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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 37 records · Page 2
All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

Preparing Li-garnet electrodes with engineered structures by phase inversion and high shear compaction processes

We report solid-state lithium batteries are promising for safety and energy density com-pared with traditional lithium-ion batteries. However, the large interfacial resistance between the electrode and electrolyte is a bottleneck to achieving high-performance solid-state batteries. Engineered electrode structures with a porous scaffold of the solid electrolyte material are promising to lower the interfacial resistance and provide a mechanical support for a thin solid electrolyte layer. In this work, two ceramic processing techniques are used to fabricate porous/dense bilayer architectures based on a Li 6.25 Al 0.25 La 3 Zr 2 O 12 (LLZO) Li-garnet material. Finger-like vertically aligned pores are created by the phase inversion (PI) process. A water bath presaturated with Li salt prevents Li loss during the PI solvent exchange step. Pore size and porosity can be optimized by adjusting the bath temperature. The high shear compaction process was used to prepare LLZO tapes with 40, 60, and 80 vol% poreformer. The porosity of the tapes after sintering is 39.5%, 58.4%, and 75.4%, respectively. Microtomography exhibits the porosity, pore shape, and pore distribution of the tapes. A typical cathode material LiNi 0.33 Mn 0.33 Co 0.33 O 2 (NMC) is filled into the pores via vacuum infiltration, and a dense cathode layer is formed within the garnet scaffold.

25 ENERGY STORAGE↗
DOE OSTI2021

Linking Perfluorosulfonic Acid Ionomer Chemistry and High-Current Density Performance in Fuel-Cell Electrodes

Transport phenomena are key in controlling the performance of electrochemical energy-conversion technologies and can be highly complex, involving multiple length scales and materials/phases. Material designs optimized for one reactant species transport however may inhibit other transport processes. We explore such trade-offs in the context of polymer-electrolyte fuel-cell electrodes, where ionomer thin films provide the necessary proton conductivity but retard oxygen transport to the Pt reaction site and cause interfacial resistance due to sulfonate/Pt interactions. We examine the electrode overall gas-transport resistance and its components as a function of ionomer content and chemistry. Low-equivalent-weight ionomers allow better dissolved-gas and proton transport due to greater water uptake and low crystallinity but also cause significant interfacial resistance due to the high density of sulfonic acid groups. These effects of equivalent weight are also observed via in situ ionic conductivity and CO displacement measurements. Of critical importance, the results are supported by ex situ ellipsometry and X-ray scattering of model thin-film systems, thereby providing direct linkages and applicability of model studies to probe complex heterogeneous structures. Structural and resultant performance changes in the electrode are shown to occur above a threshold sulfonic-group loading, highlighting the significance of ink-based interactions. Furthermore, our findings and methodologies are applicable to a variety of solid-state energy-conversion devices and material designs.

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

Dual material fused filament fabrication of composite core‐shell structures with improved impact resistance and interfacial adhesion

The mechanical performance of parts produced by fused filament fabrication (FFF) has been limited due to the presence of voids and poor interlayer welding. Recent advancements in FFF have enabled the fabrication of void-free objects with strong interlayer welding through the use of semicrystalline polymer shells such as high-density polyethylene (HDPE) along with a high viscosity core polymer like acrylonitrile-butadiene-styrene (ABS). Furthermore, the zero-shear viscosity (η0) of ABS is three orders of magnitude higher than HDPE making the ABS-HDPE core-shell configuration preferable. ABS holds the shape by preventing bulk flow and part bending while HDPE promotes full surface contact across the layers. Most polymers, however, are immiscible which causes a weak weld line along the core-shell interface. Herein, maleic anhydride (MAH) is grafted to the butadiene segment of the ABS core thereby compatibilizing the interface with HDPE, improving the interfacial adhesion. Attenuated total reflectance-Fourier transform infrared spectroscopy was employed to confirm successful grafting. Using a custom-made die affording the core-shell structure, the ABS-g-MAH is shown to improve the impact resistance by 253% and 16% compared to neat HDPE and ABS specimens, respectively. Additionally, a 10% increase compared to the unmodified ABS-HDPE core-shell configuration is observed.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Nano-Engineered Interfaces in Dual-Layer Electrodes for Protonic Ceramic Cells with Enhanced Stability and Kinetics

