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DOE OSTI2020

Quantitative comparison between sub-millisecond time resolution single-molecule FRET measurements and 10-second molecular simulations of a biosensor protein

Molecular Dynamics (MD) simulations seek to provide atomic-level insights into conformationally dynamic biological systems at experimentally relevant time resolutions, such as those afforded by single-molecule fluorescence measurements. However, limitations in the time scales of MD simulations and the time resolution of single-molecule measurements have challenged efforts to obtain overlapping temporal regimes required for close quantitative comparisons. Achieving such overlap has the potential to provide novel theories, hypotheses, and interpretations that can inform idealized experimental designs that maximize the detection of the desired reaction coordinate. Here, we report MD simulations at time scales overlapping with in vitro single-molecule Förster (fluorescence) resonance energy transfer (smFRET) measurements of the amino acid binding protein LIV-BP SS at sub-millisecond resolution. Computationally efficient all-atom structure-based simulations, calibrated against explicit solvent simulations, were employed for sampling multiple cycles of LIV-BP SS clamshell-like conformational changes on the time scale of seconds, examining the relationship between these events and those observed by smFRET. The MD simulations agree with the smFRET measurements and provide valuable information on local dynamics of fluorophores at their sites of attachment on LIV-BP SS and the correlations between fluorophore motions and large-scale conformational changes between LIV-BP SS domains. We further utilize the MD simulations to inform the interpretation of smFRET data, including Förster radius (R 0 ) and fluorophore orientation factor (κ 2 ) determinations. The approach we describe can be readily extended to distinct biochemical systems, allowing for the interpretation of any FRET system conjugated to protein or ribonucleoprotein complexes, including those with more conformational processes, as well as those implementing multi-color smFRET.

59 BASIC BIOLOGICAL SCIENCES↗

DOE OSTI2020

Oak Ridge National Laboratory Technical Input for the Nuclear Regulatory Commission Review of the 2017 Edition of ASME Section III, Division 5, ‘High Temperature Reactors’

To assist the Nuclear Regulatory Commission in its decision making on endorsement of the American Society for Mechanical Engineers Boiler and Pressure Vessel Code Section III, Division 5 (2017 Edition) for development of advanced non-light water reactors, the following Division 5 portions were reviewed: Article HBB-2000 Material; Article HCB-2000 Material; Article HGB-2000 Material; Mandatory Appendix HBB-I-14 Tables and Figures; and, Nonmandatory Appendix HBB-U Guidelines for Restricted Material Specifications to Improve Performance in Certain Service Applications. In addition to the 2017 Edition, the same parts of the 2019 Edition have also been reviewed as indicated in various sections of the report. This review was conducted by a collaboration of national laboratory and private sector participants with significant industrial experience, including some heavy lifting and deep diving from Clarus Consulting, LLC., all intended to achieve an objective, independent, and practical perspective. The report provides recommendations, descriptions of the evaluation methods, and the source references for the data used. To build confidence required for endorsement of the Code, this review was conducted as a verification and validation of the above Code contents. The objective of verification is to ensure that the Code is free of error – direct or implied; contains the information needed for its use, including proper coverage of the Code-specified materials for the intended application, and completeness and adequacy of references to other portions of the Code. The objective of validation is to authenticate that the Code tabulations and graphs represent design inputs consistent with what are determined using rules and methods specified by the Code. The authentication process used data that were assembled and/or generated independent of Code development, while the methods of analysis followed Code-specified methods where appropriate. The designated portions for this review cover the five alloys codified for high temperature reactor applications in Division 5, i.e. 316 SS, 304 SS, 800H, 2¼Cr-1Mo, and 9Cr-1Mo-V, regarding their general requirements, permitted specifications and design stress intensity values for pressure-retaining applications, deterioration in service, fatigue acceptance test, permissible weld materials, tensile and yield strength, expected minimum stress-to-rupture values (including for Alloy 718), weld stress rupture factors, permissible materials for bolting use, and restricted specifications in certain service applications. Additionally, stress intensity values for bolting materials including 316 SS, 304 SS and alloy 718 were reviewed. Analysis and discussion are also provided on contents outside of these designated Code portions where it was deemed relevant and necessary to develop a technically sound understanding of issues relating to the designated portions. Due to unavailability of sufficient test data on welds during the review period, the weld stress rupture factors in Tables HBB-I-10.14A to E, which cover a total of ten tables for the five alloys welded with twenty-eight different weld metals (some with similar properties), have been deferred to a future review effort. The review identified mainly two types of issues. The first type includes instances where the Code is found factually incomplete or incorrect, such as obsolete materials specifications listings, missing tabulation of stresses for bolting. Changes to the Code are recommended in these cases. The second type of issue includes instances where the Code tabulations and graphs are found to be less conservative than the review analysis results. In these cases, recommendations are made for further review and consideration where the difference in conservatism exceeds 10%, which is our threshold for questioning technical adequacy, meriting a risk assessment by the Nuclear Regulatory Commission and/or reactor designers. It is noted that this effort has been executed using all available data and established methods of analysis, including methods and criteria specified and used by the Code. As such, the findings that are presented in quantitative detail, in a format for convenient comparison with the Code, and with identification of where further review is recommended, should provide a sound technical basis for decisions about quantifying the implications of the reduced design margins and technical adequacy/inadequacy to form a basis for conditioning specific Code tabulation values on endorsement. Recommendations for specific changes to the Code, however, entail design conservatism considerations beyond the scope of this review effort, and are not made in this report.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

