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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 127 records · Page 7
All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

Simulating Discharge Curves of an All-Aqueous TRAB to Identify Pathways for Improving System Performance

Thermally regenerative ammonia batteries (TRABs) are an emerging technology that use low temperature heat (T < 150 °C) to recharge a flow battery that produces electrical power on demand. The all-aqueous copper TRAB can provide high power densities and thermal energy efficiencies relative to other devices that harvest energy from waste heat, but its performance is adversely impacted by the crossover of undesired species through the membrane and lower cell voltages compared to conventional batteries. In this work, we developed a numerical model to simulate discharge curves while accounting for crossover inefficiencies without tracking all electrolyte species through the membrane. The model was able to successfully reproduce discharge curves across a diverse range of battery conditions using a single fitting parameter to account for decay of electrode standard potential due to species crossover with minimal error (< 5%). The model was then used to simulate different design scenarios to estimate changes in energy output from alterations to the aspects of the battery electrolyte chemistry. Results from this study are used to identify pathways for improving future TRAB designs with respect to energy capacity and cost-effectiveness of the technology.

25 ENERGY STORAGE↗
DOE OSTI2023

Development of an All-Aqueous Thermally Regenerative Redox Flow Battery to Support Fossil Fuel Assets

Low-temperature thermal energy, a largely untapped resource, holds significant promise for large-scale electrical power generation globally. Various stationary sources, including industrial entities and thermal power plants, emit considerable low-temperature heat that currently remains unutilized. This energy is often overlooked because its low temperature renders it unsuitable for efficient power generation using conventional methods. However, current research is exploring diverse technologies capable of converting low-temperature heat into grid-scale power, aiming to enhance grid efficiency, further decarbonization initiatives, and facilitate a shift toward more decentralized power systems. One such innovative technology is the thermally regenerative battery (TRB), noted for its high power and energy densities compared to similar technologies, positioning it as a potential game-changer in power generation. TRBs integrate two scalable and well-established unit operations: a redox flow battery and a distillation column. This integration suggests that once an effective TRB chemistry is established, the pathway to commercialization could be expedited. The copper-based thermally regenerative ammonia battery (Cu aq -TRAB) stands out as the first TRB that circumvents electrodeposition/dissolution reactions, stabilizing Cu(I) and Cu(II) within the electrolyte and maintaining stability of all electroactive species in an aqueous phase. This stabilization has led to improvements in coulombic efficiency, open circuit potential, and copper solubility, thereby enhancing power density, energy density, and overall energy efficiency. Preliminary tests were conducted to determine the effects of various electrolyte species on the performance metrics of the battery, both theoretically and experimentally. These tests revealed that the solubility of copper in the Cu aq -TRAB electrolyte was constrained by the Cu(I)-NH 3 complex. Adjusting the background electrolyte to 5 M NH4Br and the ligand concentration to 4 M NH 3 enabled the copper concentration to reach a maximum of 0.6 M. This modification led to an estimated theoretical maximum energy density of 9.5 Wh L -1 for the Cu aq -TRAB. Additionally, full cell testing indicated a tradeoff between peak power and energy density with varying copper and ammonia concentrations. Increasing the applied current density during discharge linearly raised the average power output, with a minimal reduction in energy density due to a balance between higher ohmic overpotential and reduced time for undesirable ammonia crossover. Furthermore, a comprehensive numerical sensitivity analysis of the complete Cu aq -TRAB system was performed. This analysis aimed to assess how the battery and the distillation column responded to changes in system input parameters, providing insights into optimal research directions for enhancing system performance. The analysis revealed that at room temperature, battery power was significantly more sensitive to ohmic losses than to mass transfer, with reaction rates having minimal impact. This trend continued even at higher temperatures. Also, the thermal energy required for ammonia separation was studied, showing that increased temperatures generally reduced energy requirements, except in low-pressure scenarios above 65 °C. An investigation into membrane performance in the Cu aq -TRAB was undertaken, given the significant impact of ammonia transport control and ohmic losses on system performance. Various membranes were evaluated to identify key performance metrics. Among the tested membranes, Selemion CMVN exhibited the highest performance, with a peak power density of 84 mW cm -2 and average values of 26 ± 6.8 mW cm -2 for power density and 2.9 Wh L -1 for energy density at an applied current density of 50 mA cm -2 . An economic assessment indicated a levelized cost of storage at $410 per MWh under optimal conditions, highlighting the commercial potential of the Cu aq -TRAB when utilizing cost-effective, readily available materials.

