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At least 253 records · Page 14

Catalog of topological phonon materials

Phonons play a crucial role in many properties of solid-state systems, and it is expected that topological phonons may lead to rich and unconventional physics. On the basis of the existing phonon materials databases, we have compiled a catalog of topological phonon bands for more than 10,000 three-dimensional crystalline materials. Using topological quantum chemistry, we calculated the band representations, compatibility relations, and band topologies of each isolated set of phonon bands for the materials in the phonon databases. Additionally, we calculated the real-space invariants for all the topologically trivial bands and classified them as atomic or obstructed atomic bands. We have selected more than 1000 “ideal” nontrivial phonon materials to motivate future experiments. The datasets were used to build the Topological Phonon Database.

Science & Technology - Other Topics↗

Summary Report on Ion Irradiation Study of Ceramic Coating on Suppressing FCCI

Advanced cladding is critical for advanced nuclear reactors with an enhanced performance in radiation tolerance and neutron transparency. Using advanced cladding will ensure the adequate thermal conductivity and mechanical stability of the cladding base material, corrosion resistance, high-temperature coolant compatibility of the cladding surface, and chemical stability in the cladding inner wall against fuel cladding chemical interaction (FCCI). An innovative cladding with a three-layer structure (i.e., a modified surface, a clad base material, and a modified inner wall) promises to meet all these requirements. Initial research and development (R&D) regarding this innovative cladding seek to demonstrate the effectiveness of a thin ceramic coating in suppressing FCCI under ion irradiation to high dose. This United States (U.S.) Department of Energy (DOE)–Office of Nuclear Energy (NE) project report summarizes the results of recent ion irradiation studies of diffusion-couple samples with details of an ion irradiation experiment, the characterization of the interface microstructure of cerium (Ce)/titanium nitride (TiN)/oxide-dispersion strengthened (ODS), Ce/TiN/iron (Fe), Ce/ODS, and Ce/Fe samples irradiated with 80 million electron-volts (MeV) of xenon (Xe) ions to 100 displacements per atom (dpa) at 500?C using the Argonne Tandem Linac Accelerator System (ATLAS) facility at Argonne National Laboratory (ANL). The results of the ODS-substrate sample are encouraging and demonstrate the effectiveness of a thin ceramic coating on FCCI mitigation under irradiation. The results from an Fe-substrate sample revealed a complex microstructure, and the root cause is discussed.

36 MATERIALS SCIENCE↗

Enhanced Switching Reliability of Hf 0.5 Zr 0.5 O 2 Ferroelectric Films Induced by Interface Engineering

Ferroelectric materials have been widely researched for applications in memory and energy storage. Among these materials and benefiting from their excellent chemical compatibility with complementary metal–oxide–semiconductor (CMOS) devices, hafnia-based ferroelectric thin films hold great promise for highly scaled semiconductor memories, including nonvolatile ferroelectric capacitors and transistors. However, variation in the switched polarization of this material during field cycling and a limited understanding of the responsible mechanisms have impeded their implementation in technology. Here, we show that ferroelectric Hf 0.5 Zr 0.5 O 2 (HZO) capacitors that are nearly free of polarization “wake-up”─a gradual increase in switched polarization as a function of the number of switching cycles─can be achieved by introducing ultrathin HfO 2 buffer layers at the HZO/electrodes interface. High-resolution transmission electron microscopy (HRTEM) reveals crystallite sizes substantially greater than the film thickness for the buffer layer capacitors, indicating that the presence of the buffer layers influences the crystallization of the film (e.g., a lower ratio of nucleation rate to growth rate) during postdeposition annealing. This evidently promotes the formation of a polar orthorhombic (O) phase in the as-fabricated buffer layer samples. Synchrotron X-ray diffraction (XRD) reveals the conversion of the nonpolar tetragonal (T) phase to the polar orthorhombic (O) phase during electric field cycling in the control (no buffer) devices, consistent with the polarization wake-up observed for these capacitors. The extent of T–O transformation in the nonbuffer samples is directly dependent on the duration over which the field is applied. Here these results provide insight into the role of the HZO/electrodes interface in the performance of hafnia-based ferroelectrics and the mechanisms driving the polarization wake-up effect.

