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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 307 records · Page 17
All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

Localized High Concentration Electrolyte and Its Effects on Polysulfide Structure in Solution

Lithium–sulfur batteries (LiSB) are a promising next-generation lithium energy storage technology that offers a multifold improvement over the traditional lithium-ion battery. However, the LiSB still faces the unresolved issue of the polysulfide shuttle effect. This phenomenon arises from the dissolution of sulfur intermediate reduction products into the electrolyte, which then causes a cascade of issues throughout the battery. Many mitigation strategies have been proposed to counteract this effect including the use of novel electrolyte compositions. Recently, there has been increased focus on the use of hydrofluorinated ethers as a major constituent of an electrolyte for lithium batteries. Previous studies have reported that the presence of these species create localized high concentration electrolytes (LHCE) which can have many advantages resulting in improved battery performance. Here, we report on how the inclusion of a hydrofluorinated ether BTFE (bis(2,2,2-trifluoroethyl) ether) modifies the general properties of a LiSB electrolyte and the structure of dissolved polysulfide species in the electrolyte. Here, we found that the inclusion of BTFE does not modify the primary solvation structure of Li + directly but actively participates in secondary solvation shells. With a high concentration of BTFE, the LHCE formation is observed by the presence of clusters of non-BTFE molecules. The structure of polysulfide species in solution was modified by the BTFE in the same way. Much of the primary solvation structure was kept, but the presence of BTFE increased polysulfide–polysulfide clustering. These results indicate that the polysulfide solubility will be limited due to the promotion of clustering.

25 ENERGY STORAGE↗
DOE OSTI2025

Electronic and Geometric Contributors to Hydrogen Binding in Uranium Oxide Grain Boundaries

Hydrogen induced corrosion of uranium, which leads to the formation of toxic and pyrophoric UH 3 , raises significant safety concerns for long-term storage of nuclear materials. Previous work suggests hydrogen diffuses through the grain boundaries (GBs) of the passivating oxide layer to initiate hydriding reactions. However, the atomistic mechanisms underlying this phenomenon and the structural factors that control its initiation are not well understood. To address this knowledge gap, here we use a high-throughput density functional theory (DFT) workflow to investigate the adsorption of H and H 2 in the defective bulk UO 2 . Specifically, we have exhaustively investigated the adsorption of H (107 sites) and H 2 (26 sites) in three different coincident site lattice (CSL) GBs: Σ3, Σ5, and Σ9. Compared to the binding energies in pristine UO 2 , we observe significantly stronger hydrogen adsorption at these GB sites. Interestingly, we find that the trends in H and H 2 adsorption vary considerably across the three GB models. In particular, while a small number of sites in Σ5 and Σ9 show exothermic adsorption of H and H 2 , respectively, no such sites are found in Σ3. These results provide fundamental atomistic insights that could guide the development of future corrosion mitigation strategies for the storage of nuclear materials.

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

Metal Oxide-Induced Instability and Its Mitigation in Halide Perovskite Solar Cells

Halide perovskite solar cells (PSCs) have emerged as a promising photovoltaic technology for sustainable energy solutions due to their impressive power conversion efficiency and a path to be manufactured by low-cost, high-throughput methods. To reach PSCs’ full potential for practical implementation, it is crucial to solving the issues related to its long-term operational stability. Furthermore, given that PSCs consist of many layers of dissimilar materials which form multiple internal interfaces, it is prudent to examine whether there exist interfacial interactions, most importantly between transport layers and perovskite absorbers, that can trigger device performance and instability. In this perspective, we bring to the attention of the PSC research community the lesser-known interfacial degradation of halide perovskites promoted by contact with metal oxide transport layers and highlight the deleterious effects on the PSCs’ performance and stability. We also discuss various mitigation strategies that have shown promises to achieve high-performing and stable PSCs.