DOE OSTI2021

Corrosion of 347 stainless steel in the presence of uranyl sulfate solution and radiation

The U.S. molybdenum 99 (Mo-99) industry is pursuing production of fission-made Mo-99 using a uranium solution such as uranyl sulfate. In this process, uranyl sulfate solution containing low-enriched uranium will be bombarded by neutrons creating Mo-99 and other fission products. During the production, the uranyl sulfate solution will be irradiated until an acceptable activity level of Mo-99 is produced. The uranyl sulfate solution containing Mo-99 and other fission products will then undergo a series of separation steps. First, uranyl sulfate can be separated from Mo-99 using a primary titania column to recover Mo-99, with the uranyl sulfate solution to be used for another irradiation cycle. Then, raffinate from a primary titania column containing Mo-99 can be concentrated and purified using a LEU modified Cintichem process developed by Argonne National Laboratory. During irradiation, the temperature of the uranyl sulfate solution can reach near boiling (up to ~80° C assumed), causing radiolysis of water and the resultant formation of hydrogen peroxide. Because high-radiation fields will be present during each irradiation cycle, it is important to determine the corrosion rates of SS-347 under such conditions to estimate the life cycle of the target solution vessel. The buildup of corrosion products from the SS components in the uranyl sulfate solution also needs to be well understood because potential accumulation of iron, nickel, and other corrosion products may affect the Mo-99 recovery and purification process. To study the corrosion rates of SS-347 material under conditions relevant to future Mo-99 production facility, SS-347 coupons in uranyl sulfate solution at ~80° C were irradiated using Argonne’s Van de Graaff generator, which can generate high-radiation fields without fissioning of uranium or production of activation products.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2021

Scaling-Up and Roll-to-Roll Processing if Highly Conductive Sulfide Solid-State Electrolytes (CRADA 510)

This project aims to identify and address key technical barriers in scale-up synthesis and roll-to-roll processing of highly conductive solid-state electrolytes (SSEs) by leveraging PNNL’s patent pending SSEs, Ampcera Inc.’s environmentally friendly manufacturing capability, and UW’s rollto-roll processing. The ultimate goals are 1) development of novel sulfide SSEs with room temperature Li+ conductivity > 5 mS/cm and Li/SSE interfacial resistance <5 Ωcm2, 2) scalable production of sulfide SSEs at 1 metric ton/year, and 3) a high throughput roll-to-roll processing of highly conductive (>1 mS/cm) and ultra-thin solid film (10-100 μm). The materials and the solid film achieved in the project will be tested at practical conditions and validated in a realistic pouch cell format with achievable energy > 300 Wh/Kg.