Enhancing interfacial stability and charge transfer in protonic ceramic cells (PCCs) remains a critical challenge, as structural degradation and interfacial resistance often compromise durability and efficiency. Here, we report a nanoengineered dual-layer oxygen electrode architecture designed to address these limitations by introducing a fine-grained nanoparticle interfacial contact layer beneath a porous catalytic backbone. The nanoscale powders, through enhanced sintering activity, densify into a robust interfacial layer that promotes strong chemical bonding, uniform adhesion, and continuous ionic/electronic pathways with the BCZYYb electrolyte. This hierarchical architecture mitigates delamination, redistributes mechanical stress, and establishes efficient charge and mass transport channels without relying on corrosive surface treatments. Electrochemical evaluation demonstrates that the dual-layer design markedly reduces interfacial polarization resistance and accelerates electrode kinetics. Compared to the single-layer counterpart, the architecture achieves a peel strength of 44.53 N/cm 2 , a 40% improvement in peak power density (0.96 W cm –2 at 600 °C), and a 130% enhancement in electrolysis current density (4.78 A cm –2 at 1.57 V). Faradaic efficiency remains as high as 88% under high steam concentrations, underscoring minimal charge loss during practical operation. Notably, the electrode retains stability across 450–600 °C and under transient voltage cycling, with impedance spectra confirming suppressed interfacial resistance growth over prolonged use. These results highlight nanoscale interface engineering as a powerful route to enhance both mechanical robustness and electrochemical kinetics in PCCs. The demonstrated scalability and durability of this architecture provide a versatile platform for advancing solid-state electrochemical systems, including reversible fuel cells and high-efficiency hydrogen production technologies.

Faradaic efficiency↗
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 OSTI2026

Suppressing thermal transport in nonporous polymer hybrids by limiting thermally accessible vibrational modes

Achieving low thermal conductivity in nonporous polymer materials without compromising mechanical integrity remains a longstanding challenge. Conventional strategies, such as introducing porosity, are inherently limited in dense systems. Here, in this study, we demonstrate that thermal transport in polymer–organic filler hybrids is closely associated with the engineered availability of thermally accessible vibrational modes, rather than individual interfacial resistance or porosity. Using PU/organic filler hybrids as a model system, we show that incorporating rigid organic motifs shifts the vibrational density of states toward higher frequencies, where vibrational modes are weakly thermally populated at ambient conditions. This limits the number of heat-carrying channels, leading to suppressed thermal conductivity despite negligible individual interfacial resistance (∼10 −9 m 2 K W −1 ). These findings provide initial evidence that vibrational mode engineering may offer a promising molecular-level route for reducing thermal conductivity in dense polymer–organic hybrid systems.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Highly-Cyclable Room-Temperature Phosphorene Polymer Electrolyte Composites for Li Metal Batteries

Despite significant interest toward solid-state electrolytes owing to their superior safety in comparison to liquid-based electrolytes, sluggish ion diffusion and high interfacial resistance limit their application in durable and high-power density batteries. Here, a novel quasi-solid Li + ion conductive nanocomposite polymer electrolyte containing black phosphorous (BP) nanosheets is reported. The developed electrolyte is successfully cycled against Li metal (over 550 h cycling) at 1 mA cm -2 at room temperature. The cycling overpotential is dropped by 75% in comparison to BP-free polymer composite electrolyte indicating lower interfacial resistance at the electrode/electrolyte interfaces. Molecular dynamics simulations reveal that the coordination number of Li + ions around (trifluoromethanesulfonyl)imide (TFSI - ) pairs and ethylene-oxide chains decreases at the Li metal/electrolyte interface, which facilitates the Li + transport through the polymer host. Here, density functional theory calculations confirm that the adsorption of the LiTFSI molecules at the BP surface leads to the weakening of N and Li atomic bonding and enhances the dissociation of Li + ions. This work offers a new potential mechanism to tune the bulk and interfacial ionic conductivity of solid-state electrolytes that may lead to a new generation of lithium polymer batteries with high ionic conduction kinetics and stable long-life cycling.

