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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 19 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

Influence of Linker Group on Bipolar Redox-Active Molecule Performance in Non-Aqueous Redox Flow Batteries

Redox flow batteries (RFBs) are an attractive choice for stationary energy storage of renewables such as solar and wind. Non-aqueous redox flow batteries (NARFBs) have garnered broad interest due to their high voltage operation compared to their aqueous counterparts. Further, the utilization of bipolar redox-active molecules (BRMs) is a practical way to alleviate crossover faced by asymmetric RFBs. In this work, ferrocene (Fc) and phthalimide (PI) are covalently linked with various tethering groups which vary in structure and length. The compiled results suggest that the length and steric shielding ability of the linker group can greatly influence the stability and overall performance of Fc-n-PI BRM-based NARFBs. Primary sources of capacity loss are found to be BRM degradation for straight chain spacers <6 carbons and membrane (Nafion) fouling. Fc-hexyl-PI provided the most stable battery cycling and coulombic efficiencies of >98 % over 100 cycles (~13 days). NARFB using Fc-hexyl-PI as an active material exhibited high working voltage (1.93 V) and maximum capacity (1.28 Ah L -1 ). Additionally, this work highlights rational strategies to improve cycling stability and optimize NARFB performance.

25 ENERGY STORAGE↗
DOE OSTI2025

Harnessing Redox-Active Molecules in Alkylammonium Halide-Based Eutectic Solvents for Redox Flow Batteries

Redox flow batteries (RFBs) are promising for large-scale energy storage, however, advancements in performance and cost-effectiveness are critical factors for adoption. Here we report on alkylammonium halide based eutectic solvents (ESs) and found that a ESs comprising of diethylammonium chloride or bromide, in ethylene glycol demonstrated exceptional stability and a wide electrochemical stability window, making it a promising candidate for RFB applications. The electrochemical stability and redox behavior of the alkylammonium halide-based ESs are significantly influenced by hydrogen-bonding interactions, modulated by the alkyl chain length of the cation and the nature of the anion. A redox-active eutectic electrolyte containing 0.45 M methyl viologen dichloride (MV 2+ ) paired with acetylferrocene exhibited reversible redox behavior with a maximum open-circuit voltage of ∼1.34 V. The first redox couple, representing the viologen dication to radical cation transition, exhibited remarkable stability with consistent performance, achieving an energy efficiency near 70% at charge-discharge current densities of 10 mA cm −2 over 160 cycles with about 3% loss of the initial capacity. This study highlights the potential of alkylammonium halide DES systems for implementing eutectic-based RFB technologies in the future.

25 ENERGY STORAGE↗
DOE OSTI2024

An All-Soluble Fe/Mn-Based Alkaline Redox Flow Battery System

Redox flow batteries (RFBs) are membrane-separated rechargeable flow cells with redox electrolytes, offering the potential for large-scale energy storage and supporting renewable energy grids. Yet, creating a cost-effective, high-performance RFB system is challenging. In this work, we investigate an Fe/Mn RFB alkaline system based on the [(TEA)Fe–O–Fe(TEA)] 3– / 4– and MnO 4 – / 2– redox couples with a theoretical cell voltage of ~1.43 V. This combination has not been systematically studied previously, but it can lead to a very low-cost and sustainable materials for high energy storage. Constant current cycling tests were performed at ±41 mA cm –2 between 20% and 80% SOC over 800 h (400 cycles) with an apparent Coulombic efficiency (CE) approaching 100%, while the voltage efficiency (VE) gradually decreased from ~75.3% to ~61.4% due to increasing internal resistances. Finally, the voltage efficiency loss can be mitigated through a periodic acid treatment to remove MnO 2 deposits from the separator.