36 MATERIALS SCIENCE↗

DOE OSTI2023

Niowave Neutron Source Converter: Lead-Bismuth-Eutectic (LBE) Windowless Target Design and Evaluation

Los Alamos National Laboratory (LANL) is working with Niowave on the design and evaluation of their lead-bismuth-eutectic (LBE) windowless target (i.e., neutron source converter). Niowave plans to use 200 kW electron beam at 40 MeV beam energy to produce neutrons by photonuclear reaction with LBE. Then, the neutrons undergo fission at the surrounding uranium target assembly (UTA) to produce Molybdenum 99 (Mo-99) as a fission product, which eventually decays to Technetium-99 (Tc-99m). Tc-99m is one of important radioisotopes that is used for medical diagnostics. LANL conducted 3D multiphysics analysis for the Niowave neutron converter design and provided design assessment in thermohydraulic aspects. LANL conducted radiation transport calculations using Monte-Carlo N-Particle (MCNP) code with unstructured meshing scheme. The 3D volumetric heating profiles in the LBE and Stainless-Steel (SS) housing were imported into multiphase computational fluid dynamics (CFD) to obtain 3D temperature profiles of LBE and SS through conjugate heat transfer (CHT) analysis. The key findings are: LBE film thickness at the center of the beam is approximately 1.6 cm with a maximum LBE velocity of approximately 1.8 m/s, which is below a 2 m/s limit to avoid erosion issues on supporting structures; Heat deposition in the LBE peaks at ~1 cm depth from the LBE free-surface because of the forward interactions of electron, photon, and neutron with LBE; LBE maximum temperature is ~360 °C, which is below LBE evaporation initiative temperature, ~450 °C; LBE-SS interface temperature is ~350 °C, which is below the safety thermal limit to prevent severe corrosion on SS. The results indicate that Niowave’s neutron converter design satisfies both hydraulic and thermal criteria for safe operation. By virtue of such computational analysis, Niowave can move toward establishing an experimental setup to experimentally test their LBE neutron converter. The following sections describe the detailed work done by LANL.

43 PARTICLE ACCELERATORS↗

DOE OSTI2024

Bench-Scale Electrolytic Dissolution of Quarter-Scale FCA Cans

In 2016, the Savannah River National Laboratory (SRNL) led, in support of and under sponsorship of the Department of Energy’s National Nuclear Security Administration (DOE/NNSA) Office of Material Management and Minimization (M3), the removal and transfer of the plutonium based Fast Critical Assembly (FCA) fuel from the Japan Atomic Energy Agency (JAEA) Tokai facility to the Savannah River Site (SRS). The team also included JAEA, multiple organizations in Savannah River Nuclear Solutions (SRNS), International Nuclear Services, and many other entities. The FCA fuel removal project completion was a key deliverable for M3 to the 2016 Nuclear Security Summit and constituted the largest inventory of weapons-usable plutonium removed under the nonproliferation program. The FCA materials consist of thousands of stainless steel (SS) clad plates and hundreds of SS clad rods. The FCA fuel elements were packaged in a carrier can and stored at SRS pending disposition of the fuel. Following an assessment of candidate disposition options, SRNS identified electrolytic dissolution (ED) as the most promising disposition option for the FCA plates and their preferred option was endorsed by DOE. This option entails electrochemically dissolving the entire FCA carrier can with fuel elements and was based on bench-scale laboratory testing and historical work on processing SS-clad and zirconium-clad uranium-based fuel in the H-Canyon electrolytic dissolver (last operated in 1980). The FCA plate consists of a plutonium-aluminum metal alloy core hermitically sealed in SS cladding.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2025

Biofouling and Corrosion Study for a Novel Linear Guided Wave Energy Converter (Post Access Report)