36 MATERIALS SCIENCE↗

Data Mining of the Rocky Flats Library Archive for Plutonium Compatibility Studies

The objective of this project was to create a searchable database of plutonium compatibility studies from the Rocky Flats Archive. The Rocky Flats Plant was a manufacturing complex in Golden, Colorado that produced nuclear weapons. It primarily focused on producing plutonium pits, which were the cores of many nuclear implosion-type weapons. Because plutonium is an extremely reactive metal, avoiding the use of incompatible materials is imperative to avoid damaging the plutonium pit during its production. The Rocky Flats Plant had conducted extensive surveys of materials used in plutonium pit fabrication for their compatibility with plutonium.

36 MATERIALS SCIENCE↗

Strain as a Global Factor in Stabilizing the Ferroelectric Properties of ZrO 2

Since the discovery of ferroelectricity in doped HfO 2 and ZrO 2 thin films over a decade ago, fluorite-structured ferroelectric thin films have attracted much research attention due to their excellent scalability and complementary metal-oxide semiconductor compatibility compared to conventional perovskite ferroelectric materials. Although various factors influencing the formation of the ferroelectric properties are identified, a clear understanding of the causes of the phase formation have been difficult to determine. In this work, ZrO 2 films deposited by atomic layer deposition and chemical solution deposition have resulted in films with completely different structural properties. Regardless of these differences, a general relationship between strain and phase formation is established, leading to a more unified understanding of ferroelectric phase formation in undoped ZrO 2 films, which can be applied to other fluorite-structured films.

36 MATERIALS SCIENCE↗

Nanocomposite Ionogel Electrolytes for Solid‐State Rechargeable Batteries

Abstract Ionogels composed of ionic liquids and gelling solid matrices offer several advantages as solid‐state electrolytes for rechargeable batteries, including safety under diverse operating conditions, favorable electrochemical and thermal properties, and wide processing compatibility. Among gelling solid matrices, nanoscale materials have shown particular promise due to their ability to concurrently enhance ionogel mechanical properties, thermal stability, ionic conductivity, and electrochemical stability. These beneficial attributes suggest that ionogel electrolytes are not only of interest for incumbent lithium‐ion batteries but also for next‐generation rechargeable battery technologies. Herein, recent advances in nanocomposite ionogel electrolytes are discussed to highlight their advantages as solid‐state electrolytes for rechargeable batteries. By exploring a range of different nanoscale gelling solid matrices, relationships between nanoscale material structure and ionogel properties are developed. Furthermore, key research challenges are delineated to help guide and accelerate the incorporation of nanocomposite ionogel electrolytes in high‐performance solid‐state rechargeable batteries.

Hyun, Woo Jin↗

Performance Degradation of Amine-Infused Fiber Sorbents for Direct Air Capture: Mechanisms and Solutions

Sorbent stability poses significant impacts on longterm performance of direct air capture (DAC) of CO 2 and levelized cost of capture (LCOC). We report the DAC performance degradation of amine-infused fiber sorbents based on poly(ethylenimine) (PEI), mesoporous SiO 2 , and cellulose acetate (CA) over CO 2 cyclic sorption cycles in a nonoxidative environment. Infrared and nuclear magnetic resonance spectra indicate that the aminolysis reactions between CA ester moieties and PEI amine sites lead to the formation of acetamides and hence lower CO 2 affinities of the sorbents. This stability issue can be remedied by hydrolysis treatment of the CA fiber sorbents before PEI impregnation or replacing CA with poly(ether sulfone). This study underscores the importance of selecting proper support or additive materials of DAC contactors that are compatible with active species of CO 2 capture.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Development and Characterization of Electrodes for Surface-Specific Attenuated Total Reflection Two-Dimensional Infrared Spectroelectrochemistry

