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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 289 records · Page 16
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DOE OSTI2026

Mixed-anion electrolytes: from bulk speciation to interfacial dynamics in divalent metal electrodeposition

Mixing anions is emerging as a promising strategy for multivalent electrolyte design, allowing for adjustment of the solvation structure of bulk cations and enhancing the efficiency of electrochemical processes (e.g. metal deposition for batteries and catalysis). Further progress in electrolyte development requires a fundamental understanding of how tailored electrolyte speciation in mixed anion systems can modify the dynamic electrochemical interface during metal cycling. In this study, we present an anode-focused mechanistic study of exemplar Mg electrolytes containing three different secondary anions, correlating electrochemical behavior with bulk speciation and operando interfacial dynamics. Electrospray Ionization-Mass Spectrometry (ESI-MS) results reveal a general trend of forming mixed anion contact ion pairs (CIPs) across various anions, with the extent of ion pairing influenced by the association strength of the secondary anion. Operando multiharmonic electrochemical quartz crystal microbalance with dissipation (EQCM-D) reveals how these bulk species influence interfacial mass uptake, viscoelasticity, and solvent-coupled hydrodynamic behavior during deposition and stripping. The results indicate that Mg-containing ion pairs and solvated complexes shape adsorption, nucleation, and deposit growth, leading to distinct anion-dependent interphases ranging from more permeable, solvent-coupled layers to relatively compact and rigid deposits. This work establishes a quantitative link between bulk speciation and interfacial dynamics in divalent metal electrodeposition and provides mechanistic guidance for electrolyte design.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Pathways Toward High-energy Li-sulfur Batteries, Identified via Multi-reaction Chemical Modeling

Here we present a 1D model of a Li-Sulfur battery with physically derived geometric parameters and thermodynamically consistent electrochemical kinetics. The approach enables straightforward comparison of proposed Li-S mechanisms and provides insights into the influence of polysulfide intermediates on battery discharge. Comparing predictions from multiple mechanisms demonstrates the need for both lithiated and non-lithiated polysulfide species, and highlights the challenge of developing parameter estimates for complex electrochemical mechanisms. The model is also used to explore cathode design strategies. Discharge performance and polysulfide concentrations for electrolyte/sulfur ratios in the range 2–4 μ L mg −1 identifies trade-offs that limit battery energy and power density, and highlights the risk of polysulfide precipitation. New cathode and electrolyte approaches must limit polysulfide concentrations in the electrolyte, both to unlock better rate capabilities in Li-S technology and to prevent capacity fade due to polysulfide precipitation.

25 ENERGY STORAGE↗
DOE OSTI2023

Scalable Metal Phosphides as a Dual-Function Catalyst and Lithium–Metal Stabilizer for Lithium–Sulfur Batteries

Although lithium-sulfur batteries are a promising approach for achieving high energy density, their commercial viability is limited by poor sulfur redox kinetics, polysulfide shuttling, and lithium metal instability. To resolve these issues concurrently, we utilize titanium phosphides (TiP x ) as dual-function materials to catalyze the sulfur redox kinetics at the cathode and stabilize the lithium metal at the anode. Importantly, these phosphides are synthesized via a facile, highly scalable one-step mechanochemical ball-milling process that does not generate toxic phosphine gas as a byproduct, making it more viable compared to traditional synthesis routes. At the cathode, we find that higher phosphorus contents in the phosphide as in TiP 2 leads to superior redox kinetics and reduced polysulfide shuttling due to improved polysulfide adsorption ability. Meanwhile, at the anode, TiP 2 acts as a lithiophilic seed in a 3-dimensional carbonaceous host that can be lithiated to form a Li-TiP 2 /C composite. This composite alleviates the volume changes of lithium metal while utilizing TiP 2 to form a more favorable solid-electrolyte interface (SEI). Full coin cells employing TiP 2 in the cathode and anode were assembled with a sulfur loading of 4 mg cm -2 and a negative to positive capacity (N/P) ratio of 6. After 50 cycles, the TiP 2 full cells retain a higher capacity of 643 mA h g -1 compared to 422 mA h g -1 for the conventional cell, despite the higher N/P ratio of 12 for the conventional cell. Altogether, we showcase the viability of employing metal phosphides as catalysts in practical lithium-sulfur batteries.