The overall objective of this project was to examine the reliability and performance of antibiofouling coatings used for a wave energy converter (WEC) developed by E-Wave Technologies. The particular coatings were selected for their low toxicity and potential compatibility with aquaculture. The aim of this work was to 1) test coating solutions to prevent biofouling growth and saltwater corrosion on the static (paddle and attachment frame surface) components of the WEC that are submerged, 2) determine adhesion of the coatings to system components, and 3) assess the ease and effectiveness of biofouling cleaning to insure long term performance of the system. An analysis of commercial coatings was performed using methods to examine the prevention of biofouling and coating adhesion properties on two key materials of the WEC, which were 316L low carbon marine grade stainless steel (SS) and Ultra High Molecular Weight Polyethylene (PE). Three marine antifouling paints were selected based on their unique properties to test how different paint styles perform on different materials. The selected paints were ePaint Ecominder self-polishing paint with Zinc Omadine for slime control, Pettit ECO HRT Copper-Free ablative antifouling with Econea biocide, and Intersleek 1100SR foul release. Pacific Northwest National Laboratory (PNNL) prepared PE and SS substrates coated with the three paints and compared the performance against uncoated substrates when submerged in raw seawater for 3-, 6-, and 9-month (m) time periods. Results in adhesion testing indicated that Pettit and ePaint materials clearly bonded strongly to SS, but did not bond comparably well to PE. It was noted during adhesion testing that the Intersleek surfaces were especially difficult to test as the paint highly resists bonding to the epoxy adhesives used with the adherence testing platform. The wear rate of the coatings was not measured under this study; however, based on adhesion testing, coatings in the sliding regions of the Ewave device are expected to wear rapidly. Sandia National Laboratories (SNL) evaluated the adhesion of three different paints to PE and SS substrates which were exposed to a marine environment for time intervals of 0, 3, 6, and 9 months. From qualitative visual analysis of the 3 in2 coupons when pulled from the tank, the 3 in2 coupons generally only appeared to have biofouling consisting of filamentous algae or diatoms, which all have relatively low mass and can be easily wiped from the surface of coupons. Qualitative visual analysis indicated that ECO HRT and Unpainted were consistently worse than Intersleek and Ecominder at all time points. Results provide insight to aid with down-selection of commercial coatings under static conditions to support reliability of the WEC and potential maintenance schedules. This investigation was conducted using small coupon samples suspended in seawater and the development of testing rigs for dynamic component level testing is needed for future work. In addition, the potential toxicity of these commercial coatings on aquaculture has not been determined by this study. One recommendation is to conduct toxicity investigations at the Environmental Toxicity Laboratory at Oak Ridge National Laboratory.

16 TIDAL AND WAVE POWER↗

DOE OSTI2024

Transfer of beef bacterial communities onto food-contact surfaces

Introduction Food spoilage and pathogenic bacteria on food-contact surfaces, especially biofilm-forming strains, can transfer to meats during processing. The objectives of this study were to survey the bacterial communities of beef cuts that transfer onto two commonly used food-contact surfaces, stainless steel (SS) and high-density polyethylene (HDPE) and identify potentially biofilm-forming strains. Methods Top round, flank, chuck, and ground beef were purchased from 3 retail stores. SS and HDPE coupons (approximately 2cm × 5cm) were placed on beef portions (3h, 10°C), after which, the coupons were submerged halfway in PBS (24h, 10°C). Bacteria from the beef cuts and coupon surfaces ( n = 3) were collected, plated on tryptic soy agar plates and incubated (5 days, 25°C). Bacterial isolates were identified by 16S rRNA gene amplicon sequencing and assayed for biofilm formation using a crystal violet binding (CV) assay (72h, 10°C). Additionally, beef and coupon samples were collected for bacterial community analysis by 16S rRNA gene amplicon sequencing. Results and discussion Sixty-one of 972 beef isolates, 29 of 204 HDPE isolates, and 30 of 211 SS isolates were strong biofilm-formers (Absorbance>1.000 at 590 nm in the CV assay). Strong-binding isolates identified were of the genera Pseudomonas , Acinetobacter , Psychrobacter , Carnobacterium , and Brochothrix . Coupon bacterial communities among stores and cuts were distinct ( p < 0.001, PERMANOVA), but there was no distinction between the communities found on HDPE or SS coupons ( p > 0.050, PERMANOVA). The bacterial communities identified on the coupons may help determine the communities capable of transferring and colonizing onto surfaces, which can subsequently cross-contaminate foods.