25 ENERGY STORAGE↗
DOE OSTI2025

High-Voltage, Intermediate-Temperature, Fe- and Al-Mixed Metal Halide Molten Salt for Molten Sodium Battery Energy Storage

An inorganic Fe and Al halide-based, low-temperature molten salt catholyte is described, which, when paired with a molten sodium anode, has high operating potentials rivaling those of Li ion batteries. The newly developed catholyte consists of metal halides FeCl 3 /FeCl 2 –AlCl 3 –NaCl and is intended to cycle between Fe 3+ /Fe 2+ redox couples in the molten salt. The multicomponent molten salt was initially evaluated for phase behavior and basic electrochemical behavior before full battery testing. The assembled battery, utilizing a 20:35:45 (FeCl 3 :AlCl 3 :NaCl) composition, with a 50.83 Ah/kg theoretical gravimetric capacity and a specific energy of 176.95 Wh/kg, was cycled at variable depths of discharge (DoD) and current densities to determine its cycling efficiencies and limitations. In conclusion, preliminary cycling tests showed two operational potential regimes, with higher potential, 3.91 V (vs Na/Na + ), at low DoD and lower potential, 3.39 V (vs Na/Na + ), at high DoD with excellent energy efficiencies and cycling behavior under both regimes.

Aluminum↗
DOE OSTI2020

A Lithium Metal Anode Surviving Battery Cycling Above 200 °C

Lithium (Li) metal electrode cannot endure elevated temperature (e.g., >200 °C) with the regular battery configuration due to its low melting point (180.5 °C) and high reactivity, which restricts its application in high-temperature Li metal batteries for energy storage and causes safety concerns for regular ambient-temperature Li metal batteries. Herein, this work reports a Li 5 B 4 /Li composite featuring a 3D Li 5 B 4 fibrillar framework filled with metallic Li, which maintains its initial structure at 325 °C in Ar atmosphere without leakage of the liquid Li. The capillary force caused by the porous structure of the Li 4 B 5 fibrillar framework, together with its lithiophilic surface, restricts the leakage of liquid metallic Li and enables good thermal tolerance of the Li 5 B 4 /Li composite. Thus, it can be facilely operated for rechargeable high-temperature Li metal batteries. Li 5 B 4 /Li electrodes are coupled with a garnet-type ceramic electrolyte (Li 6.5 La 3 Zr 0.5 Ta 1.5 O 12 ) to fabricate symmetric cells, which exhibit stable Li stripping/plating behaviors with low overpotential of approximate to 6 mV at 200 °C using a regular sandwich-type cell configuration. This study affords new insights into realizing a stable Li metal anode for high-temperature Li metal batteries with a simple battery configuration and high safety, which is different from traditional molten-salt Li metal batteries using a pristine metallic Li anode.

25 ENERGY STORAGE↗
DOE OSTI2021

Pressure-tailored lithium deposition and dissolution in lithium metal batteries

Unregulated lithium (Li) growth is the major cause of low Coulombic efficiency, short cycle life and safety hazards for rechargeable Li metal batteries. Strategies that aim to achieve large granular Li deposits have been extensively explored, and yet it remains a challenge to achieve the ideal Li deposits, which consist of large Li particles that are seamlessly packed on the electrode and can be reversibly deposited and stripped. In this work, we report a dense Li deposition (99.49% electrode density) with an ideal columnar structure that is achieved by controlling the uniaxial stack pressure during battery operation. Using multiscale characterization and simulation, we elucidate the critical role of stack pressure on Li nucleation, growth and dissolution processes and propose a Li-reservoir-testing protocol to maintain the ideal Li morphology during extended cycling. The precise manipulation of Li deposition and dissolution is a critical step to enable fast charging and a low-temperature operation for Li metal batteries.