25 ENERGY STORAGE↗
DOE OSTI2026

Quantitative Analysis and Prediction of Thermal Runaway Metrics of High-Nickel Oxide Cathodes by Machine Learning Models

The pursuit of higher energy density in lithium-ion batteries has made high-nickel (Ni) layered oxides leading cathode candidates for next-generation electric vehicles. However, their poor thermal stability, particularly at Ni contents ≥ 90%, increases the risk of cathode-initiated thermal runaway. Furthermore, we present a data-driven framework combining linear and nonlinear machine learning models to predict key thermal runaway descriptors from a high-throughput differential scanning calorimetry database. With cathode composition and state of charge (SOC) as input features, the ensemble model accurately predicts peak temperature, heat release, and peak heat flow. SHAP analysis identifies Ni content and SOC as the dominant factors controlling thermal runaway temperature, while SOC primarily governs heat release and peak heat flow. Al, Mg, and Mn improve thermal stability by strengthening metal–oxygen bonding and delaying structural transformation, whereas B mainly reduces heat release through surface passivation. Validation with a new cathode composition confirms accurate prediction of SOC-dependent thermal runaway behavior and critical SOC.

25 ENERGY STORAGE↗
DOE OSTI2024

Transforming nanoscale VO 2 (B) into a scalable sodium-ion electrode

The intermittent nature of renewable energies requires highly reliable grid-level energy storage approaches. A critical consideration in developing this technology is the areal capacity which determines battery performance and influences the cost of battery technology. Of related importance is finding new ways of developing scalable electrodes. In recent years, three-dimensional (3D) printing of conductive scaffolds has emerged as an alternative to overcome the scalability limitations of commercial tape cast electrodes. The research carried out in the current study demonstrates a successful scalability pathway for nanoscale VO 2 (B), a desirable cathode for sodium-ion batteries which has a nano-flower morphology with a crystallite size < 20 nm. By electrodepositing VO 2 (B) onto a graphene aerogel scaffold, we were able to achieve mass loading of over 100 mg·cm −2 and still possess an areal capacity of 10 mAh·cm −2 at a current density of 5 mA·cm −2 . Moreover, after 1000 cycles, these electrodes retained 75% to 80% of their initial capacity. Even at high loading levels, the electrodeposited VO 2 (B) exhibits pseudocapacitive material signatures such as a box-like voltammetry response, linear galvanostatic response, and no phase change upon lithiation. The scalability of the VO 2 (B) electrode is demonstrated in a series of experiments which show the areal capacity to scale upon increase in both mass loading and electrode thickness, with only small changes in specific capacity. Furthermore, this study establishes that nanoscale materials can be scaled up to achieve thick electrodes without compromising their electrochemical properties.

additive manufacturing↗
DOE OSTI2022

Development of high-energy non-aqueous lithium-sulfur batteries via redox-active interlayer strategy

Abstract Lithium-sulfur batteries have theoretical specific energy higher than state-of-the-art lithium-ion batteries. However, from a practical perspective, these batteries exhibit poor cycle life and low energy content owing to the polysulfides shuttling during cycling. To tackle these issues, researchers proposed the use of redox-inactive protective layers between the sulfur-containing cathode and lithium metal anode. However, these interlayers provide additional weight to the cell, thus, decreasing the practical specific energy. Here, we report the development and testing of redox-active interlayers consisting of sulfur-impregnated polar ordered mesoporous silica. Differently from redox-inactive interlayers, these redox-active interlayers enable the electrochemical reactivation of the soluble polysulfides, protect the lithium metal electrode from detrimental reactions via silica-polysulfide polar-polar interactions and increase the cell capacity. Indeed, when tested in a non-aqueous Li-S coin cell configuration, the use of the interlayer enables an initial discharge capacity of about 8.5 mAh cm −2 (for a total sulfur mass loading of 10 mg cm −2 ) and a discharge capacity retention of about 64 % after 700 cycles at 335 mA g −1 and 25 °C.

