs) in all‐solid‐state batteries (ASSBs). Their advantages stem from the robust morphological integrity with the absence of grain boundaries and the high electrochemical oxidative stability. Here, ASSBs featuring single‐crystalline LiNiO 2 (LNO) with the highest Ni content are reported, offering a high theoretical specific capacity of 275 mAh g ‐1 alongside a high average discharge voltage (3.7 V vs Li + /Li). Through a careful investigation, it is demonstrated that micron‐sized single‐crystalline LNO (µSC‐LNO) composite cathodes with a halide ISE exhibit a high initial discharge capacity of 205 mAh g ‐1 with an outstanding cycle performance over 200 cycles in room‐temperature ASSBs. The significance of engineering parameters is emphasized, such as particle size and specific density, in promoting a homogeneous and fast Li + transport within the composite cathodes. Furthermore, the formation of undesirable interphase between the halide ISE in the cathode and sulfide ISE separator is elucidated, which may be a critical factor impeding long‐term cyclability of ASSBs. This work provides insights into the design of composite cathodes for high‐energy‐density ASSBs.

Chemistry↗
DOE OSTI2025

Stability and Performance of 3d Transition Metal Carbo‐Sulfides: A Density Functional Theory Exploration for Li‐Ion Battery Anodes

As the demand for high-performance and reliable energy storage devices continues to rise, identifying new anode materials is crucial for advancing Li-ion battery (LIB) technology. Inspired by recent experimental breakthroughs in synthesizing two-dimensional transition metal carbo-chalcogenides (2D-TMCCs), density functional theory calculations are performed to systematically explore their sulfide variants (TM 2 S 2 C) spanning all 3d transition metals in three possible phases. Through comprehensive evaluations of thermodynamic, dynamic, mechanical, and thermal stabilities, seven stable 2D-TMCC candidates are identified, four of which exhibit superior battery performance. Notably, V-based 2D-TMCCs across all three phases deliver moderate open-circuit voltages (OCV), efficient Li diffusion, and substantial capacities, making them promising candidates for industrial applications without requiring specific phase controls. A Cr-based 2D-TMCC (with sulfur atoms above carbon atoms) offers the highest capacity of 515.40 mAh g −1 , the lowest Li diffusion barrier, and an optimal OCV, highlighting its appealing potential as an anode material for LIBs. Furthermore, significant Li–Li spacing and pronounced electron delocalization in these four 2D-TMCCs suggest a reduced risk of dendrite formation. This work expands the 2D-TMCC family and identifies up-and-coming candidates for next-generation LIB anodes.

anode materials↗
DOE OSTI2022

Phosphoric acid pre-treatment to tailor polybenzimidazole membranes for vanadium redox flow batteries

We repot vanadium redox flow batteries (VRFBs) use ion-selective membranes for transporting ionic species while separating the positive and negative electrolytes. In this paper, we report phosphoric acid doped polybenzimidazole (PBI) membranes that yield high ionic selectivity and conductivity in VRFBs. The phosphoric acid pre-treatment swells the PBI matrix irreversibly and increases its sulfuric acid doping in VRFB electrolytes. The pre-treated membranes show comparable area resistance with Nafion-212 with better selectivity towards vanadium ions. A low resistance was obtained with a reduced membrane thickness, which can reduce the overall cost of materials. The VRFB using an optimized phosphoric acid pre-treated PBI membrane demonstrates coulombic, voltage, and energy efficiencies of 99.7, 90.3, and 90.0%, respectively, at 40 mA cm -2 while achieving ~40% higher discharge capacity compared to Nafion-212. Furthermore, the VRFB cell shows excellent cycling stability, i.e., only 6.8% or 0.068% per cycle capacity decay for 100 cycles while maintaining coulombic efficiency at >99.9% (98.5% coulombic efficiency for Nafion-212 with a capacity decay of 0.42% per cycle) proving the effectiveness of pre-treatment of phosphoric acid on PBI membranes.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Role of Electrolyte in Overcoming the Challenges of LiNiO 2 Cathode in Lithium Batteries

LiNiO 2 (LNO) is a high-capacity and model cathode first discovered in the 1980s that fell out of favor due to its intrinsic instabilities. However, research activities toward LNO are once again on the rise as the push for higher-energy-density cells marches on. Here we demonstrate here that with appropriate modern electrolytes, major performance improvements can be achieved with LNO with no additional modifications. Cells with a localized high concentration electrolyte (LHCE) deliver 92% capacity retention after 200 cycles compared with 56% capacity retention in a baseline carbonate electrolyte, maintain 94% capacity after high-voltage storage compared with 77% capacity, and display a higher onset temperature of thermal runaway of 244 °C compared with 188 °C. These improvements are attributed to the LHCE’s high oxidative stability and its formation of fluorine-rich interphases. Although further characterization of this new class of electrolyte is necessary, this work demonstrates that modern electrolytes can be drop-in enablers of high-capacity, long-cycle-life cells.