Electrochemical interfaces still have remaining mysteries surrounding the interfacial region of the electrical double layer, despite being prevalent throughout the energy and water remediation industries. The electrical double layer is where many important dynamic processes such as catalysis and electron transfer occur. The goal of this work is to study the electrical double layer with two-dimensional infrared (2D IR) spectroscopy to experimentally access the details of the structural dynamics of this complex environment. However, there are several experimental challenges to applying 2D IR spectroscopy to this application, such as assuring the surface specificity of the spectrum, optimizing the signal strength while minimizing spectral distortions from dispersion and Fano line shapes, and selecting electrode materials that are both sufficiently IR compatible and conductive. Here we will discuss various considerations when designing 2D IR experiments of electrode interfaces utilizing several substrates and experimental configurations and demonstrate a robust method for 2D IR experiments of electrode interfaces under applied potential that combines nonconducting Si ATR wafers with conductive ITO and thin nanostructured films of plasmonically active Au functionalized with 3-mercapto-2-butanone (MCB). We show that layered electrodes on thin Si ATR wafers with MCB are sensitive to applied potential and that the distortions in the linear and 2D IR spectra are heavily dependent on the morphology of the Au surface.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

4 V Na Solid State Batteries Enabled by a Scalable Sodium Metal Oxyhalide Solid Electrolyte

All-solid-state sodium batteries (ASSSBs) are viable candidates for large scale energy storage that could vie with lithium. Ductile solid catholytes for such cells that can be prepared without extensive ball milling and directly paired with high voltage sodium cathodes are lacking, however. We report a new amorphous fast Na-ion conducting metal oxychloride that meets these criteria, synthesized through a scalable and low-cost route based on a spontaneous solid-state reaction with simple short mixing and 100 °C annealing. It has an ionic conductivity of 1.2 mS·cm–1 and low activation energy of 0.31 eV. Due to its dual O2–/Cl– framework, it exhibits a high anodic potential of 4 V vs Na+/Na and good chemical/electrochemical compatibility with high voltage sodium cathode materials. ASSSBs consisting of the oxychloride solid electrolyte paired with a high voltage P2–Na2/3Ni1/3Mn2/3O2 cathode showed stable long-term cycling with a 4.0 V vs Na3Sn cutoff potential and even to 4.3 V.

solid-state electrolyte, solid-state batteries, Nu↗

Structural design strategies for superionic sodium halide solid electrolytes

We report sodium all-solid-state batteries (ASSBs) with superionic solid electrolytes (SEs) show substantial potential for large-scale energy-storage applications. Recently, lithium halide SEs have attracted attention owing to their potential compatibility with high-voltage cathode materials and high ionic conductivity. Although sodium halide SEs are believed to exhibit good electrochemical stability, very few compounds have been reported. This study provides design principles for superionic sodium halide SEs through systematic theoretical investigations of Na 3 MX 6 (X = Cl, Br, and I). The Na 3 MX 6 structures depend on the types and sizes of M and X: Na 3 MCl 6 and Na 3 MBr 6 prefer the $P\bar{3}$1c, P2 1 /n and $R\bar{3}$ phases, whereas Na 3 MI 6 prefers the C2/m phase. The Na 3 MI 6 C2/m phase is found to exhibit reasonably high ionic conductivity (~10 -4 S/cm -1 ) and anion mixing with Br further improve Na-ion migration, leading to an even higher ionic conductivity (~10 -3 S/cm -1 ) for Na 3 MBr 3 I 3 . The material design principles in this study provide fundamental guidelines for the development of superionic Na halide SEs for high-voltage Na ASSBs

25 ENERGY STORAGE↗

Generalizable, tunable control of divalent cation solvation structure via mixed anion contact ion pair formation