25 ENERGY STORAGE↗
DOE OSTI2022

Cosmogenic nuclide and solute flux data from central Cuban rivers emphasize the importance of both physical and chemical mass loss from tropical landscapes

We use 25 new measurements of in situ produced cosmogenic 26 Al and 10 Be in river sand, paired with estimates of dissolved load flux in river water, to characterize the processes and pace of landscape change in central Cuba. Long-term erosion rates inferred from 10 Be concentrations in quartz extracted from central Cuban river sand range from 3.4–189 Mg km –2 yr –1 (mean 59, median 45). Dissolved loads (10–176 Mg km –2 yr –1 ; mean 92, median 97), calculated from stream solute concentrations and modeled runoff, exceed measured cosmogenic- 10 Be-derived erosion rates in 18 of 23 basins. This disparity mandates that in this environment landscape-scale mass loss is not fully represented by the cosmogenic nuclide measurements. The 26 Al / 10 Be ratios are lower than expected for steadystate exposure or erosion in 16 of 24 samples. Depressed 26 Al/ 10 Be ratios occur in many of the basins that have the greatest disparity between dissolved loads (high) and erosion rates inferred from cosmogenic nuclide concentrations (low). Depressed 26 Al/ 10 Be ratios are consistent with the presence of a deep, mixed, regolith layer providing extended storage times on slopes and/or burial and extended storage during fluvial transport. River water chemical analyses indicate that many basins with lower 26 Al/ 10 Be ratios and high 10 Be concentrations are underlain at least in part by evaporitic rocks that rapidly dissolve. Our data show that when assessing mass loss in humid tropical landscapes, accounting for the contribution of rock dissolution at depth is particularly important. In such warm, wet climates, mineral dissolution can occur many meters below the surface, beyond the penetration depth of most cosmic rays and thus the production of most cosmogenic nuclides. Our data suggest the importance of estimating solute fluxes and measuring paired cosmogenic nuclides to better understand the processes and rates of mass transfer at a basin scale.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2026

Metal–Organic Framework-derived Atomic Metal Sites Promoting Sulfur Cathode for All-Solid-State Lithium–Sulfur Batteries

All-solid-state lithium–sulfur batteries (ASSLSBs) offer high energy density and intrinsic safety; however, they still face major challenges, including sluggish redox kinetics and poor sulfur utilization. Incorporating conductive materials into sulfur cathodes is an effective strategy to mitigate these limitations. Here, a highly conductive cobalt–nitrogen–doped carbon (Co–NC) derived from a metal–organic framework (MOF) is introduced to accelerate charge transfer and promote reversible sulfur conversion. Co−NC provides atomically dispersed Co–N sites and conductive carbon pathways that correlate with improved charge transfer, sulfur utilization, and rate capability. Co–NC@S cathode delivers 1499 mAh g–1 at C/20 with a high sulfur loading (5 mg cm–2) and retains 1292 mAh g–1 after five cycles (vs 443 mAh g–1 without Co–NC). Moreover, Co–NC derived ASSLSB achieves 903 mAh g–1 at 5C at 60 °C. This work provides a practical and effective approach to develop high energy, high-rate ASSLSBs.

25 ENERGY STORAGE↗
DOE OSTI2024

Design principles of heterointerfacial redox chemistry for highly reversible lithium metal anode