Guron, Giselle K. P.↗

DOE OSTI2023

Corrosion Resistance of 309L Stainless Steel Claddings on Carbon Steel Produced with Wire-Fed Directed Energy Deposition

Additive manufacturing (AM) tools are capable of applying overlay austenitic stainless steel (SS) claddings to carbon steel components. The benefits of this approach over arc welding include a smaller heat-affected zone, residual stress reduction, and material savings. In particular, wire-directed energy deposition is a suitable technique because of its low material cost and high rate of production compared to other AM methods. However, metallurgical variations in composition, phase fraction, and microsegregation can potentially influence the corrosion behavior of such claddings. In this work, 309L SS is clad on carbon steel substrates and electrochemical methods are used to measure their general and pitting corrosion resistance in simulated marine environments (3.5 wt% NaCl solutions). Two-layer claddings are fabricated with four laser powers to understand the effects of bulk chemical composition, austenite/δ-ferrite phase fractions, and individual phase compositions on corrosion behavior. The two-layer claddings are compared to a single-layer cladding, wrought 304 SS, and the carbon steel substrate for a comprehensive assessment of corrosion performance. The two-layer claddings are remarkably resistant to general corrosion in the 3.5 wt% NaCl environment because of their high Cr content (21.6 wt% to 23.3 wt% Cr). The single-layer cladding exhibits localized corrosion at unmixed Fe-rich peninsulas that originate at the dissimilar metal boundary and protrude into the first cladding layer. All two-layer claddings possess higher pitting corrosion resistance than wrought 304 SS, demonstrating their effectiveness as a corrosion-resistant barrier. Here, the pitting corrosion resistance is superior for claddings made with lower laser powers, due to low dilution and greater δ-ferrite contents.

36 MATERIALS SCIENCE↗

DOE OSTI2023

Development, Characterization, and Testing of Solid-State Electrolytes for Batteries

Traditional liquid electrolytes used in lithium (Li) metal batteries (LMBs) have severe safety issues, poor power density, as well as thermal and electrochemical instability that prevents their scaling to newer applications, such as electric vehicles. Using sulfide-based solid-state electrolytes (SSEs) is a viable method to address many of the issues that plague LMBs. However, the key issue preventing the expansion of sulfide-based SSEs is an interplay between poor interfacial stability with the electrodes and massive external stack pressure required to maintain electrode-electrolyte contact. The need for extensive pressure requires large system-level (i.e., battery pack used in an electric vehicle) housing that causes a disconnect between performance at a smaller scale and actual application. Secondary prevention to sulfide-based SSE adoption are difficulties in manufacturing, as toxic deterioration occurs when these materials are exposed to humidity, as well as drastic reduction in SSE performance at low temperature. This work hypothesizes that unique interfacial designs of electrodes and the modification of the sulfide-based SSE will enable reduction of necessary external cell pressure, and therefore support the design of practical LMBs. This will be done through collaboration within Idaho National Laboratory (INL), where manufacturing practices will be parameterized to produce low defect, low porosity SSEs with slight modifications. Next, artificial interfaces will be produced on electrodes to observe the conformality and mass transport properties between the modified SSE and pre-treated anode. External pressure on Li-metal cells will also be parameterized to reduce interfacial impedance while a reduction in the pressure will allot reasonable housing design for larger scale applications. Focus on novelty in this work occurs by modifications to the solid-solid interfaces between electrolyte and electrode, done through doping of the electrolyte and production of artificial interfaces on the Li-metal anode. The modifications at these interfaces, in addition to modified external pressure could identify and address the poor interfacial impedance that hinders high performance SSEs. Fundamental understanding on how to reduce the key hindrances of all-solid-state batteries (ASSBs) will support the advancement for larger scale production and performance, of which will be held in perspective for future works. Beyond battery development, the knowledge gained from process control and defect analysis is applicable to other ceramic systems, such as nuclear fuel coatings and high temperature electrolyzers.

25 ENERGY STORAGE↗

DOE OSTI2023

Development, Characterization, and Testing of Solid-State Electrolytes for Batteries

25 ENERGY STORAGE↗

DOE OSTI2023

Seismic detection switch

A seismic switch (SS) that is able to detect and signal when internal faults have occurred within the SS is described. The SS provides safety class functionality to the detection of seismic activity. For example, the SS may detect earthquakes above a specified level, resulting in the disconnection of electrical power to a radioactive waste storage facility, which could result in the ignition of waste materials should the storage facility and/or storage container fail during a seismic event. By reducing the risk of fire under these circumstances, the possibility of offsite releases is significantly reduced.

