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At least 469 records · Page 26

Phase Stability Through Machine Learning

Understanding the phase stability of a chemical system constitutes the foundation of materials science. Knowledge of the equilibrium state of a system under arbitrary thermodynamic conditions provides valuable information about the types of phases that are likely to be synthesized and how to get there. Accessing the phase diagram in a materials system provides one with the information necessary to design materials and microstructures with optimal properties. While the materials science community has long been focused on exploiting this knowledge to navigate the materials space, recent advances in machine learning (ML) and artificial intelligence (AI) have provided the community with novel ways of interrogating the materials thermodynamics space. Furthermore, this work presents some of the most recent advances in ML/AI applied to phase stability and thermodynamics of materials. Prof. John Morral always had a passion for understanding and teaching the fundamental characteristics of phase diagrams. This review is written to honor his memory.

36 MATERIALS SCIENCE↗

Relationship between Sodium Content and Copper Activity for High Voltage Stability in O3-Type Layered Oxide Cathodes

Layered oxides with an O3 framework have attracted attention as cathode materials for sodium-ion batteries due to their high discharge capacity. Yet they are hampered for commercialization by poor cyclability due to structural instability during the sodium (de)intercalation process. The introduction of Cu in small fractions to the transition metal layers has been empirically observed to improve reversible specific capacity and cycling stability. Understanding the redox activity of Cu in O3-type Na x TMO 2 materials is crucial, as it could directly influence the charge compensation mechanism, voltage profile, and structural stability. However, the precise role of Cu in O3-type sodium cathodes under high-voltage cycling conditions (>4.1 V) remains insufficiently understood. To close this gap of knowledge, we studied the effect of Cu in two representative layered oxides with the same O3 stacking but different sodium stoichiometry, Na 0.9 Mn 1/2 Fe 1/3 Cu 1/6 O 2 and NaMn 1/2 Fe 1/3 Cu 1/6 O 2 . X-ray spectroscopy reveals that in Na 0.9 Mn 1/2 Fe 1/3 Cu 1/6 O 2 , Cu exhibits dual redox activity, Cu + /Cu 2+ in the pristine state and Cu 2+ /Cu 3+ upon charging in the sodium-deficient material, whereas only the Cu + /Cu 2+ redox couple is observed in the fully stoichiometric layered oxide. Furthermore, the results indicate that even a slight deficiency in sodium can significantly impact the electrochemical performance and material stability and alter the elemental redox activity of Cu.

Batteries↗

Mitigation of Dielectric Heating of Piezoelectric Actuators at Cryogenic Temperatures

The new generation of low beam intensity superconducting linacs will require high accelerating gradients for new scientific discoveries. The high accelerating gradient cavities in pulsed SRF linacs will experience large (~1000’s of Hz) detuning caused by Lorentz force detuning (LFD). The piezo actuators that will be used to compensate large LFD must operate at a nominal voltage of 120V to 150V to deliver the required stroke to the cavity. In this high voltage range, the piezo is expected to warm up drastically due to its location in an insulating vacuum environment. Overheating of the piezo will significantly decrease the longevity of the actuator. A collaboration between FNAL and Physik Instrumente (PI) developed a novel piezo actuator design that mitigates piezo overheating. The design consists of using a metal foam in contact with the piezoelectric ceramic stack for heat removal. The second solution used lithium niobite as an alternative material. A comparison of the temperature stability will be presented and discussed. This study characterizes the dielectric properties for both materials. The results obtained are in the temperature range of 10 K to 300 K.

43 PARTICLE ACCELERATORS↗

Increasing the Lifetime of Epoxy Components with Antioxidant Stabilizers

Epoxy thermoset resins are ubiquitous materials with extensive applications where they are used as encapsulants, composites, and adhesives/staking compounds used to secure sensitive components. Epoxy resins are inherently sensitive to thermo-oxidative aging, especially at elevated temperatures, which changes the bulk properties of the material and can lead to component failure for example by cracking due to embrittlement or by adhesion failure between the epoxy and filler material in a composite. This project investigated the effects of three commercial antioxidants (Irganox ® 1010 (I-102), butylated hydroxytoluene (BHT), or Chisorb ® 770 (HALS)) at two different loadings (2.5 and 5 wt%) on the mechanical and chemical aging of a model epoxy system (EPON TM 828 / Jeffamine ® T-403) under ambient conditions, 65, 95, and 110 °C. Additionally, synthetic routes towards an antioxidant capable of being covalently bound to the resin so as to prevent leaching were explored with one such molecule being successfully synthesized and purified. One commercial antioxidant (Irganox ® 1010) was found to reduce the degree of thermo-oxidatively induced damage in the system.