High electrochemical reversibility is required for the application of high-energy-density lithium (Li) metal batteries; however, inactive Li formation and SEI (solid electrolyte interface)-instability-induced electrolyte consumption cause low Coulombic efficiency (CE). The prior interfacial chemical designs in terms of alloying kinetics have been used to enhance the CE of Li metal anode; however, the role of its redox chemistry at heterointerfaces remains a mystery. Herein, the relationship between heterointerfacial redox chemistry and electrochemical transformation reversibility is investigated. It is demonstrated that the lower redox potential at heterointerface contributes to higher CE, and this enhancement in CE is primarily due to the regulation of redox chemistry to Li deposition behavior rather than the formation of SEI films. Low oxidation potential facilitates the formation of the surface with the highly electrochemical binding feature after Li stripping, and low reduction potential can maintain binding ability well during subsequent Li plating, both of which homogenize Li deposition and thus optimize CE. In particular, Mg hetero-metal with ultra-low redox potential enables Li metal anode with significantly improved CE (99.6%) and stable cycle life for 700 cycles at 3.0 mA cm -2 . This work provides insight into the heterointerfacial design principle of next-generation negative electrodes for highly reversible metal batteries.

25 ENERGY STORAGE↗
DOE OSTI2024

Entropy-Stabilized Multication Fluorides as a Conversion-Type Cathode for Li-Ion Batteries–Impact of Element Selection

Metal fluorides (e.g., FeF 2 and FeF 3 ) have received attention as conversion-type cathode materials for Li-ion batteries due to their higher theoretical capacity compared to that of common intercalation materials. However, their practical use has been hindered by low round-trip efficiency, voltage hysteresis, and capacity fading. Cation substitution has been proposed to address these challenges, and recent advancements in battery performance involve the introduction of entropy stabilization in an attempt to facilitate reversible conversion reactions by increasing configurational entropy. Building on this concept, high entropy fluorides with five cations were synthesized by using a simple mechanochemical route. In order to examine the impact of element selection, Co 0.2 Cu 0.2 Ni 0.2 Zn 0.2 Fe 0.2 F 2 (HEF-Fe) was compared with Co 0.2 Cu 0.2 Ni 0.2 Zn 0.2 Mg 0.2 F 2 (HEF-Mg), replacing electrochemically inactive Mg with Fe as an active participant in the conversion reaction. Combining electrochemical measurements with first-principles calculations, high-resolution electron microscopy, and synchrotron X-ray analysis, HEFs’ battery performances and conversion reaction mechanisms were investigated in detail. The results highlighted that replacement of Mg with Fe was beneficial, with enhanced capacity, rate capability, and surface stability. In addition, it was found that HEF-Fe showed similar cycle stability without an electrochemically inactive element. In conclusion, these findings provide valuable insights for the design of high entropy multielement fluorides for improved Li-ion battery performance.

25 ENERGY STORAGE↗
DOE OSTI2022

Integrated reactor architecture of conductive network and catalytic nodes to accelerate polysulfide conversion for durable and high-loading Li-S batteries

The development of carbon-based heterogeneous framework host with synergistic catalytic and conductive effects for sulfur cathode is a promising strategy to realize high performance lithium sulfur batteries (LSBs). Here, an integrated reactor architecture with defective carbon nodes (IRA-DC) is designed for serving as high-loading (92.4 wt%) sulfur host. The hierarchical porous IRA-DC consists of untangled conductive carbon nanotube network and Co/N co-doped catalytic nodes with high dispersity. Therein the optimization of electric field distribution and homogenization of adsorption-catalysis sites offer the multi-electron conversion reaction of polysulfides with excellent kinetics and stability. The resultant IRA-DC/S cathode enables a high areal capacity of 8.86 mAh cm -2 under ultra-high sulfur loading (13.1 mg cm -2 ) and lean electrolyte (8 μL mg sulfur -1 ). It also displays a long-term cycling performance (1200 cycles at 1 C) and ultrahigh rate performance up to 20 C (with a capacity of 473.6 mAh g -1 ). In conclusion, this work provides an electrode building strategy by optimizing the environments of heterogeneous electrocatalysis and micro electric field to activate the polysulfide conversion efficiency and utilization of high-loading sulfur in monolithic sulfur-carbon cathodes.