25 ENERGY STORAGE↗
DOE OSTI2026

Mechano-chemical understanding of NaSICON for aqueous redox-flow batteries

Redox-flow batteries utilizing a sodium superionic conductor (NaSICON) can be cost-effective systems for grid energy storage by combining high sodium selectivity with reliance on abundant, low-cost elements. However, improving membrane toughness while maintaining a sufficiently thin membrane for ion conduction is needed. Addressing this issue requires deeper insight into the mechanical properties of NaSICON, its interactions with aqueous chemistries, and the chemo-mechanical degradation mechanisms that arise at the intersection of these phenomena. Here, we provide a framework for understanding these problems, strategies to address them, and highlight the potential of unconventional sintering and thin-film fabrication to optimize the performance of NaSICON in practical flow cells.

Grid energy storage↗
DOE OSTI2024

Strategically Modified Ligand Incorporating Mixed Phosphonate and Carboxylate Groups to Enhance Performance in All-Iron Redox Flow Batteries

Iron redox flow batteries (Fe-RFBs) hold significant promise for achieving cost-effectiveness and utilizing abundant materials for stationary energy storage applications. Here, a design of a novel Fe complex utilizing a nitrogenous phosphonate/carboxylate mixed ligand, N,N-Bis(phosphonomethyl)glycine (BMPG), is presented to achieve high performance Fe anolyte. Compared to its all-phosphonate form, nitrilotri(methylphosphonic acid) (NTMPA), the new complex Fe(BPMG) 2 demonstrates a negatively shifted redox potential, resulting in ≈0.07 V (≈10%) increase in battery output voltage. Full battery testing paired with ferrocyanide catholyte demonstrates stable cycling (capacity degradation <0.0001%/cycle) over 730 consecutive charge/discharge cycles with Coulombic Efficiency of 100% at a current density of 20 mA cm -2 under near neutral pH (≈8). Of particular interest, density functional theory (DFT) studies and operando Raman measurements provide strong evidence supporting a molecular structure in BPMG, which reveals the mixed phosphonate/carboxylate groups in BPMG maintain the octahedral coordination of the Fe ion center with phosphonates exclusively, while leaving the carboxylate unbound for both Fe(II) and Fe(III) complexes. This structural similarity between BPMG-based Fe(II) and Fe(III) complexes effectively mitigates the slow redox reaction kinetics observed in Fe(NTMPA) 2 anolyte, where significant ligand reorientation occurs between Fe(II) and Fe(III) complexes.

25 ENERGY STORAGE↗
DOE OSTI2024

Binder-Coated Carbon Cloth Electrodes for All-Vanadium Redox Flow Batteries

Vanadium redox flow batteries (VRFBs) are a promising solution for integrating intermittent renewable energy sources into the existing power grid. However, enhancing the electrochemical performance of VRFBs is critical for their widespread adoption in grid-scale energy storage. This study investigates the impact of adding a porous binder to a carbon-cloth electrode, with a focus on optimizing thermal activation conditions. The electrochemical performance of the binder-coated electrodes compared to uncoated electrodes is evaluated through electrochemical impedance spectroscopy, polarization curve measurements, and charge-discharge cycling. The surface morphology and structural integrity of the binder-coated electrodes at each activation stage are examined using various material characterization techniques to assess the effects of thermal activation. The results are benchmarked against the experiments using non-coated electrodes to determine the performance improvements offered by the binder coating. Notably, the study reveals that binder-coated electrodes exhibit significantly lower resistance and improved efficiency compared to their uncoated counterparts, with optimal activation conditions enhancing performance metrics crucial for VRFB applications. These findings provide valuable insights for further optimizing electrode design and activation strategies, advancing the development of more efficient VRFB systems for large-scale energy storage.

Caiado, Ashley A.↗
DOE OSTI2025

A hybrid numerical and machine learning framework for evaluating the performance of a 780 cm 2 aqueous organic redox flow battery

