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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 19 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2025

Dynamic separation of gases using microsieves

Separation of light weight molecules, such as nitrogen, argon, and oxygen, from heavier compounds can have significant impacts on energy capture, environmental monitoring, or isotopic applications. Large-scale gas separation techniques, like gas centrifugation and membrane mitigation, can be problematic as they impart tremendous energy and induce high mechanical stress onto the instrumentation. Microsieves, also known as micronozzles or microfunnels, are developed to create physical barriers to separate specific isotopes and gases. Separation is achieved using a converging and diverging micronozzle to impose supersonic gas flow around a curved wall, and it has been used for the separation of heavy actinide isotopes in low weight gas as well as separation of low weight gas compositions of nitrogen and argon back in 1900s. However, systematic reviews of this unique technology are lacking. The application of the Laval style nozzle, which has a converging/diverging entrance fundamental to the micronozzle, is included in this review due to its importance in industrial applications in uranium (U) isotope refinement. Using advanced computational fluid dynamic (CFD) simulations, the extent of gas separation can be modelled. Herein, we first examine the literature and survey recent advances on fabrication techniques for creating curved micronozzles, methods and separation principles used to design devices. Furthermore, we then follow with highlights of CFD simulations applied to evaluate the separation effects using microsieves. Finally, identification of the gap and recommendation for future development and applications are suggested for using intrinsic molecular features and fluidic dynamics in formulating separation strategies.

30 Microfluidics↗
DOE OSTI2024

An Adsorptive Membrane Platform for Precision Ion Separation: Membrane Design and First‐Principles Studies

One of the key challenges in separation science is the lack of precise ion separation methods and mechanistic understanding crucial for efficiently recovering critical materials from complex aqueous matrices. Herein, first-principles electronic structure calculations and in situ Raman spectroscopy are studied to elucidate the factors governing ion discrimination in an adsorptive membrane specifically designed for transition metal ion separation. Density functional theory calculations and in situ Raman data jointly reveal the thermodynamically favorable binding preferences and detailed adsorption mechanisms for competing ions. How membrane binding preferences correlate with the electronic properties of ligands is explored, such as orbital hybridization and electron localization. The findings underscore the importance of the phenolate group in oxime ligands for achieving high selectivity among competing transition metal ions. In-depth understanding on which specific atomistic site within the microenvironment of metal-ligand binding pockets governs the ion discrimination behaviors of the host will build a solid foundation to guide the rational design of next-generation materials for precision separation essential for energy technologies and environment remediation. In tandem, synthetic controllability is demonstrated to transform 3D micrometer-scale crystals to a 2D crystalline selective layer in membranes, paving the way for more precise and sustainable advances in separation science.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

SPIKANs: separable physics-informed Kolmogorov–Arnold networks

Physics-Informed Neural Networks (PINNs) have emerged as a promising method for solving partial differential equations (PDEs) in scientific computing. While PINNs typically use multilayer perceptrons (MLPs) as their underlying architecture, recent advancements have explored alternative neural network structures. One such innovation is the Kolmogorov–Arnold Network (KAN), which has demonstrated benefits over traditional MLPs, including faster neural scaling and better interpretability. The application of KANs to physics-informed learning has led to the development of Physics-Informed KANs (PIKANs), enabling the use of KANs to solve PDEs. However, despite their advantages, KANs often suffer from slower training speeds, particularly in higher-dimensional problems where the number of collocation points grows exponentially with the dimensionality of the system. To address this challenge, we introduce Separable Physics-Informed Kolmogorov–Arnold Networks (SPIKANs). This novel architecture applies the principle of separation of variables to PIKANs, decomposing the problem such that each dimension is handled by an individual KAN. This approach drastically reduces the computational complexity of training without sacrificing accuracy, facilitating their application to higher-dimensional PDEs. Through a series of benchmark problems, we demonstrate the effectiveness of SPIKANs, showcasing their superior scalability and performance compared to PIKANs and highlighting their potential for solving complex, high-dimensional PDEs in scientific computing.

Kolmogorov-Arnold networks↗
DOE OSTI2025

Multimetallic Layered Composites (MMLCs) for Rapid, Economical Advanced Reactor Deployment (Final Report)