Multivalent batteries are a promising new technology for energy storage, but they face challenges to developing suitable electrolytes that can support reversible deposition/dissolution at the metal anode and enable compatibility with high voltage oxide cathode materials. Here, in this work, we investigate the solvation behavior of Zn 2+ , Mg 2+ , Ca 2+ and Cu 2+ in mixed anion electrolytes containing TFSI - and Cl - . Raman and nuclear magnetic resonance spectroscopies are utilized to probe the bulk solvation structure of these electrolytes and demonstrate that mixed anion contact ion pairs (CIPs) are formed in all four systems, indicating this behavior is likely general to divalent cations. Furthermore, the relative population of mixed anion CIPs can be tuned by controlling the relative ratio of TFSI : Cl, with significant CIP populations observed even at low relative fractions of Cl - . These findings imply that modifying the anion chemistry can easily adjust the solvation structure of bulk cations, which has important implications for the development of next-generation electrolytes. By understanding the factors that influence the formation of mixed anion CIPs, we can design systems that promote the formation of electrochemically-active solvation structures that can enable multivalent batteries with improved performance and lifetimes.

25 ENERGY STORAGE↗

Decoupling electrode kinetics to elucidate reaction mechanisms in alkaline water electrolysis

Alkaline water electrolysis (AWE) presents key advantages, including reduced material costs, enhanced operational stability, and compatibility with non-precious metal catalysts, positioning it as a scalable route for hydrogen production. In this study, we introduce a minimally invasive single-cell configuration incorporating a reference electrode via diaphragm extension to form an internal ion channel. This setup, combined with an interfaced potentiostat and auxiliary electrometer, enables real-time, independent monitoring of anode and cathode behavior, offering high-resolution electrochemical diagnostics. While it is well established that the hydrogen evolution reaction (HER) exhibits sluggish kinetics in alkaline media, our study reveals that this limitation persists even in practical AWE systems where nickel-based substrates are used as electrodes. This observation is supported by both experimental data and voltage breakdown modeling. Arrhenius-type analysis reveals that localized electric fields induced by catalysts shift the reaction kinetics from classical Butler–Volmer behavior toward a Marcus-like regime, where interfacial molecular dynamics and bimolecular charge transfer dominate. We propose a semi-empirical model and a surficial reaction mechanism to describe these dynamics. This work underscores the critical need for cathode innovation and provides a rational framework for designing advanced catalysts and electrode architectures to optimize AWE performance.

08 HYDROGEN↗

Versatile acid solvents for pristine carbon nanotube assembly

Chlorosulfonic acid and oleum are ideal solvents for enabling the transformation of disordered carbon nanotubes (CNTs) into precise and highly functional morphologies. Currently, processing these solvents using extrusion techniques presents complications due to chemical compatibility, which constrain equipment and substrate material options. Here, we present a novel acid solvent system based on methanesulfonic or p-toluenesulfonic acids with low corrosivity, which form true solutions of CNTs at concentrations as high as 10 g/liter (≈0.7 volume %). The versatility of this solvent system is demonstrated by drop-in application to conventional manufacturing processes such as slot die coating, solution spinning continuous fibers, and 3D printing aerogels. Through continuous slot coating, we achieve state-of-the-art optoelectronic performance (83.6 %T and 14 ohm/sq) at industrially relevant production speeds. This work establishes practical and efficient means for scalable processing of CNT into advanced materials with properties suitable for a wide range of applications.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

LAW Glass Formulation to Support Melter Runs with Simulants

The major objective of this work was to prepare and characterize glass formulations in order to develop and select formulations that are compliant with contractual and processing requirements to support melter tests with each of the LAW Sub-Envelopes. Glasses that cover composition ranges of interest were prepared and characterized to ensure that selected glass compositions can tolerate expected composition variations resulting from process errors without adversely affecting processing characteristics or product quality. Glass compositions that are expected to result during transitions from one waste stream to another were also prepared and characterized. Other objectives of the work included preparation and characterization of glasses with respect to the properties of interest, optimization of sulfate loading in the glasses, evaluation of ability to achieve waste loading limits, testing to demonstrate compatibility of glass melts with melter materials of construction, and identification of glass formulation issues with respect to contract specifications and processing requirements.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Experimental Operation of a Prototype 750C Advanced Chloride Molten Salt Bellows Valve