14 SOLAR ENERGY↗
DOE OSTI2024

Hybrid Density Functional Theory Comparison of Oxygen Release and Solvent Decomposition Kinetics on Li x NiO 2 Surfaces

High-nickel-content layered oxides are among the most promising electric vehicle battery cathode materials. However, their interfacial reactivity with electrolytes and tendency toward oxygen release (possibly yielding reactive 1 O 2 ) remain degradation concerns. Elucidating the most relevant (i.e., fastest) interfacial degradation mechanism will facilitate future mitigation strategies. We apply screened hybrid density functional (HSE06) calculations to compare the reaction kinetics of Li x NiO 2 surfaces with ethylene carbonate (EC) with those of O 2 release. Further, on both the (001) and (104) facets, EC oxidative decomposition exhibits lower activation energies than O 2 release. Our calculations, coupled with previously computed liquid-phase reaction rates of 1 O 2 with EC, strongly question the role of “reactive 1 O 2 ” species in electrolyte oxidative degradation. The possible role of other oxygen species is discussed. To deal with the challenges of modeling Li x NiO 2 surface reactivity, we emphasize a “local structure” approach instead of pursuing the global energy minimum.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Band-edge Engineering to Eliminate Radiation-Induced Defect States in Perovskite Scintillators

Under radiative environments such as extended hard X- or γ-rays, degradation of scintillation performance is often due to irradiation-induced defects. To overcome the effect of deleterious defects, novel design mitigation strategies are needed to identify and design more resilient materials. The potential for band-edge engineering to eliminate the effect of radiation-induced defect states in rare-earth-doped perovskite scintillators is explored, taking Ce 3+ -doped LuAlO 3 as a model material system, using density functional theory (DFT)-based DFT + U and hybrid Heyd–Scuseria–Ernzerhof (HSE) calculations. Furthermore, from spin-polarized hybrid HSE calculations, the Ce 3+ activator ground-state 4f position is determined to be 2.81 eV above the valence band maximum in LuAlO 3 . Except for the oxygen vacancies which have a deep level inside the band gap, all other radiation-induced defects in LuAlO 3 have shallow defect states or are outside the band gap, that is, relatively far away from either the 5d 1 or the 4f Ce 3+ levels. Finally, we examine the role of Ga doping at the Al site and found that LuGaO 3 has a band gap that is more than 2 eV smaller than that of LuAlO 3 . Specifically, the lowered conduction band edge envelopes the defect gap states, eliminating their potential impact on scintillation performance and providing direct theoretical evidence for how band-edge engineering could be applied to rare-earth-doped perovskite scintillators.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Critical Contribution of Imbalanced Charge Loss to Performance Deterioration of Si-Based Lithium-Ion Cells during Calendar Aging

Increasing the energy density of lithium-ion batteries, and thereby reducing costs, is a major target for industry and academic research. One of the best opportunities is to replace the traditional graphite anode with a high-capacity anode material, such as silicon. However, Si-based lithium-ion batteries have been widely reported to suffer from a limited calendar life for automobile applications. Heretofore, there lacks a fundamental understanding of calendar aging for rationally developing mitigation strategies. Both open-circuit voltage and voltage-hold aging protocols were utilized to characterize the aging behavior of Si-based cells. Particularly, a high-precision leakage current measurement was applied to quantitatively measure the rate of parasitic reactions at the electrode/electrolyte interface. The rate of parasitic reactions at the Si anode was found 5 times and 15 times faster than those of LiNi 0.8 Mn 0.1 Co 0.1 O 2 and LiFePO 4 cathodes, respectively. Here, the imbalanced charge loss from parasitic reactions plays a critical role in exacerbating performance deterioration. In addition, a linear relationship between capacity loss and charge consumption from parasitic reactions provides fundamental support to assess calendar life through voltage-hold tests. These new findings imply that longer calendar life can be achieved by suppressing parasitic reactions at the Si anode to balance charge consumption during calendar aging.