25 ENERGY STORAGE↗
DOE OSTI2022

Achieving low-temperature hydrothermal relithiation by redox mediation for direct recycling of spent lithium-ion battery cathodes

Lithium-ion battery (LIB) recycling is an urgent need to address the massive generation of spent LIBs from portable devices and electrical vehicles. However, the large-scale recycling is hampered by economic and safety issues associated with today's recycling processes. In this study, we demonstrate a safe and energy efficient direct regeneration process based on low-temperature hydrothermal relithiation (LTHR) at low pressure for spent LiNi x Co y Mn z O 2 (0 < x,y,z <1, x + y + z = 1, or NCM) cathode materials. A low concentration of low-cost redox mediator is employed to improve the relithiation kinetics of spent NCM materials, enabling full relithiation temperature to be reduced from 220 °C to 100 °C or below. Correspondingly, the pressure incurred in the relithiation process can be reduced from ~25 bar to 1 bar, offering significantly improved operation safety. Specifically, three NCM materials, including chemically delithiated NCM111, cycled (degraded) NCM111, and cycled NCM622, were successfully regenerated with complete recovery of composition, crystal structure, and electrochemical performance, achieving the same effectiveness as that achieved at high temperature process. Meanwhile, the total energy consumption of spent cell recycling and the greenhouse gas emission is also reduced. This work provides a facile and scalable way to more sustainable LIB recycling with high economic return, high operation safety and low cost.

25 ENERGY STORAGE↗
DOE OSTI2024

Effect of Zwitterionic Additives on Solvation and Transport of Sodium and Potassium Cations in (Ethylene Oxide)10: A Molecular Dynamics Simulation Study

Sodium- (Na + ) and potassium- (K + ) ion batteries are cost-effective alternatives to lithium-ion (Li + ) batteries due to the abundant sodium and potassium resources. Solid polymer electrolytes (SPEs) are essential for safer and more efficient Na + and K + batteries because they often exhibit low ionic conductivity at room temperature. While zwitterionic (ZW) materials enhance Li+ battery conductivity, their potential for Na + and K + transport in batteries remains unexplored. In this study, we investigated the effect of three ZW molecules (ChoPO4, i.e., 2-methacryloyloxyethyl phosphorylcholine, ImSO3, i.e., sulfobetaine ethylimidazole, and ImCO2, i.e., carboxybetaine ethylimidazole) on the dissociation of Na + and K + coordination with ethylene oxide (EO) chains in EO-based electrolytes through molecular dynamics simulations. Our results showed that ChoPO4 possessed the highest cation–EO10 dissociation ability, while ImSO3 exhibited the lowest. Such dissociation ability correlated with the cation–ZW molecule coordination strength: ChoPO4 and ImSO3 showed the strongest and the weakest coordination with cations. However, the cation–ZW molecule coordination could slow the cationic diffusion. The competition of these effects resulted in accelerating or decelerating cationic diffusion. Our simulated results showed that ImCO2 enhanced Na + diffusion by 20%, while ChoPO4 and ImSO3 led to a 10% reduction. For K + , ChoPO4 reduced its diffusion by 40%, while ImCO2 and ImSO3 caused a similar decrease of 15%. These findings suggest that the ZW structure and the cationic size play an important role in the ionic dissociation effect of ZW materials.

25 ENERGY STORAGE↗
DOE OSTI2021

Nanostructured, Targeted Layered Metal Oxides as Active and Selective Heterogeneous Electrocatalysts for Oxygen Evolution

Oxygen evolution reaction (OER) is an important chemical transformation that governs the performance of technologically relevant energy conversion and storage processes, such as electrochemical water splitting in electrolyzers and metal-air batteries. This reaction involves the evolution of oxygen gas from (i) oxygen ions formed from water splitting at high temperatures, (ii) oxygen containing species (i.e., OH, OOH) formed from water splitting at low temperatures, and (iii) metal-oxide discharge products (M x O 2 ) in metal-air batteries. One of the main challenges with OER is that it is catalyzed at low temperatures by noble metal-based electrocatalysts, which are expensive (making this process economically unviable), or at high temperatures by metal-oxide based electrocatalysts that are inefficient and lead to high overpotential losses. Our preliminary results, as well as other results in the literature, show that non-noble metal-based oxide electrocatalysts with layered structures, known as nickelate oxides, exhibit promising OER activity. Nickelate oxides (A 2 MO 4+δ ) belong to the Ruddlesden-Popper series composed of alternating perovskite-like and rocksalt-like layers. They are promising OER electrocatalysts due to their high oxygen transport/exchange properties compared to the state-of-the-art perovskite-type oxides. Unfortunately, these materials are fairly unexplored and little is known about the properties that govern their OER activity. Our preliminary studies, where we combine density functional theory (DFT) calculations, selective synthesis and characterization, show that engineering their nanocrystalline structure can significantly impact their catalytic activity.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