25 ENERGY STORAGE↗
DOE OSTI2021

Investigation of Membrane Chemical Degradation as a Function of Catalyst Platinum Loading

Membrane chemical degradation is one of many factors that can impact fuel cell durability. Additionally, the fuel cell’s lifetime heavily depends on the membrane and its ability to maintain chemical and mechanical integrity. Previous studies indicate that chemical degradation is due to the formation of hydroxyl radicals that attack the polymer structure resulting in membrane thinning, pinhole formation, and the release of fluoride and sulfate ions. Membrane durability was investigated using ultra-low Pt electrode loadings (≤ 0.1 mg Pt cm -2 ). Accelerated stress testing (US-DOE protocols) demonstrated that the degradation rate was found to increase with higher Pt loadings. This is most likely due to more heterogeneous sites for radical formation due to hydrogen crossover to the cathode. We also explored membrane degradation rates while varying catalyst layer thickness, ionomer to carbon ratio, and types of carbon support. All of the aforementioned variables impact the membrane degradation rates.

25 ENERGY STORAGE↗
DOE OSTI2023

A global meta‐analysis of cover crop response on soil carbon storage within a corn production system

Abstract By influencing soil organic carbon (SOC), cover crops play a key role in shaping soil health and hence the system's long‐term sustainability. However, the magnitude by which cover crops impacts SOC depends on multiple factors, including soil type, climate, crop rotation, tillage type, cover crop growth, and years under management. To elucidate how these multiple factors influence the relative impact of cover crops on SOC, we conducted a meta‐analysis on the impacts of cover crops within rotations that included corn ( Zea mays L.) on SOC accumulation. Information on climatic conditions, soil characteristics, management, and cover crop performance was extracted, resulting in 198 paired comparisons from 61 peer‐reviewed studies. Over the course of each study, cover crops on average increased SOC by 7.3% (95% CI, 4.9%–9.6%). Furthermore, the impact of cover crop–induced increases in percent change SOC was evaluated across soil textures, cover crop types, crop rotations, biomass amounts, cover crop durations, tillage practices, and climatic zones. Our results suggest that current cover crop–based corn production systems are sequestering 5.5 million Mg of SOC per year in the United States and have the potential to sequester 175 million Mg SOC per year globally. These findings can be used to improve carbon footprint calculations and develop science‐based policy recommendations. Taken altogether, cover cropping is a promising strategy to sequester atmospheric C and hence make corn production systems more resilient to changing climates.

60 APPLIED LIFE SCIENCES↗
DOE OSTI2022

Structure/Interface Coupling Effect for High-Voltage LiCoO 2 Cathodes

LiCoO 2 (LCO) is widely applied in today's rechargeable battery markets for consumer electronic devices. However, LCO operations at high voltage are hindered by accelerated structure degradation and electrode/electrolyte interface decomposition. To overcome these challenges, co-modified LCO (defined as CB-Mg-LCO) that couples pillar structures with interface shielding are successfully synthesized for achieving high-energy-density and structurally stable cathode material. Benefitting from the "Mg-pillar" effect, irreversible phase transitions are significantly suppressed and highly reversible Li + shuttling is enabled. Interestingly, bonding effects between the interfacial lattice oxygen of CB-Mg-LCO and amorphous Co x B y coating layer are found to elevate the formation energy of oxygen vacancies, thereby considerably mitigating lattice oxygen loss and inhibiting irreversible phase transformation. Meanwhile, interface shielding effects are also beneficial for mitigating parasitic electrode/electrolyte reactions, subsequent Co dissolution, and ultimately enable a robust electrode/electrolyte interface. As a result, the as-designed CB-Mg-LCO cathode achieves a high capacity and excellent cycle stability with 94.6% capacity retention at an extremely high cut-off voltage of 4.6 V. We report these findings provide new insights for cathode material modification methods, which serves to guide future cathode material design.