36 MATERIALS SCIENCE↗

A cost-effective all-in-one halide material for all-solid-state batteries

All-solid-state batteries require advanced cathode designs to realize their potential for high energy density and economic viability. Integrated all-in-one cathodes, which eliminate inactive conductive additives and heterogeneous interfaces, hold promise for substantial energy and stability gains but are hindered by materials lacking sufficient Li + /e − conductivity, mechanical robustness and structural stability. Here, in this work, we present Li 1.3 Fe 1.2 Cl 4 , a cost-effective halide material that overcomes these challenges. Leveraging reversible Fe 2+ /Fe 3+ redox and rapid Li + /e − transport within its framework, Li 1.3 Fe 1.2 Cl 4 achieves an electrode energy density of 529.3 Wh kg −1 versus Li + /Li. Critically, Li 1.3 Fe 1.2 Cl 4 shows unique dynamic properties during cycling, including reversible local Fe migration and a brittle-to-ductile transition that confers self-healing behaviour. This enables exceptional cycling stability, maintaining 90% capacity retention for 3,000 cycles at a rate of 5 C. Integration of Li 1.3 Fe 1.2 Cl 4 with a nickel-rich layered oxide further increases the energy density to 725.6 Wh kg −1 . By harnessing the advantageous dynamic mechanical and diffusion properties of all-in-one halides, this work establishes all-in-one halides as an avenue for energy-dense, durable cathodes in next-generation all-solid-state batteries.

25 ENERGY STORAGE↗

Chiral Spin Textures in Amorphous Iron–Germanium Thick Films

Topological solitary fields, such as magnetic and polar skyrmions, are envisioned to revolutionize microelectronics. These configurations have been stabilized in solid-state materials with a global inversion symmetry breaking, which translates in magnetic materials into a vector spin exchange known as the Dzyaloshinskii-Moriya interaction (DMI), as well as spin chirality selection and isotropic solitons. This work reports experimental evidence of 3D chiral spin textures, such as helical spins and skyrmions with different chirality and topological charge, stabilized in amorphous Fe-Ge thick films. Overall, these results demonstrate that structurally and chemically disordered materials with a random DMI can resemble inversion symmetry broken systems with similar magnetic properties, moments, and states. Disordered systems are distinguished from systems with global inversion symmetry breaking by their degenerate spin chirality that allows for forming isotropic and anisotropic topological spin textures at remanence, while offering greater flexibility in materials synthesis, voltage, and strain manipulation.

36 MATERIALS SCIENCE↗

Structural Stability of Tin-Lead Halide Perovskite Solar Cells

One of the key features that makes halide perovskite solar cells such an attractive and intensely researched photovoltaic (PV) technology, is the tunability of the bandgap of these halide perovskite materials [1], [2]. Shortly after it was established that the bandgap could be increased to 1.7-1.8 eV, investigations into the application for silicon based tandem solar cells launched. Within a few years, conversion efficiencies of up to 28 % have been reported [3]. Concurrently, the interest in commercial application of this technology emerged and have rapidly increased. Whereas there are advantages to piggy backing on an established PV technology such as silicon, efforts to develop all-perovskite tandem solar cells are of considerable interest. Partly substituting the metal cation in the ABX3 perovskite enables the low bandgap absorbers required for an all-perovskite tandem solar cell. One common approach is to partially substitute the lead with tin, however these materials often suffered from poor stability. Therefore the development of an efficient, stable mixed tin-lead perovskite is key to enabling all-perovskite tandem solar cells.

degradation↗

Computational Analysis of the Energetic Stability of High-Entropy Structures of a Prototypical Lanthanide-Based Metal–Organic Framework

High-entropy materials are characterized by their complex compositions, typically comprising five or more elements in near-equiatomic proportions. Applying this concept to metal ions in metal−organic frameworks (MOFs) has paved the way for exploring a new class of high-entropy MOFs. While the compositional strategy of high-entropy materials leverages configurational entropy to aid thermodynamic stability, it also poses significant analytical challenges due to the vast compositional landscape and diverse phases that these materials can adopt. We present a computational study of several complexities associated with selecting potential high-entropy versions of a prototype lanthanidebased MOF. We compute the energetics of metal mixing of these heterometallic MOFs using density functional theory (DFT) and machine learning interatomic potential (MLIP) methods. The use of MLIP methods allows a systematic exploration of the convex hull of thermodynamically stable MOF structures containing up to 5 distinct metals.