25 ENERGY STORAGE↗
DOE OSTI2025

Size-Selective Nanoporous Atomically Thin Graphene Separators for Lithium–Sulfur Batteries

Lithium–sulfur batteries (LSBs) are extensively researched for their high energy densities but are hindered by the lithium polysulfide (LiPS) shuttling effect, which results in poor cyclability. A popular mitigation strategy is separator modification, where a LiPS trapping material is slurry-coated onto a conventional microporous polypropylene (PP) separator. This additional mass and volume unfortunately compromise the overall energy density of the LSB. This study aims to take a separator modification approach that avoids this issue. Nanoporous atomically thin membranes (NATMs) made of graphene are gaining attention for their scalable synthesis, tunable pore size, and negligible pore length. Herein, we apply a well-characterized graphene NATM for reasons similar to those of a size-selective interlayer in LSBs. The tailored pore size of ∼0.7–1.0 nm and atomic thinness facilitate the passage of Li + (solvated ionic diameters ∼0.54–1.26 nm) and blockage of larger LiPS (solvated ionic diameters ∼0.81–1.69 nm) without adding significant impedances or mass. The sulfur confinement is confirmed through scanning electron microscopy and energy-dispersive X-ray spectroscopy elemental analysis of the Li anode. An LSB with a NATM@PP separator shows virtually no capacity loss over 150 cycles, demonstrating efficacy of size-selective molecular sieving using NATMs in LSBs.

battery separator↗
DOE OSTI2022

Nanoengineering Porous Silica for Thermal Management

Thermal insulation of solid materials originates from the nanoscale porous architectures to regulate thermal management in energy-critical applications from energy-efficient buildings to heat-sensitive energy devices. Here, we show nanoengineering of porous silica materials to control the architecture transition from mesoporous to nanocage networks. A low thermal conductivity of such a porous silica network is achieved at 0.018 W/(m K) while exhibiting a porosity of 92.05%, specific surface area of 504 m 2 /g, and pore volume of 2.37 cm 3 /g after ambient pressure drying. Meanwhile, the crosslinking of the porous silica and ceramic fiber frameworks show a tensile Young’s modulus of 2.8 MPa while maintaining high thermal insulation, which provides an effective thermal runway mitigation strategy for rechargeable lithium-ion batteries. Furthermore, the nanoengineering strategy reported here would shed light on achieving superthermal insulation of nanostructures for energy-critical applications.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Role of Polymer Architecture in CO 2 Capture from Air Using Supported Poly(alkylenimine)s: Linear vs Branched Polymers

Direct air capture (DAC) of CO 2 coupled with geologic storage is a promising climate change mitigation strategy, with some applications employing amines supported on porous solids as CO 2 sorbents. While branched poly(ethylenimine) (PEI) is the standard benchmark amine material, it suffers from limited oxidative stability. Poly(propylenimine) (PPI), as an alternative, has previously demonstrated improved resistance to degradation under harsh oxidative conditions. Linear and branched PEI are commercially available, though at different molecular weights, while PPI is not commercially available. For this reason, a comparative study of all four polymers (linear PEI, branched PEI, linear PPI, branched PPI) has not been reported for DAC. In this study, we synthesize and compare low-molecular-weight (∼800 g/mol) linear (L) and branched (B) PEI and PPI supported on a model support, SBA-15 silica. These materials are evaluated for CO 2 adsorption under dry, DAC-relevant conditions (400 ppm of CO 2 , 30 °C). LPPI exhibited the highest amine efficiency at all loadings, reaching a maximum of 0.14 mmol CO 2 /mmol N, outperforming BPEI, while LPEI consistently showed the lowest uptake capacity. Temperature-programmed desorption reveals that the structure of the amine polymer impacts the CO 2 binding strength, with branched polymers displaying higher desorption energies of 102−111 kJ/mol. In situ infrared spectroscopy experiments show that all sorbents preferentially capture CO 2 as ammonium carbamate. Isobaric CO 2 uptake studies further underscore the influence of polymer mobility and support pore crowding on performance, while demonstrating the sorbents’ performance at elevated temperatures and CO 2 concentrations. All materials demonstrated good stability over 25 adsorption−desorption cycles using thermal regeneration in an inert gas purge, with only BPPI displaying a 10−11% decrease in capacity/amine efficiency during cycling, possibly due to the loss of low molecular weight, oligomeric amines. This is the first side-by-side comparison of the CO 2 sorption properties of linear and branched PEI and PPI with similar molecular weights. These findings highlight the significant role of polymer architecture in CO 2 capture efficiency and inform future designs of durable, high-performance DAC sorbents.