This project focused on the development of multi-metallic layered composites (MMLCs) for advanced fission reactor technologies. There are many instances where one alloy or material simply cannot meet all the demands thrown at it by a reactor system, or cannot allow it to perform as strongly as one would like. Instead of focusing all our effort on developing one perfect alloy, we seek to leverage the design principle of “separation of functionality,” used in many other arenas in design, to boost performance beyond single alloys alone. One illustrative example shows the power of this approach for molten salt-cooled reactors: A three meter tall, three meter diameter reactor vessel made of Incoloy 800 was quoted at $\$$500k in 2018. A Hastelloy N vessel was quoted at $\$$5M. An MMLC vessel, in which a layer of Hastelloy N would be weld-overlaid onto Incoloy 800, was quoted at $\$$700k, and it would achieve the same performance. The potential economic gains of leveraging this approach are therefore substantial. At a minimum, each MMLC would contain one core structural layer and one coolant-facing corrosion-resistant layer. Sometimes, MMLCs required buffer layers, as the structural and corrosion-resistant layers were metallurgically incompatible. In other words, they didn’t always play nice, thus separating layers compatible with both functioned as intermediaries to keep the composite together. However, in doing so we inevitably produce new interfaces, where new issues can arise. Therefore, this project focused on what happens at these interfaces from a combination of high temperatures, irradiation, corrosion, and time. After all, a reactor makes money when it is operating, and outages of any kind erode its economic viability. First, we set out to experimentally prove that MMLCs for at least two advanced reactor systems can be made, today, in US domestic facilities. In this respect we were successful – one MMLC (a Ni-201/Incoloy 800H composite) was successfully made and drawn into two-inch coolant piping. Others were attempted, though new issues relating to cracking in vanadium layers for one and radiation damage performance of the corrosion-resistant layer in another prevented us from moving further in those specific arenas – these are engineering problems which deserve continued focus after this project. Additional experimental work focused on long-term corrosion testing of the outermost layers of the salt-cooled and liquid lead-cooled MMLC concepts, which would then be fed into predictions of how long the MMLCs could last. Next, computational (thermodynamics and atomistic) simulation studies studied how much we expect the interfaces to “blend,” due to the mixing action of neutron irradiation. This eats into both the margin for the structural layer of each MMLC, as dilution from the corrosion-resistant layer into the structural layer would decrease the total load-bearing capacity of an MMLC of finite size. On the other hand, dilution of the corrosion-resistant layer into the structural layer further reduced the margin of corrodible material, reducing the lifetime of the MMLC or necessitating extra thickness to be imparted to the MMLC to meet its functional requirements. Work here focused on irradiation-induced segregation to predict new phases which may embrittle the MMLCs, as well as quantifying irradiation-induced mixing at each interface. The results showed that mixing is expected, but it is both steady and therefore predictable, and not lifetime-limiting for most MMLC concepts – it simply has to be accounted for in calculations of reactor performance when utilizing an MMLC. Then, full-core simulations using the experimentally-derived corrosion data, the computationally discovered irradiation-induced mixing data (partially validated by experiment), and existing, benchmarked core designs for large and small sized reactor concepts (one salt-cooled, one lead-cooled) were conducted to quantify any expansion of reactor operating envelopes achieved by utilizing these MMLCs. This new framework, called REX (Reactor Envelope Expansion), incorporates a combination of core neutronics, thermal hydraulics, and the material performance data derived from this project to see how using an MMLC expands advanced fission reactor operating envelopes. It was discovered that in some cases, MMLC utilization does indeed increase the maximum operating temperatures and cycle lengths of reactor concepts, while in other cases it does not. Finally, our tech-to-market (T2M) strategy was not necessarily to create specific embodiments of MMLCs for immediate sale (because getting into the nuclear market is incredibly slow and laden with regulation, this is a long-term goal), but rather immediate stimulation of US industry using the design approach of MMLCs derived from this project. In this respect we were successful, as one of the PhD students funded on this project co-founded Allium Engineering, Inc., which created a stainless steel / low-alloy steel MMLC to function as chloride corrosion-resistant rebar for embedding into concrete structures. Allium Engineering continues to be successful, having recently opened their first factory as of this writing.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2025

Numerical analysis of air dehumidification through electrospray-enhanced vortical flow cyclone separator

The dehumidification of air is a highly energy-intensive process, typically requiring vapor compression systems to cool the air significantly below its dew point temperature. Here, this study numerically investigates air dehumidification achieved by electrostatic and dielectrophoresis forces in a converging duct and centrifugal principles in cyclone separators. An electrospray was employed to energize water droplets, which then captured water vapor via dielectrophoresis. A novelty of the present study is the inclusion of a cyclone separator positioned downstream of the electrospray. This combination increased the dehumidification efficiency and controlled the flow of the condensate. By integrating electrospray technology and applying an electric field, this study examines the impact of particle separation efficiency, pressure drops, and cyclone performance on air dehumidification. The control parameters for air dehumidification were investigated. Three cyclones were modelled for airflow rates of 5 cubic feet per minute [cfm] (0.0024 m 3 /s), 38 cfm (0.0179 m 3 /s), and 200 cfm (0.094 m 3 /s). The results indicated air dehumidification was up to 5.7 % under environmental conditions, similar to those used to validate the CFD model. The degree of air dehumidification was primarily influenced by the electric charge acquired by the water droplets, their flight trajectory, and the vorticity intensity within the cyclone. Air dehumidification could increase by up to 13 % by increasing the number of droplets injected into the air stream, the flight time, and the electrical charge. The breakdown electric field strength threshold near the electrospray was a limiting factor for further enhancing dehumidification performance. This study examines the optimization of an electro-assisted dehumidification system that includes cyclone-based droplet separation through numerical analysis. The results provide insights into the design of energy-efficient air treatment technologies.