Chemical structure↗

Iridium metallene oxide for acidic oxygen evolution catalysis

Exploring new materials is essential in the field of material science. Especially, searching for optimal materials with utmost atomic utilization, ideal activities and desirable stability for catalytic applications requires smart design of materials’ structures. Herein, we report iridium metallene oxide: 1 T phase-iridium dioxide (IrO 2 ) by a synthetic strategy combining mechanochemistry and thermal treatment in a strong alkaline medium. This material demonstrates high activity for oxygen evolution reaction with a low overpotential of 197 millivolt in acidic electrolyte at 10 milliamperes per geometric square centimeter (mA cm geo –2 ). Together, it achieves high turnover frequencies of 4.2 s UPD –1 (3.0 s BET –1 ) at 1.50 V vs. reversible hydrogen electrode. Furthermore, 1T-IrO 2 also shows little degradation after 126 hours chronopotentiometry measurement under the high current density of 250 mA cm geo –2 in proton exchange membrane device. Theoretical calculations reveal that the active site of Ir in 1T-IrO 2 provides an optimal free energy uphill in *OH formation, leading to the enhanced performance. The discovery of this 1T-metallene oxide material will provide new opportunities for catalysis and other applications.

36 MATERIALS SCIENCE↗

Combining artificial intelligence and physics-based modeling to directly assess atomic site stabilities: from sub-nanometer clusters to extended surfaces

The performance of functional materials is dictated by chemical and structural properties of individual atomic sites. In catalysts, for instance, the thermodynamic stability of constituting atomic sites is a key descriptor from which more complex properties, such as molecular adsorption energies and reaction rates, can be derived. In this study, we present a widely applicable machine learning (ML) approach to instantaneously compute the stability of individual atomic sites in structurally and electronically complex nano-materials. Conventionally, we determine such site stabilities using computationally intensive first-principles calculations. With our approach, we predict the stability of atomic sites in sub-nanometer metal clusters of 3–55 atoms with mean absolute errors in the range of 0.11–0.14 eV. To extract physical insights from the ML model, we introduce a genetic algorithm (GA) for feature selection. This algorithm distills the key structural and chemical properties governing the stability of atomic sites in size-selected nanoparticles, allowing for physical interpretability of the models and revealing structure–property relationships. The results of the GA are generally model and materials specific. In the limit of large nanoparticles, the GA identifies features consistent with physics-based models for metal–metal interactions. By combining the ML model with the physics-based model, we predict atomic site stabilities in real time for structures ranging from sub-nanometer metal clusters (3–55 atom) to larger nanoparticles (147 to 309 atoms) to extended surfaces using a physically interpretable framework. Finally, we present a proof of principle showcasing how our approach can determine stable and active nanocatalysts across a generic materials space of structure and composition.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Impact of Humidity and Temperature on the Stability of the Optical Properties and Structure of MAPbI3, MA0.7FA0.3PbI3 and (FAPbI3)0.95(MAPbBr3)0.05 Perovskite Thin Films

In situ real-time spectroscopic ellipsometry (RTSE) measurements have been conducted on MAPbI3, MA0.7FA0.3PbI3, and (FAPbI3)0.95(MAPbBr3)0.05 perovskite thin films when exposed to different levels of relative humidity at given temperatures over time. Analysis of RTSE measurements track changes in the complex dielectric function spectra and structure, which indicate variations in stability influenced by the underlying material, preparation method, and perovskite composition. MAPbI3 and MA0.7FA0.3PbI3 films deposited on commercial fluorine-doped tin oxide coated glass are more stable than corresponding films deposited on soda lime glass directly. (FAPbI3)0.95(MAPbBr3)0.05 films on soda lime glass showed improved stability over the other compositions regardless of the substrate, and this is attributed to the preparation method as well as the final composition.