adsorbents↗
DOE OSTI2024

Controlling Product Selectivity in Photochemical CO 2 Reduction with the Redox Potential of the Photosensitizer

The ability to selectively reduce CO 2 to a particular product or mixture of products is expected to play a key role in mitigation strategies aiming to alleviate the devastating impact of this greenhouse gas in our climate and oceans. Among those, the production of liquid solar fuels from CO 2 and H 2 O will likely need cascade strategies involving multiple catalysts carrying out different functions. This will require that the catalysts doing the initial CO 2 reduction steps deliver the right product or products to downstream catalysts. CO, H 2 and formate are the most common products in CO 2 reduction by molecular catalysts. Here, in this work, we demonstrate control over the selectivity of C 1 products in photochemical CO 2 reduction with the same catalyst, simply by changing the redox potential of the photosensitizer and/or the water concentration. Turnover numbers for CO generation with one of the photosensitizers under anhydrous conditions reached 85,000, one of the largest values reported to date. A combination of experimental results and DFT calculations show that control of the selectivity is achieved, in part, due to the interplay between regimes under kinetic or thermodynamic control. These regimes are largely dictated by the proton sources and the CO 2 reduction byproducts generated.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

From Micro-environments to Macroscopic Effects: How the Alkaline Hydrogen Evolution Reaction Drives Cu Cathodic Corrosion

Cathodic corrosion of copper (Cu) has posed a significant challenge for over a century, impeding various technological progresses such as electrochemical conversion of CO 2 (eCO 2 RR) into fuels and other value-added carbon products. Here, in this study, employing a combined Density Functional Theory (DFT) and kinetic Monte Carlo (kMC) simulation approach, we delve into the atomistic level mechanism driving this phenomenon in Cu. Our hypothesis posits the pivotal role of alkaline hydrogen evolution reaction (HER) in facilitating cathodic corrosion in Cu. We rigorously develop a pH-dependent hydroxide (OH) adsorption mechanism and calculate the equilibrium OH coverage (𝜃 OH ) at varying pH levels, the thermodynamic stability of subsurface oxygen (O sub ), as well as the Cu-vacancy mediated diffusion of subsurface oxygens (O sub ). Through comprehensive analysis, we establish correlation among various microenvironments, including oxygen diffusion in subsurface layers, pH-dependent OH adsorption, and Cu dissolution into the electrolyte as (Cu-OH) complexes. Furthermore, our investigation explores the correlation between surface coordination environment of active sites and cathodic corrosion of Cu. Finally, by integrating DFT-derived thermodynamic data into a kMC model, we successfully predict the formation of experimentally observed corrosion pits on Cu-surfaces. This combined approach not only advances our fundamental understanding of Cu cathodic corrosion but also offers insights crucial for developing effective corrosion mitigation strategies.

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

Mixing Matters: Nanoscale Heterogeneity and Stability in Metal Halide Perovskite Solar Cells

The structural stability of the metal halide perovskite (MHP) absorber material is crucial for the long-term solar cell stability in this thin-film photovoltaic technology. Here, we use mixed A-site FA0.83Cs0.17PbI3 to demonstrate that nanoscale compositional heterogeneity can serve as initiation sites for more macroscale, irreversible phase segregation, which causes device performance degradation. Probing compositional heterogeneity on length scales that has not been detected with conventional characterization techniques, we analyze the tetragonal to cubic phase transition behavior to indirectly determine the level of nanoscale compositional heterogeneity in the initial films. Further, we show that the thermal annealing conditions of the MHP layer during film processing influence the initial nanoscale compositional heterogeneity, and changing these processing conditions can be used to improve the device performance stability. The insights into structural degradation mechanisms initiated by nanoscale compositional heterogeneity and the proposed mitigation strategies will help guide the way toward long-term stable MHP solar cells.