2D materials↗
DOE OSTI2021

Interfacial engineering of lithium-polymer batteries with in situ UV cross-linking

Developing promising solid-state Li batteries with capabilities of high current densities have been a major challenge partly due to large interfacial resistance across the electrode/electrolyte interfaces. This work represents an integrated network of self-standing polymer electrolyte and active electrode materials with in situ UV cross-linking. This method provides a uniform morphology of composite polymer electrolyte with low thickness of 20–40 μm. This modification leads to promising cycling results with 85% specific capacity retention in Li||LiFePO4 cell over 100 cycles at high current densities of 170 mA g -1 (~25 μA cm -2 , 1 C). By applying this method, the interfacial resistance decreases as high as seven folds compared to noncross-linked interfaces. The following work introduce a facile and cost-effective method in developing fast-charging self-standing polymer batteries with enhanced electrochemical properties.

25 ENERGY STORAGE↗
DOE OSTI2020

In Situ Formation of Li 3 P Layer Enables Fast Li + Conduction across Li/Solid Polymer Electrolyte Interface

Abstract Solid‐state polymer electrolytes provide better flexibility and electrode contact than their ceramic counterparts, making them a worthwhile pursuit for all‐solid‐state lithium‐metal batteries. However, their large Li/solid state electrolyte interfacial resistance, small critical current density, and rapid lithium dendrite growth during cycling still limit their viability. Owing to these restrictions, all‐solid‐state cells with solid polymer electrolytes must be cycled above room‐temperature and with a small current density. These problems can be mitigated with an in situ formed artificial solid electrolyte interphase that rapidly conducts Li + ions. Herein, a Li 3 P layer formed in situ at the Li‐metal/solid polymer electrolyte interphase is reported that significantly reduces the electrode/electrolyte interfacial resistance. Additionally, this layer increases the wettability of the solid polymer by the metallic lithium anode, allowing for the critical current density of lithium symmetric cells to be doubled by homogenizing the current density at the interface. All‐solid‐state Li/Li symmetric cells and Li/LiFePO 4 cells with the Li 3 P layer show improved cycling performance with a high current density.

Wu, Nan↗
DOE OSTI2026

Designing carbon wetting layers with inorganic salts as additives for enhanced adhesion and molten sodium wettability in electrochemical application

ß” alumina solid-state electrolyte (BASE) is considered one of the most promising materials for sodium batteries due to its high ionic conductivity and exceptional stability with molten sodium. However, at lower operating temperatures, the poor physical contact at the liquid-solid interface between molten sodium and BASE results in high interfacial resistance. In this study, we explore the optimization of carbon wetting layers with various salt additives to enhance adhesion and improve molten sodium wettability. Using a spray-coating method, carbon layers incorporating sodium hexametaphosphate (Na6(PO3)6, SHMP) as an additive demonstrate superior adhesion, mechanical stability, and enhanced wettability with molten sodium. Scanning Electron Microscopy (SEM) analysis reveals that SHMP preserves the porous carbon network required for efficient sodium transport while minimizing structural defects such as cracks and voids. Electrochemical testing using Na symmetric cells confirms that SHMP-modified layers significantly reduce interfacial resistance and overpotential, outperforming No salts counterparts. These findings highlight that the strategic incorporation of suitable additives, such as SHMP, in the design of microscale carbon layers could significantly enhance the performance of molten sodium batteries at lower operating temperatures.

Han, Henry H.↗
DOE OSTI2024

The Microscopic Mechanism of Lithiation and Delithiation in the Ag/C Buffer Layer for Anode‐Free Solid‐State Batteries

Abstract Lithium metal solid‐state batteries (LMSSBs) have demonstrated their high energy density and cycling performance at high current densities in an anode‐free architecture, featuring a thin Ag/C composite buffer layer (BL) between the current collector (CC) and the solid electrolyte (SE). This study explains the microscopic mechanism of the Ag/C BL by using first‐principles atomistic and continuum modeling. It is shown that Ag effectively acts as a homogeneous solid‐solution beyond AgLi 2.32 and maintains a positive potential even at AgLi 25 during lithiation. Key factors underlying the working of the Ag/C BL include lower interfacial resistance at the BL/CC interface than at the BL/SE interface, leading to predominant Li deposition on BL/CC, and substantial Ag–Li volume expansion during lithiation. This, combined with stronger BL/SE adhesion, causes BL/SE separation and Ag–Li extrusion toward the CC side. During delithiation, Ag re‐precipitates as nanoparticles uniformly on the CC, with its positive lithiation potential homogenizing Li currents in subsequent cycles. Other metals are less effective due to their relatively large overpotential, premature lithiation termination, and limited volume expansions hindering movement toward the CC. The study aids the BL design, focusing on metal choice and optimization material and microstructural properties, such as the Li‐ion conductivity and interfacial resistance.