36 MATERIALS SCIENCE↗

Reducing Mass of Steel Auto Bodies using Thin Advanced High Strength Steel with Carbon-Fiber Reinforced Epoxy

Diversitak, a company based in Detroit, MI, has developed a proprietary, low specific gravity, carbon fiber-reinforced epoxy (CFRE) under U.S. patent number 9,963,58832. Preliminary testing on this new material conducted in collaboration with ArcelorMittal Steel Company proved out the CFRE concept. A thin layer of this CFRE was applied to a stamped sheet of steel with residual stamping oils from a mill, in a time corresponding to automotive processing (e.g., ~15 seconds), and processed following automotive e-coat procedures (phosphating + 175–200°C heating), to complete the curing. No problems with adherence or performance were noted. While the CFRE does add weight to a thin gauge steel panel, it weighs much less than what is displaced by using thicker conventional mild steel gauges. The application of the coating showed a significant increased dent resistance, oil canning resistance, and part stiffness.This current two-year project was designed to mature this new technology to near manufacturing readiness to reduce the weight of a vehicle and lower the cost of weight reduction. The process involves the use of thinner gauge steels than are currently used. The collaborative development team included two industrial manufacturers: Diversitak and ArcelorMittal Steel Company; LightMAT; and two National Laboratories: Oak Ridge National Laboratory (ORNL) and Idaho National Laboratory (INL). The team developed a new manufacturing process to reduce the weight of a vehicle and lower the cost of weight reduction, as well as a better understanding of how to apply the coating so that it will perform to a high standard in-service. The team also performed an in-depth study to determine the long-term durability of the materials manufactured using this technology and well-known automotive industry standard tests.The overall process involved stiffening the thinner gauge steel by applying the CFRE on only one side. To accomplish this goal, the optimal reinforcement fiber length and fiber concentration was first determined. This was followed by measuring the coefficient of thermal expansion (CTE) in all three directions, so it could be fed into manufacturing models and methods for rapidly and inexpensively applying the coating. This was followed by panel level evaluations of the coating and steel combination, and then by full part demonstration of the technology on door panels. The final step was corrosion testing of the parts.ArcelorMittal characterized the advanced high strength steel (AHSS) (e.g., metallurgy-heat treatment for required AHSS properties as a function of the sheet thickness, state of internal stress) and quantified CFRE adhesion to the steel as a function of sheet preparation (e.g., rolling and stamping).ORNL optimized the fiber length, fiber concentration, and coating thickness for best vehicle function and performance at the least cost. Along with the suppliers, ORNL developed a durable CFRE application process (e.g., gun material, design, robotic dispensing process) and identified the adhesion stability of the CFRE during process holding. An approach to ensure that application/curing timing conforms to conventional assembly line speed and plant cycle times was determined. ORNL also determined the CTE of the material in all three directions and performed material scanning electron microscopy (SEM) analyses.INL characterized the corrosion properties of the steel panels coated with CFRE. The panels were investigated for corrosion resistance and stability as replacement materials used in automotive body panels to reduce mass. The coupons tested at INL were supplied by Diversitak after an optimized CFRE formulation was achieved in the already coated form for corrosion testing.

99 GENERAL AND MISCELLANEOUS↗

Synthetic accessibility and stability rules of NASICONs

In this paper we develop the stability rules for NASICON-structured materials, as an example of compounds with complex bond topology and composition. By first-principles high-throughput computation of 3881 potential NASICON phases, we have developed guiding stability rules of NASICON and validated the ab initio predictive capability through the synthesis of six attempted materials, five of which were successful. A simple two-dimensional descriptor for predicting NASICON stability was extracted with sure independence screening and machine learned ranking, which classifies NASICON phases in terms of their synthetic accessibility. This machine-learned tolerance factor is based on the Na content, elemental radii and electronegativities, and the Madelung energy and can offer reasonable accuracy for separating stable and unstable NASICONs. This work will not only provide tools to understand the synthetic accessibility of NASICON-type materials, but also demonstrates an efficient paradigm for discovering new materials with complicated composition and atomic structure.