14 SOLAR ENERGY↗
DOE OSTI2024

Ramifications of Ion Migration in 2D Lead Halide Perovskites

Lower dimensional or 2D halide perovskites with their versatile structural and functional properties, are known to improve the performance and room temperature stability of perovskite solar cells. One would expect 2D perovskites to be more resistant to ion migration compared to their 3D counterparts because of the presence of bulky organic cations. However, recent findings show ion migration indeed is prevalent in 2D halide perovskites similar to 3D perovskites. Halide ion migration in 2D perovskites manifests itself as halide ion segregation under photoirradiation as well as in halide exchange between physically paired films of 2D perovskites with different halide ions. Besides halide ion migration, cation migration of spacer cations and A-site cation is also seen when 2D/3D perovskite films are subjected to light and thermal stress. It is important to recognize the importance of ion migration while incorporating 2D perovskites in solar cells and other optoelectronic devices as it can be detrimental for achieving streamlined performance and long-term stability Furthermore, this perspective discusses recent reports on ion migration in 2D and in 2D/3D halide perovskite films under the operational conditions (at elevated temperature and given in-built bias) and presents a few mitigating strategies.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2026

Quantification of Shallow Defect Suppression in Aminosilane-Passivated Lead Halide Perovskites via Optical and Electrochemical Methods

We combine fluence-dependent photoluminescence (PL) and electrochemical characterization to estimate defect-dependent trapping rates, energetic distributions, and densities of defects, in lead halide perovskite films Cs 0.1 FA 0.9 PbI 3 and Cs 0.17 FA 0.83 Pb­(I 0.75 Br 0.25 ) 3 , before and after trap passivation with vapor-deposited (3-aminopropyl)­trimethoxysilane (APTMS). For both compositions, the PL studies show that energetically shallow subgap near-valence defect densities lead to bimolecular nonradiative recombination which is reduced by 92% after APTMS treatment. Electrochemical characterization of these same active layers shows for the first time that APTMS passivation impacts mainly on near-valence (mobile anionic) defects that decrease in density by 4 orders of magnitude, from 10 18 cm –3 to 10 14 cm –3 , as a result of silane modification. Here, the combination of PL and electrochemical characterization promises a unique approach to speciation and quantification of a broader distribution of trap states in perovskites and provides straightforward assessments of the efficacy of defect mitigation strategies.

Defects↗
DOE OSTI2026

Source-Resolved Inversion of Elemental Carbon Emissions in California Using Log-Space Bayesian Inference

Elemental carbon (EC), operationally quantified by thermal-optical analysis, is widely used as a proxy for black carbon (BC) relevant to short-term climate forcing and public health. Current EC emission inventories remain highly uncertain, with persistent discrepancies between bottom-up and top-down estimates. In this study, we develop a source-resolved, log-space Bayesian inversion framework applied to estimate California’s statewide EC emissions in 2019. By integrating surface EC measurements from the EPA’s Air Quality System network with high-resolution source contributions simulated by a chemical transport model, we identify a one-third underestimation in the existing statewide EC inventory, requiring an increase of the total from a prior of 8.58 [5.49–13.75] Gg year–1 to a posterior estimate of 12.78 [10.71–15.37] Gg year–1. This discrepancy is primarily driven by substantial underestimations in the power and industrial and off-road mobile sectors. Furthermore, population-weighted exposure analysis reveals a marked sectoral divergence between emission mass and health burden: off-road mobile sources dominate both emissions and exposure, accounting for 31% of statewide exposure, while residential wood combustion contributes 26% of total exposure despite comprising only 19% of total emissions, due to its source proximity to population. These findings underscore the need to update sector-specific EC speciation profiles and demonstrate that mitigation strategies targeting off-road mobile sources and residential wood combustion are critical for reducing EC-related health impacts in California.