Hayward, Allen D.↗

DOE OSTI2025

Filter-Banks for Ultra-Wideband Communications, Sensing, and Localization

Recently, filterbank multi-carrier spread spectrum (FBMC-SS) has been proposed as a candidate waveform for ultrawideband (UWB) communications. It has been noted that FBMCSS is a perfect match to this application, leading to a trivial method of matching to the required spectral mask at different regions of the world. FBMC-SS also allows easy rejection of high-power interfering signals that may appear over different parts of the UWB spectral band. In this paper, we concentrate on the use of staggered multitone spread spectrum (SMT-SS) for UWB communications. SMT makes use of offset QAM modulation to transmit data symbols over narrowband, overlapping subcarrier bands. This form of FBMC-SS is well-suited to UWB communications because it has good spectral efficiency and a flat power spectral density (PSD), resulting in good utilization of the UWB spectral mask. Additionally, we explore new methods for multi-coding that result in higher bit rates than previous FBMCSS systems. Moreover, we study methods for equalizing the UWB multipath channel and cancelling narrowband interference. Excellent performance of the proposed methods are substantiated by presenting simulation results.

99 - GENERAL AND MISCELLANEOUS↗

DOE OSTI2024

Spike-and-Slab Shrinkage Priors for Structurally Sparse Bayesian Neural Networks

Network complexity and computational efficiency have become increasingly significant aspects of deep learning. Sparse deep learning addresses these challenges by recovering a sparse representation of the underlying target function by reducing heavily overparameterized deep neural networks. Specifically, deep neural architectures compressed via structured sparsity (e.g., node sparsity) provide low-latency inference, higher data throughput, and reduced energy consumption. In this article, we explore two well-established shrinkage techniques, Lasso and Horseshoe, for model compression in Bayesian neural networks (BNNs). To this end, we propose structurally sparse BNNs, which systematically prune excessive nodes with the following: 1) spike-and-slab group Lasso (SS-GL) and 2) SS group Horseshoe (SS-GHS) priors, and develop computationally tractable variational inference, including continuous relaxation of Bernoulli variables. We establish the contraction rates of the variational posterior of our proposed models as a function of the network topology, layerwise node cardinalities, and bounds on the network weights. Furthermore, we empirically demonstrate the competitive performance of our models compared with the baseline models in prediction accuracy, model compression, and inference latency.

97 MATHEMATICS AND COMPUTING↗

DOE OSTI2020

3D Hybrid Nanofiber Aerogels Combining with Nanoparticles Made of a Biocleavable and Targeting Polycation and MiR‐26a for Bone Repair

Abstract The healing of large bone defects represents a clinical challenge, often requiring some form of grafting. 3D nanofiber aerogels could be a promising bone graft due to their biomimetic morphology and controlled porous structures and composition. miR‐26a has been reported to induce the differentiation of bone marrow‐derived mesenchymal stem cells (BMSCs) and facilitate bone formation. Introducing miR‐26a with a suitable polymeric vector targeting BMSCs could improve and enhance the functions of 3D nanofiber aerogels for bone regeneration. Herein, the comb‐shaped polycation (HA–SS–PGEA) is first developed, carrying a targeting component, biocleavable groups, and short ethanolamine (EA)‐decorated poly(glycidyl methacrylate) (PGMA) (abbreviated as PGEA) arms as miR‐26a delivery vector. Thereafter, the cytotoxicity and transfection efficiency of this polycation and cellular response to miR‐26a‐incorporated nanoparticles (NPs) are assessed in vitro. HA–SS–PGEA exhibits a stronger ability to transport miR‐26a and exert its functions than the gold standard polyethyleneimine (PEI) and low‐molecular‐weight linear PGEA. The efficacy of HA–SS–PGEA/miR‐26a NPs loaded 3D hybrid nanofiber aerogels showing a positive effect on the cranial bone defect healing is finally examined. Together, the combination of 3D nanofiber aerogels and functional NPs consisting of a biodegradable and targeting polycation and therapeutic miRNA could be a promising approach for bone regeneration.