25 ENERGY STORAGE↗
DOE OSTI2025

Reduced Erosion Augments Soil Carbon Storage Under Cover Crops

ABSTRACT Cover crops, a promising strategy to increase soil organic carbon (SOC) storage in croplands and mitigate climate change, have typically been shown to benefit soil carbon (C) storage from increased plant C inputs. However, input‐driven C benefits may be augmented by the reduction of C outputs induced by cover crops, a process that has been tested by individual studies but has not yet been synthesized. Here we quantified the impact of cover crops on organic C loss via soil erosion (SOC erosion) and revealed the geographical variability at the global scale. We analyzed the field data from 152 paired control and cover crop treatments from 57 published studies worldwide using meta‐analysis and machine learning. The meta‐analysis results showed that cover crops widely reduced SOC erosion by an average of 68% on an annual basis, while they increased SOC stock by 14% (0–15 cm). The absolute SOC erosion reduction ranged from 0 to 18.0 Mg C −1 ha −1 year −1 and showed no correlation with the SOC stock change that varied from −8.07 to 22.6 Mg C −1 ha −1 year −1 at 0–15 cm depth, indicating the latter more likely related to plant C inputs. The magnitude of SOC erosion reduction was dominantly determined by topographic slope. The global map generated by machine learning showed the relative effectiveness of SOC erosion reduction mainly occurred in temperate regions, including central Europe, central‐east China, and Southern South America. Our results highlight that cover crop‐induced erosion reduction can augment SOC stock to provide additive C benefits, especially in sloping and temperate croplands, for mitigating climate change.

Huang, Wenjuan [Department of Ecology, Evolution, ↗
DOE OSTI2022

Rationalizing nitrogen-doped secondary carbon particles for practical lithium-sulfur batteries

Nanostructured carbon host materials are widely used to improve both sulfur utilization rate and reaction kinetics in lithium-sulfur (Li-S) batteries. However, high complexity/cost of materials synthesis and difficulty in processing nano-materials into high-mass-loading electrodes are still significant barriers to the development of low-cost and high-energy Li-S batteries. In this study, we reported a generic and scalable synthesis approach to prepare nitrogen-doped secondary carbon particles. By using nitrogen-containing precursor as an integration reagent, the nanosized Ketjen Black particles were integrated into micron-size secondary ones and nitrogen-doped (NKB) simultaneously through a one-step heat treatment. With NKB as an example material, the effects of particle integration degree on the secondary particles’ structures, pore volume and connectivity, sulfur loading capability, and cell performance were studied and discussed. At an optimal integration condition, the NKB particles had significantly improved particle dimensions with well-maintained high specific surface area and pore volume. Here, contributed by the micron size and high pore volume, the NKB/S were successfully used for high-sulfur-loading cathodes (4–7 mg s /cm -2 ) and were able to deliver a specific capacity of ~1100 mAh g -1 at a low-porosity (50%) and lean-electrolyte conditions (E/S =4 µL/mg -1 ). Feasibility of the materials for practical use was validated through scaling up synthesis (40 g/batch), large-area electrode coating, and practical pouch cell (1.6 Ah) assembly and test.

25 ENERGY STORAGE↗
DOE OSTI2024

A weakly ion pairing electrolyte designed for high voltage magnesium batteries

High-voltage rechargeable magnesium batteries (RMBs) are potential alternatives to lithium-ion batteries owing to the low cost and high abundance of magnesium. However, the parasitic reactions of the latter with many electrolytes greatly hinders the stability and kinetics of Mg plating/stripping. Here we report a new and easily accessible solvent-designed electrolyte, which effectively solves the difficulty of ion pair dissociation and facilitates fast nanoscale Mg nucleation/growth using simple Mg(TFSI)2 as the salt, enabling a facile interfacial charge transfer process. Dendrite-free Mg plating/stripping is maintained for over 7000 hours (∼10 months) at a practical areal capacity of 2 mA h cm−2. The high-voltage stability of these electrolytes is demonstrated by benchmarking with polyaniline||Mg full cells with an operating voltage up to 3.5 V that exhibit stable cycling at a 2C rate with 99% coulombic efficiency after 400 cycles. This work opens up new frontiers in coupling low-cost electrolytes with next-generation high-voltage cathode materials for fast-charging RMBs with long life and high energy densities.

Li, Chang↗