To achieve DOE 2030 SunShot targets that reduce the cost of liquid-based solar by an additional 40% to 70% beyond 2018 costs, a more reliable, highly manufacturable flow valve, capable of achieving operational temperatures of >700°C is required [1]. This paper investigates the development of an innovative high-temperature chloride molten salt valve, with operation up to 750°C. This valve is intended to be employed within Gen 3 CSP liquid-based thermal energy storage (TES) systems as well as Gen 4 modular salt reactor (MSR) technologies. This work details the general design and flow testing of a bellows-seal flow control valve (FCV). This design includes an integrated closed-loop thermal control system to ensure robust design for freeze-thaw cycles. The self-contained thermal management STM system, is unique in the salt valve industry since it is an integrated solution to provide a consistent, repeatable alternative to typical heat tracing. Additionally, the design includes the employment of a novel heat pipe valve stem to facilitate enhanced passive thermal management into the valve assembly. This valve stem heat pipe is designed to facilitate natural circulation within the bonnet to ensure robust operation, during both nominal and transient thermal operation. The valve body and trim will be designed using SS316H, consistent with Flowserve Corporation’s existing product base and is code qualified but will utilize clad material for materials corrosion, manufacturing cost reduction and compatibility to ensure design flexibility. A test campaign was performed in this investigation utilizing a novel 750°C ternary chloride (20%NaCl/40%MgCl2/40%KCl by mol. wt. %) molten salt flow loop. A discussion about the design and installation of the valves within this test bed is provided for this investigation. Valve test results from this study assessed Cv curves as well as multiple actuator cycles, under varying thermodynamic and operational mode conditions, which would be characteristic within a commercial molten salt facility. The results indicate nominal operation for the baseline design, though improved performance and reliability is expected with the full designed FCV.

Armijo, Kenneth (ORCID:0000000346832147)↗

Colloidal Semiconductor Nanocrystal Lasers and Laser Diodes

Lasers and optical amplifiers based on solution-processable materials have been long-desired devices for their compatibility with virtually any substrate, scalability, and ease of integration with on-chip photonics and electronics. These devices have been pursued across a wide range of materials including polymers, small molecules, perovskites, and chemically prepared colloidal semiconductor nanocrystals, also commonly referred to as colloidal quantum dots. The latter materials are especially attractive for implementing optical-gain media as in addition to being compatible with inexpensive and easily scalable chemical techniques, they offer multiple advantages derived from a zero-dimensional character of their electronic states. These include a size-tunable emission wavelength, low optical gain thresholds, and weak sensitivity of lasing characteristics to variations in temperature. Here we review the status of colloidal nanocrystal lasing devices, most recent advances in this field, outstanding challenges, and the ongoing progress toward technological viable devices including colloidal quantum dot laser diodes.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Scalable slot-die coating of phyllosilicate membranes for selective ion separations

Abstract Two-dimensional (2D) materials have recently drawn attention as candidate materials for molecular-scale membrane separations due to their tunable nanoscale interlayer properties. Phyllosilicates, a broad class of naturally abundant 2D clay minerals, offer significant advantages over synthetic 2D materials, including low cost, stability, and environmental compatibility. While these properties make phyllosilicates attractive for industrial-scale nanofiltration applications, phyllosilicate-based membranes have, to date, only been fabricated at the lab scale via vacuum filtration. Scalable fabrication methods are essential to advance the technical maturity of phyllosilicate membranes and bring these promising materials closer to large-scale adoption. Herein, we have successfully scaled up phyllosilicate (vermiculite) membrane fabrication via slot-die coating and roll-to-roll coating of an ethylenediamine–vermiculite (EDAVM) mixture onto nylon. The coated membranes are 1–2 μm $ \unicode{x03BC} \mathrm{m} $ mu m in thickness and exhibit similar structure and performance to vacuum-filtered EDAVM membranes. The membranes also show selectivity for monovalent ions over multivalent ions in binary salt mixtures. This work represents a major step toward scaling up phyllosilicate membranes for industrial ion separation applications such as resource recovery from water.