Zhang, Jie↗
DOE OSTI2025

Antimicrobial Peptides Can Facilitate Whole Blood Safety from Bacteria: A Proof of Concept

With continuous improvements to blood donor deferrals and the availability of sensitive tests for donation screening for infectious agents, bacterial contamination of whole blood (WB) and blood components stored for transfusion is a rare event. Nonetheless, it still occurs and remains a transfusion-associated risk in terms of septic transfusion reactions (STRs) and transfusion-transmitted bacterial infections with morbidity and mortality outcomes. One of the risk mitigation strategies for bacterial contamination is to implement treatment with currently available proactive pathogen reduction technologies (PRTs) for these transfusion products. Here, as a proof of concept, we tested two recently developed unique cationic antimicrobial peptides (AMPs; D-CONGA and D-CONGA-Q7) for WB safety from bacterial contamination. In this study, WB was inoculated with Escherichia coli and Staphylococcus epidermidis and treated with the two peptides to evaluate their bactericidal efficacy. The results demonstrated that D-CONGA and D-CONGA-Q7 exhibit potent inhibitory activity against the bacteria with a minimal inhibitory concentration (MIC) range of 4–8 and 1–8 μM, respectively, depending on the bacterial species tested. Time-kill kinetics further confirmed that the peptides exhibit bactericidal efficacy at 8 μM by achieving a 5-log 10 reduction (99.999%) of the bacterial load in WB with a time-dependent killing profile. Furthermore, even at 20 μM, the AMPs did not negatively impact hemolysis or hemostatic properties. We have further demonstrated using a cationic exchange resin that the cationic AMPs can be separated and removed from WB after the peptide treatments. During 35-day WB storage at 2–8 °C, 4 μM D-CONGA-Q7 one-time treatment prevented S. epidermidis growth and preserved WB quality and integrity. Overall, the results described here provide the first proof of concept that certain AMPs, such as D-CONGA and D-CONGA-Q7, can facilitate WB safety from bacteria during storage.

60 APPLIED LIFE SCIENCES↗
DOE OSTI2026

Atomic-Scale Characterization and Electronic Properties of Gold-Capped Niobium Films for Superconducting Qubits

Niobium thin films are central to superconducting qubits, but their complex native oxides contribute significantly to microwave losses. A promising mitigation strategy is to suppress oxide formation using engineered thin-film encapsulation layers. Recent experiments have shown that ∼10 nm metallic overlayers on Nb capacitor films can improve the energy relaxation time T1 of transmon qubits. Here, we present a comparative study of Au-capped Nb films fabricated in situ by molecular beam epitaxy and ex situ by sequential deposition benchmarked against bare Nb films. Using complementary structural, chemical, and spectroscopic techniques, we correlate the interface quality with superconducting electronic properties of the Au surface. Low-temperature scanning tunneling spectroscopy (STS) provides spatially resolved quasiparticle density-of-states maps. While both Au-capped Nb samples exhibit large areas with uniform, fully gapped density of states, clear differences emerge between the two interfaces. Compared to in situ Nb-Au, ex situ Nb-Au exhibits a reduced induced superconducting gap, broadened coherence peak, and localized in-gap states, consistent with a residual NbxOy layer at the interface. Supported by complementary structural and chemical analyses, these findings demonstrate that STS directly links nanoscale superconducting properties to interface preparation, highlighting the importance of controlled in situ encapsulation for minimizing dissipation and improving quantum coherence.

Makita, Junki [MIT; Temple U.] (ORCID:000000026889↗
DOE OSTI2026

Self-Healing Lithium Dendrites through Spontaneous Passivating Layer Formation for Stable Solid-State Lithium–Metal Batteries

All-solid-state lithium–metal batteries have attracted significant attention, owing to their high energy density and superior safety. However, lithium–metal penetration through the solid electrolyte, leading to short-circuiting, remains a critical failure mode that demands comprehensive mitigation strategies. Most existing strategies are effective only prior to the initiation of lithium-dendrite formation and fail once dendrites begin to propagate through the electrolyte. In this study, we propose a self-healing mechanism in which the penetrated lithium reacts with a self-healing agent to form a passivating layer along the particle boundaries. Lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) was incorporated into a Li 6 PS 5 Cl solid electrolyte as the self-healing agent to suppress lithium-dendrite propagation even after dendrite formation initiated under high current densities. The self-healing induced by LiTFSI was verified through comprehensive experimental analyses and was further demonstrated in a full-cell configuration. Moreover, LiTFSI incorporation plays an important role in increasing the critical current density by reducing the overall electronic conductivity of the solid electrolyte and facilitating the formation of a robust LiF-containing solid-electrolyte interphase.

25 ENERGY STORAGE↗