25 ENERGY STORAGE↗

Nanographene Coupled with Interfacial Pyrene Derivatives for Thermally Stable Perovskite Solar Cells

Although high-efficiency perovskite solar cells (PSCs) have been achieved using a hole-extracting material, spiro-MeOTAD, thermal stability has been unattainable due to the low glass transition temperature of spiro-MeOTAD and additives therein. In this paper we report on the use of nanographene-based hole-transporting materials coupled with a pyrene derivative as an interface modifier for thermally stable and high efficiency PSCs. Asymmetric methyl and methoxy groups are introduced in the diphenylamino group that is attached to the hexa-peri-hexabenzocoronene (HBC) nanographene core, coded HBC-DPAMeOMe. 1-Pyrenemethylammonium iodide is coupled to enhance the chemical interaction between perovskite and HBC-DPAMeOMe, which leads to a power conversion efficiency over 23%. A thermal stability test at 85 degrees C for 1000 h reveals that 83.6% of the initial efficiency (23.04% --> 19.25%) is maintained for the device with HBC-DPAMeOMe, while a significant degradation from 20.69% to 5.08% is observed for the device with spiro-MeOTAD. Nanographene-based hole conductors shed light on the thermal stability issue in PSCs.

14 SOLAR ENERGY↗

Knowledge gaps for neuromorphic ionic computing

BACKGROUND Neuromorphic computing, inspired by the human brain’s ability to process information efficiently, represents a transformative approach to computation. In this Review, we explore the emerging field of neuromorphic ionic computing, which leverages ionic conduction and coupling to mimic neural processes, and identify critical knowledge gaps that must be addressed to realize its full potential. A central theme of the discussion is energy efficiency, a challenge that is both a limitation and an opportunity for this technology. Although complementary metal-oxide semiconductor (CMOS)–based neuromorphic technologies have made strides in scaling to billions of neurons and are increasingly applied in artificial intelligence and numerical computing, they remain orders of magnitude behind the human brain in terms of connectivity and energy efficiency. Neuromorphic ionic computing promises to overcome these limitations by leveraging the distinct architectural and operational principles of the brain. Our brains achieve this energy efficiency by combining several key features: using the same network elements to store and process information; using an incredibly complex and massively interconnected three-dimensional (3D) network of locally active elements that enables sparsity, robustness in the presence of noise, adaptation, and life-long learning; computing at comparatively low voltage and frequency; and last, taking advantage of a plethora of ions and small molecules as information carriers. Here, we propose that ionic computing systems can take advantage of similar features to achieve substantial gains in energy efficiency. ADVANCES Since the first reports of neuromorphic ionic behavior in nanofluidic channels, we have witnessed an explosion of reports that used ionic devices to produce synaptomimetic behaviors. However, achieving the goals of ionic computing requires not only implementation of much more sophisticated device functionality but also overcoming fundamental barriers in materials science, device architecture, and system integration. Current ionic devices, even those incorporating state-of-the-art materials, still suffer from limited functionality and stability, which restrict their performance and increase energy demands. Developing new materials with enhanced ionic properties is essential to overcome these limitations. Similarly, the design of neuromorphic devices must evolve to leverage the particular advantages of ionic processes. Existing architectures often follow a single-information-carrier logic of conventional electronics or are constructed of mesoscale fluidics, failing to capitalize on the energy-efficient mechanisms inherent to ionic systems or implement the multiple-information-carrier paradigm. Current neuromorphic chips focus on large-scale networks of analog memory elements based on mechanisms such as charge trap (flash), filamentary, phase change, or spin, which are built on top of a network of artificial CMOS neurons. Although such prototype networks have achieved impressive performance, it is difficult to envision how they can implement the key features such as massive connectivity, sophisticated plasticity, adaptability, sparsity, and “multichromatic” computing. Although small-scale devices have demonstrated promising results, integrating them, maintaining energy efficiency, and implementing temperature control as systems grow in complexity and size to computationally relevant scale remain major hurdles. Furthermore, interfacing neuromorphic ionic devices with existing computing technologies presents technical and conceptual challenges that will require innovative approaches that combine insights from neuroscience, materials science, and engineering. OUTLOOK Despite these challenges, the potential impact of neuromorphic ionic computing is profound with potential applications ranging from artificial intelligence to robotics and beyond. We also argue that neuromorphic ionic computing systems should not, at least in the beginning, compete with CMOS technologies but rather should focus on applications that require extreme energy efficiency with chemical and/or biological compatibility, such as biomedical applications (for example, brain-computer interfaces), environmental monitoring, and agricultural and food applications. Ultimately, this Review highlights the crucial role of interdisciplinary collaboration in advancing the field. Neuromorphic ionic computing is not merely a technological innovation; it represents a substantial step toward sustainable computation, aligning with the growing demand for energy-conscious solutions in a world that is increasingly reliant on data and computation.