Booth, Austin [Princeton University]↗

Solar Steam on Demand

INTRODUCTION: This Report summarizes the research and development project performed by Sunvapor and the subrecipient National Renewable Energy Laboratory (NREL) during the period of 10/01/2018-9/30/2021. The work was aimed at the economic integration of solar steam with an industrial process, and in particular, the advantages that a novel type of thermal energy storage and collector design could bring to the system. The completed work includes experimental research on the storage material, design of the collector, engineering of a complete solar steam plant, and economic analysis. The plant was, in the end, not constructed, due to COVID-19 impacts to the project host. PURPOSE: The purpose of the project was to test the hypothesis that a levelized cost of heat (LCOH) of 2¢/kWh delivered to a steam-consuming process, including energy discharged from storage, could be feasibly achieved. PROJECT OBJECTIVES: For Budget Period 1 our objectives were to engineer a prototype industrial solar steam generation system, and design and test a Latent Heat Energy Storage (LHES) lab-scale system. For Budget Period 2 our objectives were to construct and test the solar steam prototype plant, and to build and factory-test a full LHES module. For Budget Period 3 our objective was to integrate the storage module with the solar steam generator, show successful long duration energy tests of the combined system, and use the results to project the LCOH of delivered steam to a second-generation plant. PROJECT OUTCOMES: Various phase change materials (PCMs) for the LHES were tested for compatibility with industrial steam uses as measured by phase change temperature, stability of latent heat of fusion, and their corrosive effects on steel (the heat exchanger material). Two of these materials (sodium formate and sodium/ potassium) showed potential to meet the technical criteria. The estimated cost of a complete LHES module with these materials did not meet economic targets. The developmental collector design builds from previous work to exploit the potential cost advantages of a spaceframe of lumber construction. Design improvements were achieved in assembly efficiency and structural performance. A complete engineering package was completed for the solar steam system without storage that included the developmental as well as commercial arrays. The plant was permitted for construction. The storage CAPEX for a reference plant was estimate to be greater than $\$ 57$/kWh. The LCOH of the system without storage and with developmental collectors of lumber construction was projected to be 2¢/kWh, assuming a FCR of 8.2% over thirty years. PROJECT MILESTONES: The Milestones fully achieved in the first Budget Period includes obtaining a Letter of Intent from an industrial steam-consuming project host, issuance of a construction permit, and corrosion resistance. The Milestone that was partly achieved was the degradation in the latent heat of fusion. Milestones associated with Budget Periods 2 and 3, related to the construction and operation of the plant were not achieved as a result of the host shutting down the plant due to COVID-19 impacts. CONCLUSIONS: Sunvapor was able to secure an agreement with a host to build a fully engineered and permitted solar steam plant that met the host’s economic goals. As a basis for comparison, the solar field design was comprised of eight commercial collector arrays and one developmental Green Parabolic Trough Collector (GPTC) array. The projected LCOH with a solar field entirely populated with a second generation GPTC met the goal of 2¢/kWh. The experimental program concerning the PCM indicated the feasibility of meeting their technical requirements for industrial steam uses. The cost of the complete LHES exceeded its $\$ 14$/kWh target, and therefore the inclusion of LHES could not be economically justified. Due to COVID-19 impacts on the host, the solar steam plant was not constructed.

14 SOLAR ENERGY↗