Aqueous organic redox flow battery (AORFB) is a promising cost-competitive technology for large-scale energy storage. Among existing work, the dihydroxyphenazine (DHP)-based AORFB has demonstrated high energy density and low capacity degradation in 10 cm2 cells during lab tests. However, its commercial-scale performance in more complex environments remains unknown, posing a barrier for commercialization. To address this gap, this work presents a comprehensive performance evaluation of a 780 cm 2 DHP-based AORFB by combining physics-based numerical model, machine learning (ML)-based surrogate models, and ML-derived sensitivity quantification. Specifically, we first select 12 key battery parameters that include 10 physicochemical quantities and 2 operation quantities, then select 6 performance metrics that include energy efficiency (EE), discharging capacity, charging energy, and power losses due to concentration, activation, and ohmic over-potentials. With such selection, 12800 combinations of the 12 parameters are subsequently generated using the Latin Hypercube Sampling method. These combinations, together with 38 pre-defined State of Charge, are then integrated to a validated AORFB model developed in COMSOL to compute the performance metrics. With both input parameters and performance metrics, 60 deep neural network (DNN) surrogate models are then trained to approximate the relationship between the 10 physicochemical quantities and 6 performance metrics at each flow rate and current density. Sensitivity scores are then calculated based on the DNN models. Two additional sensitivity analysis tools, i.e., MARS, and SHAP, are also used to cross-validate the sensitivity scores from the DNN. The results demonstrate that 1) the standard potential ranks the first in controlling EE and charging energy, 2) the membrane conductivity is most critical for power loss and EE, and 3) specific area and reaction rate control activation power loss.

25 ENERGY STORAGE↗
DOE OSTI2024

Stable, Impermeable Hexacyanoferrate Anolyte for Nonaqueous Redox Flow Batteries

Redox-active molecules, or redoxmers, in nonaqueous redox flow batteries often suffer from membrane crossover and low electrochemical stability. Transforming inorganic polyionic redoxmers established for aqueous batteries into nonaqueous candidates is an attractive strategy to address these challenges. Here, in this study, we demonstrate such tailoring for hexacyanoferrate (HCF) by pairing the anions with tetra-n-butylammonium cation (TBA + ). TBA 3 HCF has good solubility in acetonitrile and >1 V lower redox potential vs the aqueous counterpart; thus, the familiar aqueous catholyte becomes a new nonaqueous anolyte. The lowering of redox potential correlates with replacement of water by acetonitrile in the solvation shell of HCF, which can be traced to H-bond formation between water and cyanide ligands. Symmetric flow cells indicate exceptional stability of HCF polyanions in nonaqueous electrolytes and Nafion membranes completely block HCF crossover in full cells. Ion pairing of metal complexes with organic counterions can be effective for developing promising redoxmers for nonaqueous flow batteries.

25 ENERGY STORAGE↗
DOE OSTI2024

Machine learning for the redox potential prediction of molecules in organic redox flow battery

Here, organic redox flow batteries (ORFB) are recognized as an innovative technology for the large-scale storage of renewable energy. The redox potential of organic redox-active molecules plays a vital role in their performance. Advanced screening techniques like high-throughput experiment and machine learning (ML) have significantly enhanced organic material performance and transformed the field of ORFB. However, the scarcity of experimental data poses a considerable challenge for ML model development in this domain. In our study, we developed lightweight graph-based Gaussian process regression (GPR) models with GPU-accelerated marginalized graph kernel and hybrid kernel to predict the redox potentials of organic redox-active molecules for ORFBs, specifically focusing on small datasets. To evaluate model accuracy, we created a new experimental database of organic redox-active molecules by the data from hundreds of published papers and assembled previous computational datasets. We also considered some key parameters, such as pH conditions and solvent type, to assess their impact on redox potential prediction. Our GPR model predicted redox potentials with high accuracy across all datasets using minimal training data. The study provides powerful tools for molecule screening and design and delivers valuable guidance on designing training datasets for costly experiments.