Neuromorphic↗

High-Performance Coal-Based Commercial Facade Panels and Architectural Components (Phase I Final Report)

Semplastics has developed, tested, and documented the viability for commercialization of a new class of composite architectural panel materials that use coal as the primary constituent. This project produced sample panels using these novel materials that comprise 55% coal by mass (71% carbon by mass) and are comparable in dimensions to commercially available materials, while displaying superior mechanical strength, significant weight savings, and better insulating ability at a competitive cost. Phase I moved this coal-based composite materials technology from a Technology Readiness Level (TRL) of 3 to TRL 5. Semplastics’ new coal-based composite materials display an array of high-performance characteristics, including light weight, mechanical durability, temperature stability, and water resistance. These new materials require less energy to produce than comparable commercial products and could be manufactured on existing conventional plastic resin processing equipment in commercial quantities. The coal particles are completely encapsulated in ceramic from a polymer-derived ceramic (PDC) precursor, then bonded together by another inorganic resin. The material can be molded and cured to produce fireproof components such as ceiling panels, facades, and extruded underlayment, blocking, and backer boards, as well as other architectural design components such as moldings. The project included the production of sample panels for proof of concept, testing of the panels to show their improved characteristics, and development of a scale-up strategy to demonstrate the viability of the coal-based panels as a commercial alternative to existing building materials.

36 MATERIALS SCIENCE↗

Stromataxic Stabilization of a Metastable Layered ScFeO3 Polymorph

Metastable polymorphs--materials with the same stoichiometry as the ground state but a different crystal structure--enable many critical technologies. This work describes the development of a stabilization approach for metastable polymorphs that are difficult to achieve through other stabilization techniques (such as epitaxy or quenching) called stromataxy. Stromataxy is a method based on controlling the precursor structure during the initial stages of material growth to dictate phase formation. To illustrate this approach, we controlled the atomic layering of the precursors of ScFeO3 and stabilized the metastable P63cm phase, under conditions that previously led to the ground-state Ia3¯ bixbyite phase. Ab initio mechanistic calculations highlight the importance of the variable oxidation state of Fe and the layer stability during layer-by-layer growth. The broad applicability of a stromataxy approach was demonstrated by stabilizing this metastable phase on substrates that have previously been shown to stabilize other polymorphs under continuous growth. Stromataxy is shown as a viable option for accessing polymorphs that are close in energy, difficult to differentiate by strain, or that lack a well epitaxially matched substrate.

calculations↗

Development of direct ink write radially graded alumina/zirconia

Functionally graded materials (FGMs) are of interest in multiple fields, yet many materials combinations are limited by coefficient of thermal expansion (CTE) mismatch. Here, a radially graded alumina/yttria-doped zirconia (Al 2 O 3 /8YZ) FGM is used to demonstrate processing strategies to mitigate CTE and sintering behavior differences between these oxides. FGM materials are especially sensitive to ink stability during printing, as all components (in this case, Al 2 O 3 and 8YZ) must be stabilized in the same dispersant or additive solution. Thus, this system is also ideal to demonstrate ink optimization best practices. Materials were characterized throughout processing to correlate the effects of common additives on both the ceramic particle suspensions and final sintered components. Aggregation observed in the initial additive-containing suspensions were present in the sintered component. The differences in sintering onset temperature and shrinkage rate resulted in internal stresses within the sintered component, which ultimately caused mechanical failure of the component under low stress. In conclusion, a processing strategy was recommended to mitigate the sintering behavior mismatch of alumina and 8 wt% yttria-stabilized zirconia.

Lamm, Benjamin W. [Oak Ridge National Laboratory (↗