25 ENERGY STORAGE↗
DOE OSTI2021

Robust Solid/Electrolyte Interphase (SEI) formation on Si Anodes Using Glyme-based Electrolytes

Silicon (Si) is the most naturally abundant element possessing 10-fold theoretical capacity than graphitebased anodes. The practicality of implementing Si anodes is, however limited by the unstable solidelectrolyte interphase (SEI) and anode fracturing during continuous lithiation/delithiation. We demonstrate that glyme-based electrolytes (GlyEls) assure a conformal SEI on Si and keep the Si ‘fracture-free’. Benchmarking against the optimal, commonly-used carbonate electrolyte with the fluoroethylene carbonate (FEC) additive, Si anode cycled in a GlyEl exhibits reduced early parasitic current (by 62.5%) and interfacial resistance (by 72.8%), while the cell capacity retention is promoted by >7% over a course of 110 cycles. The mechanistic investigation by X-ray photoelectron spectroscopy (XPS) and energy-dispersive X-ray spectroscopy (EDX) indicates GlyEl enriches Si SEI with elastic polyether but diminishes its carbonate species. Glyme-based electrolytes prove viable in stabilizing the SEI on silicon for future high energy density lithium-ion batteries.

Yang, Guang↗
DOE OSTI2020

Unveiling the critical role of interfacial ionic conductivity in all-solid-state lithium batteries

Advancement of all-solid-state lithium-ion (Li + ) batteries (ASSLIBs) has been hindered by the large interfacial resistance mainly originating from interfacial reactions between oxide cathodes and solid-state sulfide electrolytes (SEs). To suppress the interfacial reactions, an interfacial coating layer between cathodes and SEs is indispensable. However, the kinetics of interfacial Li + transport across the coating layer has not been well understood yet. Herein, we tune the interfacial ionic conductivity of the coating layer LiNb 0.5 Ta 0.5 O 3 (LNTO) by manipulating post-annealing temperature. It is found that the interfacial ionic conductivity determines interfacial Li + transport kinetics and enhancing the interfacial ionic conductivity can significantly boost the electrochemical performance of SE-based ASSLIBs. A representative cathode LiNi 0.5 Mn 0.3 Co 0.2 O 2 coated by LNTO with the highest interfacial ionic conductivity exhibits a high initial capacity of 152 mAh.g -1 at 0.1 C and 107.5 mAh.g -1 at 1C. This work highlights the importance of increasing interfacial ionic conductivity for high-performance SE-based ASSLIBs.

25 ENERGY STORAGE↗
DOE OSTI2021

Current Status and Future Directions of All-Solid-State Batteries with Lithium Metal Anodes, Sulfide Electrolytes, and Layered Ternary Oxide Cathodes

All-solid-state batteries (ASSBs) offer great promise as a next-generation energy storage technology with higher energy density, wider operating temperature range, and improved safety for electric vehicles. ASSBs employing lithium metal anodes (Li), sulfide-based solid-state electrolytes (SSE), and Ni-rich layered transition metal oxide cathodes (LiMO 2 , M = Ni, Mn, Co, Al) are particularly promising due to its superior electrochemical performance compared to other solid-electrolyte systems. However, the battery cycle life at high cathode mass loading and high current is still limited because the failure mechanism is not fully understood. Lithium dendrite growth at the anode or inside a solid electrolyte still represents as a serious risk of cell failure. Interfacial resistance increases attributed to electrolyte decomposition and interfacial void formation at both cathode–electrolyte and anode–electrolyte interfaces lead to gradual capacity fading. In this Review, we present the fundamental challenges and recent scientific understandings of each component in ASSBs. The novel diagnostic tools for these components, especially the interfaces buried under the surface that are often hard for characterization are mainly examined. Lastly, we offer a perspective for future research directions. We hope this Review will provide a timely snapshot of state-of-the-art research progress in ASSBs to accelerate the development of ASSBs.