25 ENERGY STORAGE↗
DOE OSTI2025

Conjugation effect of amine molecules in non-aqueous Mg redox flow batteries

Nonaqueous magnesium redox flow batteries (Mg RFBs) are attractive for low-cost, high-energy-density and long-cycle-life stationary energy storage applications. However, state-of-the-art cathode redox-active molecules suffer from low solubility and low redox potential. Herein, we screened a range of cathode redox-active molecules and identified amine molecules as optimal to couple with the Mg anode. The properties of amine derivatives and their performances were collected to establish the correlation between molecular structures and electrochemical performances. The redox potential and solubility of these amine molecules were influenced by the π-conjugated and non-conjugated structures of amine derivatives. Density functional theory (DFT) simulations and the inverse aromatic fluctuation index (FLU −1 ) verified that conjugation had an important role in stabilizing the molecule and increasing its redox potential. Notably, tris[4-(diethylamino)phenyl]amine (TDPA) achieved the highest theoretical energy density (∼120 Wh L −1 ) due to its high solubility (∼0.9 M) and voltage (∼2.5 V vs. Mg/Mg 2+ ). We also demonstrated that ether solvents were crucial for stable, high-solubility catholytes, while bulk anions did not affect the redox potential of these p-type molecules. In a Mg-amine RFB configuration, the battery delivered 2.50 V, a specific discharge capacity of 106.5 mAh g −1 , an initial coulombic efficiency of 90.74%, and a capacity retention of 93.88% after 150 cycles.

Qin, Yunan [University of Utah, Salt Lake City, UT↗
DOE OSTI2025

Bipolar plate flow channel designs for vanadium redox flow battery: a review

Vanadium redox flow battery is one of the preferred systems for grid scale energy storage due to long service life (>20000 cycles), higher efficiency (>85 %), deep discharge capability (>95 % DoD), and inherent scalability and safety. Among system components, flow field is most critical as it governs electrolyte distribution, mass transport and hydraulic performance. Here, this review examines emerging flow channel geometries, highlighting the impact of channel width (0.66 to 1.5 mm), depth (1 to 1.5 mm) and land width (0.5 to 1.5 mm) can reduce pressure drop to <10 kPa while enabling power densities above 600 mW.cm -2 . A key finding is that low channel width to depth ratio (<1) enhances voltage and energy efficiencies by improving under rib convection. The review also provides an overview of progress and perspective in bipolar plate materials, manufacturability, and shunt current mitigation strategies for stack scaling up. Cost analysis emphasizes the influence of flow field designs on the levelized cost of storage and pathways towards the US DOE's $\$$0.05 per kWh energy generation cost target. In addition, opportunities for AI/ML/DT tools assisted design and data driven optimization strategies are also outlined to accelerate next generation flow field development.

Efficiency optimization↗
DOE OSTI2025

Triphenylphosphine Oxide-Derived Anolyte for Application in Nonaqueous Redox Flow Battery

Recent advances in redox flow batteries have made them a viable option for grid-scale energy storage, however they exhibit low energy density. One way to boost energy density is by increasing the cell potential using a nonaqueous system. Molecular engineering has proven to be an effective strategy to develop redox-active compounds with extreme potentials but these are usually challenged by resource sustainability of the newly developed redox materials. Here, we investigate the utility of phosphine oxides as anolytes with extremely negative potentials. Specifically, we found that cyclic triphenylphosphine oxide (CPO), has a highly negative potential (–2.4 V vs Fc/Fc + ). Importantly, CPO is synthesized from triphenylphosphine oxide, a common industrial chemical waste with no commercial value. Structural and electrochemical characterization of the reduced radical anion showed that enhanced stability is due to cyclization or extended pi-conjugation. Importantly, mechanistic investigation into the decomposition of CPO under various solvents and electrochemical conditions allowed us to utilize an acetonitrile/DMF binary solvent system to enable a long-lived anolyte which exhibited no fade over 350 cycles. In conclusion, this work led to the development of a waste-derived cyclic phosphine oxide that exhibits excellent cycling stability making it an ideal anolyte toward the development of energy-dense RFBs.

25 ENERGY STORAGE↗
DOE OSTI2024

Relating Solvent Parameters to Electrochemical Properties to Predict the Electrochemical Performance of Vanadium Acetylacetonate for Non-Aqueous Redox Flow Batteries

Non-aqueous redox flow batteries have shown promise for applications in grid energy storage. Increasing the efficiency of these batteries by developing the electrolyte chemistries is needed. Herein, we investigate the correlation between solvent properties and the electrochemical parameters of vanadium acetylacetonate V(acac) 3 . Using cyclic voltammetry (CV) and rotating disk electrode experiments (RDE), we show that trends in the performance of the V(acac) 3 kinetics are directly related to solvent properties. In this study, we found strong relationships between the solvents polarity, viscosity, and donor number with the electrochemical behavior of V(acac) 3 in terms of the electrochemical working widow, electron kinetics and stability towards cycling. Based on these finding, we also demonstrate how solvent selection can be improved with limited a priori knowledge.