42 ENGINEERING↗
DOE OSTI2025

Separating Sensible and Latent Cooling with Electrically Charged Rotating Vortexes and Vapor Capturing Air Handler Technology

The dehumidification of air is a highly energy-intensive process, typically requiring vapor compression systems to cool the air below its dew point temperature. This project investigated air dehumidification achieved by electrostatic and dielectrophoresis forces in electrosprays and centrifugal principles in cyclone separators. As a practical implementation of these processes, Electrospray Vortical Flow eXchanger (EVFX) prototypes were designed, fabricated, and tested. Electrosprays were employed to energize water droplets, which then captured water vapor via dielectrophoresis. A cyclone separator was positioned downstream of the electrosprays. This combination increased the dehumidification efficiency and controlled the flow of the water vapor condensate removed from the air.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗
DOE OSTI2024

Recovery of Oxpure 612C-50 Coconut Carbon Particles Using Bump Arrays

Cyanide is used to leach gold from crushed ore (solid matrix) into a gold cyanide solution. The gold is extracted from the cyanide solution by adsorption onto activated carbon. The gold extraction process occurs when the activated coconut carbon is placed into tanks that contain the gold cyanide solution either in a batch process or into a continuous flow circuit. The coconut carbon is then removed from the solution for gold recovery. The use of the mesofluidic separation system (a deterministic lateral displacement system) can significantly reduce costs and waste generated from the process of removing the coconut carbon from the solution. In the coconut carbon recovery process used at many gold mines in Nevada, the gold is attached to carbon particles that are still in the cyanide liquor. The mesofluidic system can rapidly remove the gold bearing carbon particles from the cyanide liquor quickly and with no operating costs. The benefits include: • Reduce operational costs related to filtration and hydro-cyclones • Reduced acid usage for the elution gold stripping phase as only 25% of the fluids will follow the carbon particles to the final express lane when two mesofluidic systems are used in series This alternative particle removal techniques would be advantageous. A promising technique for removing larger particles from slurries is mesofluidic separation, similar to deterministic lateral displacement arrays or “bump” arrays [1] but operates at much larger flow rates. As described by Pease, et al. [2], “Bump arrays in deterministic lateral displacement devices separate large particles from small particles using arrays of staggered posts. Large particles, defined as those with radii larger than the distance between the edge of a post and the stagnation streamline from the next downstream post, must bump toward one side of the device, whereas particles smaller than this distance slalom from entrance to exit without net lateral displacement.” Unlike filters or sieves, the posts in the arrays that cause separation do not block or occlude particle flow but work because particles go around the posts. Unlike hydrocyclones separation, separation is not driven by particle density, because gravitational forces are unimportant to mesofluidic separation. Burns, et al., and Pease, et al., have shown that particles may be separated from complex suspensions, under turbulent flow conditions, and at industrially important flow rates [3-5]. They have also recently shown that mesofluidic devices may be arranged in series to increase separation performance [6]. In this paper, we evaluate the mesofluidic system for the separation of commercial OxPure GR 612 Charred Coconut shell particles as a proof of principle test for the rapid separation using the 1500 micron cut mesofluidic separator. We first describe the experimental system and conditions. We then present the experimental results. [1] Huang, L.R., E.C. Cox, R.H. Austin, J.C. Sturm. 2004. Continuous particle separation through deterministic lateral displacement. Science, 304, 987–990. https://doi.org/10.1126/science.1094567. [2] Pease L.F., J.A. Bamberger, C.A. Burns, and M.J. Minette. 2021. Large Particle Separation from Non-Newtonian Slurries using Bump Arrays. In Proceedings of the ASME 2021 Fluids Engineering Division Summer Meeting FEDSM2021-65904, V003T08A023. New York, New York: ASME. doi:10.1115/FEDSM2021-65904 [3] Burns C.A., T.G. Veldman, J. Serkowski, R.C. Daniel, X.-Y. Yu, M.J. Minette, L.F. Pease. 2021. Mesofluidic separation versus dead-end filtration. Separation and Purification Technology, 254, 117256. https://doi.org/10.1016/j.seppur.2020.117256. [4] Pease L.F., J.E. Serkowski, T.G. Veldman, J. Williams, X.-Y. Yu, M.J. Minette, J.A. Bamberger, C.A. Burns. 2021. Can Bump Arrays Separate Particles from Turbulent Flows?. In Proceedings of the ASME 2021 Fluids Engineering Division Summer Meeting FEDSM2021-67696, V003T08A024. New York, New York: ASME. doi:10.11