25 ENERGY STORAGE↗
DOE OSTI2022

Transport and mechanical behavior in PEO-LLZO composite electrolytes

Abstract Composite solid electrolytes (CEs), wherein ion-conducting polymer and ceramic/glass is mixed, are promising candidates for all-solid-state batteries due to their promise of acceptable ionic conductivity and mechanical properties compared to their individual constituents. While numerous studies have focused on improving the performance of CEs, it is still unclear what the material targets are that can result in improved macroscopic performance especially in light of the coupled needs for high transport and high mechanical strength in these materials. In this study, a two-dimensional (2D) mathematical model is developed to investigate electrochemical and mechanical characteristics of CEs. The model is compared to CEs consisting of poly-ethylene-oxide (PEO) polymer and lithium lanthanum zirconium oxide (LLZO) ceramic material with examination of the impact of varying LLZO volume fractions. The potential drop at the PEO-LLZO interface is evaluated using the junction potential theory. Using experimental data from the literature, the model estimates the ionic conductivity, effective transference number, and mechanical stiffness of the CEs. While the mechanical stiffness improves with increasing volume fraction of LLZO, the impact on conductivity and transference number depends on interfacial resistance at the interface. Finally, the study reports CE’s potential to enhance Li-ion transport and mechanical properties to inhibit lithium (Li) dendrite growth.

25 ENERGY STORAGE↗
DOE OSTI2022

Mitigating Interfacial Mismatch between Lithium Metal and Garnet-Type Solid Electrolyte by Depositing Metal Nitride Lithiophilic Interlayer

Solid-state lithium batteries are generally considered as the next-generation battery technology that benefits from inherent nonflammable solid electrolytes and safe harnessing of high-capacity lithium metal. Among various solid-electrolyte candidates, cubic garnet-type Li 7 La 3 Zr 2 O 12 ceramics hold superiority due to their high ionic conductivity (10 –3 to 10 –4 S cm -1 ) and good chemical stability against lithium metal. However, practical deployment of solid-state batteries based on such garnet-type materials has been constrained by poor interfacing between lithium and garnet that displays high impedance and uneven current distribution. Herein, we propose a facile and effective strategy to significantly reduce this interfacial mismatch by modifying the surface of such garnet-type solid electrolyte with a thin layer of silicon nitride (Si 3 N 4 ). This interfacial layer ensures an intimate contact with lithium due to its lithiophilic nature and formation of an intermediate lithium–metal alloy. The interfacial resistance experiences an exponential drop from 1197 to 84.5 Ω cm 2 . Lithium symmetrical cells with Si 3 N 4 -modified garnet exhibited low overpotential and long-term stable plating/stripping cycles at room temperature compared to bare garnet. Furthermore, a hybrid solid-state battery with Si 3 N 4 -modified garnet sandwiched between lithium metal anode and LiFePO 4 cathode was demonstrated to operate with high cycling efficiency, excellent rate capability, and good electrochemical stability. This work represents a significant advancement toward use of garnet solid electrolytes in lithium metal batteries for the next-generation energy storage devices.

25 ENERGY STORAGE↗
DOE OSTI2022

Effect of differently oriented interlayer phases on the radiation damage of Inconel-$\mathrm{Ni}$ multimetallic layered composite

Multimetallic layered composites (MMLCs) have shown an excellent potential for application under extreme environments, e.g., accident-tolerant fuel cladding, because of their low oxidation tendency and high corrosion resistance. Interfacial phases or complexions in nanocrystalline materials accelerate the annihilation of defects and enhance the radiation resistance of materials, making MMLCs with engineered interlayer phases compelling to deploy in extreme conditions. However, implementation of MMLCs in full capacity remained a challenge due to a lack of fundamental understanding of the underlying mechanisms governing the characteristics of the interface between the metallic layers. The precise role of interlayer phases in MMLCs and their interaction with defects, specifically under extreme conditions, is still unexplored. Pursuing atomistic simulations for various Inconel-Ni MMLCs model materials, we revealed accelerated defect mobility in interlayers with larger crystalline misorientation and the inverse relationship between the interface sink strength to the misorientation angle. Furthermore, we found a linear relation between interlayer misorientation angle with the density of radiation-induced defects and radiation enhanced displacements. So, our results indicate that radiation-induced material degradation is accelerated by the higher defect formation tendency of MMLCs with a high-angle interlayer interface.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