25 ENERGY STORAGE↗
DOE OSTI2024

Condensation-based redox flow battery rebalancing

In a redox flow battery (RFB), the base solvent of the electrolytes tends to migrate across the barrier layer from one electrode toward the other. This can result in a volume and concentration imbalance between the electrolytes that is detrimental to battery efficiency and capacity. Compatible electrolytes can be mixed to rebalance the system, but for incompatible electrolytes mixing is not a viable option. To this end, the RFB herein includes a separator that recovers base solvent from the vapor phase of one of the electrolytes and returns the recovered base solvent to the other electrolyte to thereby reverse the imbalance.

Saraidaridis, James D.↗
DOE OSTI2024

Physics-Guided Continual Learning for Predicting Emerging Aqueous Organic Redox Flow Battery Material Performance

Aqueous organic redox flow batteries (AORFBs) have gained popularity in renewable energy storage due to their low cost, environmental friendliness and scalability. The rapid discovery of aqueous soluble organic (ASO) redox-active materials necessitates efficient machine learning surrogates for predicting battery performance. The physics-guided continual learning (PGCL) method proposed in this study can incrementally learn data from new ASO electrolytes while addressing catastrophic forgetting issues in conventional machine learning. Using a AORFB database with a thousand potential materials generated by a 780 $\text{cm}^2$ interdigitated cell model, PGCL incorporates AORFB physics to optimize the continual learning task formation and training strategies to retain previously learned battery material knowledge. Finally, the trained PGCL demonstrates its capability in assessing emerging ASO materials within the established parameter space when evaluated with the dihydroxyphenazine isomers.

25 ENERGY STORAGE↗
DOE OSTI2024

Electrode-decoupled redox flow battery

Described herein is a novel electrode-decoupled redox flow battery, a novel reinforced electrode-decoupled redox flow battery, and methods of using same to store energy. Advantages of these novel electrode-decoupled redox flow batteries include long life, excellent rate capability, and stability.

Sankarasubramanian, Shrihari↗
DOE OSTI2024

Miniaturize the Redox Flow Battery for Accelerated Materials Discovery and Development

Redox flow batteries are a promising technology for grid-scale energy storage. The aqueous organic redox flow battery is of particular interest for its potentially low material cost and sustainability. Developing novel organic active material for flow battery electrolytes typically entails molecular engineering toward desired properties, necessitating organic synthesis. In a research laboratory setting, the synthesis of specifically designed organic molecules featuring targeted functional groups is time and resources intensive. In the past, synthesizing materials required for battery testing has often required gram-scale production, presenting considerable constraints on the pace of novel organic material discovery. In this report, we introduce a miniaturized cell design that mandates only milligram-scale material synthesis while yielding testing outcomes equivalent or superior to those reported with other commercially available or homemade flow cells in the literature. The test results under various pH conditions validate the scale-down strategy to accelerate the flow battery material discovery and development using the newly designed mini cell. This approach offers researchers an efficient means to notably reduce the time and resources required to develop novel materials for flow batteries.

25 ENERGY STORAGE↗
DOE OSTI2024

Methods and system for rebalancing electrolytes in a redox flow battery system

A method of rebalancing electrolytes in a redox flow battery system comprises directing hydrogen gas generated on the negative side of the redox flow battery system to a catalyst surface, and fluidly contacting the hydrogen gas with an electrolyte comprising a metal ion at the catalyst surface, wherein the metal ion is chemically reduced by the hydrogen gas at the catalyst surface, and a state of charge of the electrolyte and pH of the electrolyte remain substantially balanced.

Song, Yang↗