Li, Ruiquan↗

DOE OSTI2025

Manganese‐Based Spinel Cathodes: A Promising Frontier for Solid‐State Lithium‐Ion Batteries

Recently, all-solid-state lithium-ion batteries (ASSLIBs), which exhibit improved safety and enhanced energy density compared to conventional commercialized lithium-ion batteries (LIBs), thereby have garnered extensive research interest. Among the promising cathode candidates, Mn-based spinel cathodes LiMn 2 O 4 (LMO) and LiNi 0.5 Mn 1.5 O 4 (LNMO), with the unique characteristics of low cost, structural stability, and 3D Li-ion diffusion channels, have demonstrated excellent performance in LIBs and presented great potential in ASSLIBs applications. However, several challenges, including structural degradations, poor interfacial contact, large interfacial resistance, and Mn-dissolution/diffusion during the electrochemical cycling, hinder their practical applications and commercialization in the ASSLIBs. Particularly, the high-voltage LNMO cathodes suffer from the challenge of electrochemical incompatibility with most of the solid-state electrolytes (SSEs). Herein, the spinel structure, the electrochemical behavior, and the structural degradation of the LMO/LNMO are explored. The characteristics and recent progress of the mitigating strategies to the challenges of various SSEs, including polymer-, oxide-, composite-, sulfide-, halide-, and LiPON-based SSEs, are introduced when paired with LMO/LNMO. Finally, the directions for future research to advance Mn-based spinel cathodes and fulfill the requirements of the next-generation ASSLIBs are also discussed.

Dou, Yu [Concordia University, Montreal, QC (Canad↗

DOE OSTI2025

Chemical Bond Covalency in Superionic Halide Solid‐State Electrolytes

Abstract Halide solid‐state electrolytes (SSEs) are promising superionic conductors with high oxidative stability and ionic conductivity, making them attractive for all‐solid‐state lithium‐ion batteries. However, most studies have focused on ion‐stacking structures, overlooking the role of bond characteristics in ionic transport. Here, we investigate bond dynamics and the superionic transition (SIT) in bromide electrolyte, Li 3 InBr 6 , using synchrotron X‐ray techniques and ab initio molecular dynamics (AIMD) simulations. We demonstrate that the SIT in halide SSEs is driven by a thermally induced transition in bonding character (ionic to covalent) rather than a change in crystal phase. AIMD simulations further reveal enhanced Li⁺ diffusion and collective anion motion at elevated temperatures. Expanding our study to Li 3 LnBr 6 (Ln = Gd, Tb, Ho, Tm, and Lu), we confirm the widespread occurrence of SIT in this material class, with Li 3 GdBr 6 exhibiting the highest ionic conductivity (5.2 mS cm −1 at 298 K). More importantly, the ionic‐covalent transition is highly tunable through electrolyte modifications, such as cation/anion substitution and synthesis methods. Our findings provide a new perspective on ionic transport, highlighting the critical role of chemical bond characteristics in halide SSEs.

Chemistry↗

DOE OSTI2025

Binder Effects on Processing, Mechanical Properties, and Performance of Thin Sulfide Solid‐State Electrolytes

All‐solid‐state batteries (ASSBs) offer enhanced safety and energy density compared to conventional lithium‐ion batteries by replacing flammable liquid electrolytes with solid‐state electrolytes (SSEs). Among SSEs, sulfide‐based electrolytes exhibit high ionic conductivity and mechanical deformability, making them promising candidates for next‐generation energy storage. However, their practical implementation is hindered by interfacial instability, mechanical brittleness, and challenges in fabricating ultrathin electrolyte membranes (<30 μm) with robust mechanical integrity. Here, this study systematically examines the influence of polymeric binders—polyisobutylene, hydrogenated nitrile butadiene rubber, and styrene–ethylene–butylene–styrene (SEBS)—on the structural, mechanical, and electrochemical performance of thin sulfide SSE membranes. Key findings reveal that SEBS enables the fabrication of ultrathin, uniform membranes, while binder elasticity significantly affects structural stability during cycling. Operando stack pressure measurements indicate that binder properties directly influence adhesion force for LPSCl particles, influencing their stabilizing cycling period. These results underscore the critical role of polymer binders beyond mechanical reinforcement, positioning them as essential design variables in sulfide SSE engineering. By linking binder chemistry to processability and electrochemical performance, this study provides insights into optimizing sulfide SSEs, advancing their commercial viability in ASSBs.

argyrodite sulfide electrolyte↗