25 ENERGY STORAGE↗
DOE OSTI2022

Bifacial all-perovskite tandem solar cells

The efficiency of all-perovskite tandem devices falls far below theoretical efficiency limits, mainly because a widening bandgap fails to increase open-circuit voltage. We report on a bifacial all-perovskite tandem structures with an equivalent efficiency of 29.3% under back-to-front irradiance ratio of 30. This increases energy yield and reduces the required bandgap of a wide-bandgap cell. Open-circuit voltage deficit is therefore minimized, although its performance under only front irradiance is not ideal. The bifacial device needs a sputtered rear transparent electrode, which could reduce photon path length and deteriorate stability of Pb-Sn perovskites. Embedding a light-scattering micrometer-sized particle layer into perovskite to trap light, effectively increases absorptance by 5 to 15% in the infrared region. Using a nonacidic hole transport layer markedly stabilizes the hole-extraction interface by avoiding proton-accelerated formation of iodine. These two strategies together increase efficiency of semitransparent Pb-Sn cells from 15.6 to 19.4%, enabling fabrication of efficient bifacial all-perovskite tandem devices.

14 SOLAR ENERGY↗
DOE OSTI2020

Sweeping potential regulated structural and chemical evolution of solid-electrolyte interphase on Cu and Li as revealed by cryo-TEM

A fundamental understanding of solid-electrolyte interphase (SEI) is paramount importance for controlling the cycling performance of rechargeable lithium metal batteries. The structural and chemical evolution of SEI with respect to electrochemical operating condition remains barely established. Here we develop a unique method for imaging the evolution of SEI formed on the Cu foil under sweeping electrochemical potential. By using cryogenic TEM imaging combined with energy dispersive X-ray spectroscopy and X-ray photoelectron spectroscopy electronic structure analyses, we reveal that, for the vinylene carbonate (VC)-free electrolyte, the SEI formed at 1.0 V is a monolithic amorphous structure, which evolves to amorphous matrix embedded with Li 2 O particles as the voltage decreases to 0 V. In the case of VC-containing electrolyte, the SEI is featured by an amorphous matrix with Li 2 O particles from 1.0 V to 0 V. The thickness of SEI formed on Cu foil increases with decreasing voltage. Associated with the localized charge modulation by the surface topographic feature and defects in the Cu foil, the SEI layer shows direct spatial correlation with these structural defects in the Cu. In addition, upon Li deposition, the SEI formed on the Li metal has similar thickness with, but different composition from the SEI formed on the Cu foil at 0 V. Furthermore, those results provide insight toward SEI engineering for enhanced cycling stability of Li metal.

25 ENERGY STORAGE↗
DOE OSTI2024

Importance of High Valence Element Nb in Ni-Rich Layered Cathodes for High-Voltage Lithium-Metal Batteries

Ni-rich layered cathode materials have attracted extensive attention due to their higher energy density and technological maturity in commercialization. As the nickel content is raised, especially surpassing 80%, the increased energy density comes with the tradeoff of diminished thermal stability and increased electrochemical structural instability of the cathode. Compared with Co, Al, B, and Ta, the introduction of high valence element Nb significantly improved the electrochemical cycling, delivering a capacity of 202 mAh/g, corresponding to a capacity retention of 92% after 200 cycles tested at 45 °C. Further, the ex situ differential scanning calorimetry and in situ isothermal microcalorimetry demonstrate that the Nb-modified cathode has the potential to enhance the safety of ultrahigh nickel (Ni) NMCs and displays remarkable resilience to extensive cycling by inhibiting high-temperature decomposition reactions and exhibiting a lower heat flow during electrochemical cycling.

25 ENERGY STORAGE↗