Low Melting Temperature Gallium–Indium Liquid Metal Anode for Solid-State Li-Ion Batteries

Solid-state Li-ion batteries are attracting attention for their enhanced safety features, higher energy density, and broader operational temperature range compared to systems based on liquid electrolytes. However, current solid-state Li-ion batteries face performance challenges, such as suboptimal cycling and poor rate capabilities, often due to inadequate interfacial contact between the solid electrolyte and electrodes. To address this issue, we incorporated a gallium–indium (Ga–In) liquid metal as the anode in a solid-state Li-ion battery setup, employing Li 6 PS 5 Cl as the solid electrolyte. Operating at room temperature, this configuration achieved an initial capacity of 389 mAh g –1 and maintained 88% of this capacity after 30 cycles at a 0.05 C rate. It also demonstrated a capacity retention of 66% after 500 cycles at a 0.5 C rate. In comparison to solid anode materials, such as tin, the Ga–In liquid metal exhibited superior cycling stability and rate capacity, which is due to the self-healing and fluid properties of the alloy that ensure stable interfacial contact with solid electrolytes. In situ X-ray diffraction (XRD) and ex situ scanning electron microscope (SEM) analyses revealed that indium does not directly participate in the lithiation/delithiation process. Instead, it helps maintain the alloy’s low melting point, facilitating its return to a liquid state after delithiation. In a comparative analysis of stack pressure during cycling in cells utilizing Ga–In liquid metal and tin, the Ga–In liquid metal cell demonstrated an ability to buffer pressure increases associated with deformation. In conclusion, these findings suggest a promising approach for enhancing solid-state batteries by integrating liquid metal anodes, which improve interfacial contact and stability.

Alloys↗
DOE OSTI2025

Quantitative and mechanistic insights into proton dynamics for fast energy storage

Proton conduction in hydrogen-bond-rich protic electrolytes enables fast mass and charge transport, crucial for electrochemical energy storage and power conversion. Such transport can give proton-based batteries exceptional rate capability and low-temperature operation beyond other working ions. Here we show that in phosphoric acid (H 3 PO 4 ) electrolytes, vehicular and structural proton transport coexist, and their contributions to conductivity can be quantitatively distinguished. We link structural diffusion directly to hydrogen-bond strength, enabling the precise tuning of proton migration. Guided by this, we reveal a double conductivity peak from regulated structural diffusion. The optimal electrolyte (5.8-M H 3 PO 4 ) achieves high overall (232.9 mS cm −1 ) and structural (164.9 mS cm−1) conductivity. A MoO 3 ‖CuFe-TBA battery with this electrolyte outperforms a deep-eutectic benchmark (8.3-M H 3 PO 4 ), delivering >17,474 W kg −1 at room temperature and retaining 15.1 Wh kg −1 at −75 °C. These findings provide a framework for designing advanced protic electrolytes across electrochemical systems.

Li, Ziyue [Fudan University, Shanghai (China, Peop↗
DOE OSTI2025

Machinable, high‐conductivity NaSICON through mitigation of humidity effects during solid‐state synthesis

The Na + super ion conductor (NaSICON, Na 1+x Zr 2 Si x P 3-x O 12 ) is a solid electrolyte well-known for fast, selective Na + transport at low temperatures, uniquely enabling sodium-based batteries. Producing high-quality NaSICON from solid-state methods, especially when cost-effective, potentially hygroscopic precursors are used, is not trivial. To understand and eliminate the influence of humidity during processing, a scheme was developed to reproducibly yield a high Na + conductivity (3.75 mS/cm at 25°C, 81.7 mS/cm at 150°C), high density (97%), and machinable NaSICON without the use of binders, sintering aids, or dopants. Controlled humidity studies over 20%–50% RH coupled with thermal, structural, and electrical analysis reveal that calcination temperatures < 1000°C leave NaSICON processing susceptible to water absorption at > 20% RH due to the presence of hygroscopic Na 3 PO 4 and Na 2 CO 3 during shaping, pressing, and sintering. Water absorption results in NaSICON with lower densities, machinability, and Na+ conductivity, due to impaired intergranular Na+ transport. At the other extreme, fully converting precursor to the NaSICON phase at 1230°C before pressing and sintering leads to poor conductivity and density. By calcining at 1000°C, excellent quality NaSICON may be produced under a range of laboratory environments, enabling low-cost production of high-conductivity, machinable NaSICON necessary the ever-growing energy storage market.

NaSICON↗
DOE OSTI2024

Can a Coating Mitigate Molten Na Dendrite Growth in NaSICON Under High Current Density?

Alkali metals are among the most desirable negative electrodes for long duration energy storage due to their extremely high capacities. Currently, only high-temperature (>250 °C) batteries have successfully used alkali electrodes in commercial applications, due to limitations imposed by solid electrolytes, such as low conductivity at moderate temperatures and susceptibility to dendrites. Toward enabling the next generation of grid-scale, long duration batteries, we aim to develop molten sodium (Na) systems that operate with commercially attractive performance metrics including high current density (>100 mA cm –2 ), low temperature (<200 °C), and long discharge times (>12 h). In this work, we focus on the performance of NaSICON solid electrolytes in sodium symmetric cells at 110 °C. Specifically, we use a tin (Sn) coating on NaSICON to reduce interfacial resistance by a factor of 10, enabling molten Na symmetric cell operation with “discharge” durations up to 23 h at 100 mA cm –2 and 110 °C. Unidirectional galvanostatic testing shows a 70% overpotential reduction, and electrochemical impedance spectroscopy (EIS) highlights the reduction in interfacial resistance due to the Sn coating. Detailed scanning electron microscopy (SEM) and energy-dispersive spectroscopy (EDS) show that Sn-coated NaSICON enables current densities of up to 500 mA cm –2 at 110 °C by suppressing dendrite formation at the plating interface (Mode I). In conclusion, this analysis also provides a mechanistic understanding of dendrite formation at current densities up to 1000 mA cm –2 , highlighting the importance of effective coatings that will enable advanced battery technologies for long-term energy storage.

25 ENERGY STORAGE↗
DOE OSTI2025

Anion sublattice design enables superionic conductivity in crystalline oxyhalides

Solid-state batteries are attractive energy storage systems as a result of their inherent safety, but their development hinges on advanced solid-state electrolytes (SSEs). Most SSEs remain largely confined to single-anion systems (e.g., sulfides, oxides, halides, and polymers). Through mixed-anion design strategy, we develop crystalline Li 3 Ta 3 O 4 Cl 10 (LTOC) and its derivatives with excellent ionic conductivities (up to 13.7 millisiemens per centimeter at 25°C) and electrochemical stability. The LTOC structure features mixed-anion spiral chains, consisting of corner-shared oxygen and terminal chlorine atoms, which induces continuous “tetrahedron-tetrahedron” Li-ion migration pathways with low energy barriers. Additionally, LTOC demonstrates holistic cathode compatibility, enabling solid-state batteries operation at 4.9 volts versus Li/Li + and low temperature, down to −50°C. In conclusion, these findings describe a promising class of superionic conductors for high-performance solid-state batteries.

Zhao, Feipeng [Western University, London, ON (Can↗
DOE OSTI2026

Are There Opportunities To Re-Think How We Manufacture Synthetic Graphite?

This manuscript contributes a Viewpoint article to ACS Sustainable Resource Management and discusses the graphite supply chain, growing mismatch between graphite demand and global manufacturing capacity, current graphite manufacturing technologies, and different feedstocks.

alternative carbon feedstocks↗