mesofluidic separation, slurry, bump array↗
DOE OSTI2024

Multiscale Normalizing Flows for Gauge Theories

Scale separation is an important physical principle that has previously enabled algorithmic advances such as multigrid solvers. Previous work on normalizing flows has been able to utilize scale separation in the context of scalar field theories, but the principle has been largely unexploited in the context of gauge theories. This work gives an overview of a new method for generating gauge fields using hierarchical normalizing flow models. This method builds gauge fields from the outside in, allowing different parts of the model to focus on different scales of the problem. Numerical results are presented for $U(1)$ and $SU(3)$ gauge theories in 2, 3, and 4 spacetime dimensions.

Abbott, Ryan↗
DOE OSTI2026

Tokamak Energy’s pre-concept design for a fusion power plant: an overview of ST-E1

Climate change and rapidly rising energy demand, driven in part by artificial intelligence and data-centre growth, create an urgent need for stable, low-carbon, and abundant power. Fusion is a promising long-term solution, yet its commercialisation faces a fundamental paradox in today’s investment environment: pilot plants are essential to de-risk physics, engineering, and operations, but their limited lifetime energy output and high upfront costs make them difficult to finance. This paper presents Tokamak Energy’s response: ST-E1, a pre-concept design for a low-aspect-ratio tokamak power plant engineered specifically to overcome this challenge. ST-E1 is designed from the outset for phased operation—pilot and commercial phases, with an upgrade phase in between—with emphasis on commercial viability, maintainability, nuclear engineering, modularity, and upgradability. A key design principle is the deliberate separation of long-lived assets, such as the magnet cage and vacuum vessel, from replaceable in-vessel systems. This provides an attractive and credible investment approach to generate operational data and de-risk key technologies while preserving most capital-intensive assets for later commercial phases. The architecture supports continuous optimisation toward high net electric power (targeting 800–1000 MW net electric), a normalised capital expenditure of $\$$ 12–14k/kW of net electric power, and high availability (targeting > 80%). A tokamak core with a 5 m major radius, aspect ratio of 2.3, and on-plasma axis toroidal field of 5.25 T was selected to meet these objectives. This paper summarises the ST-E1 design philosophy, principal features, and development methodology. It introduces a Focus Collection of 11 papers detailing the pre-concept design of the entire tokamak and corresponding plant.

ST-E1↗
DOE OSTI2024

Quantitative Predictive Theories through Integrating Quantum, Statistical, Equilibrium, and Nonequilibrium Thermodynamics

Today's thermodynamics is largely based on the combined law for equilibrium systems and statistical mechanics derived by Gibbs in 1873 and 1901, respectively, while irreversible thermodynamics for nonequilibrium systems resides essentially on the Onsager Theorem as a separate branch of thermodynamics developed in 1930s. Between them, quantum mechanics was invented and was quantitatively solved in terms of density functional theory (DFT) in 1960s. Furthermore, these three scientific domains operate based on different principles and are very much separated from each other. In analogy to the parable of the blind men and the elephant articulated by Perdew, they individually represent different portions of a complex system and thus are incomplete by themselves alone, resulting in the lack of quantitative agreement between their predictions and experimental observations. Over the last two decades, the author's group has developed a multiscale entropy approach (recently termed as zentropy theory) that integrates DFT-based quantum mechanics and Gibbs statistical mechanics and is capable of accurately predicting entropy and free energy of complex systems. Furthermore, in combination with the combined law for nonequilibrium systems developed by Hillert, the author developed the theory of cross phenomena beyond the phenomenological Onsager Theorem. The zentropy theory and theory of cross phenomena jointly provide quantitative predictive theories for systems from electronic to any observable scales as reviewed in the present work.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2025

Application of Cyber-Informed Engineering for Protecting BESS

This white paper synthesizes an array of crucial grid services provided by BESS technology, assesses its architecture and communications, and presents a case study for analysis against the principles introduced by Cyber-Informed Engineering (CIE). Furthermore, in walking through the analysis, this paper presents a framework to evaluate risks and solutions when considering BESS components. Asset owners and buyers could perform this analysis to assess their BESS product implementations, alternative inverter-based resources (IBR), and energy management systems (EMS). Battery systems fulfill various roles contingent on the unique market demands and the specific challenges presented by regional grid infrastructures. These roles also vary due to the differing utility models for ownership and operation, which are adapted to meet regional and local capabilities and requirements. Concerns have been raised regarding the potential for adversaries to exploit knowledge of battery operational patterns to orchestrate decisive attacks. However, the security of operational data for these systems may not be the primary vulnerability, as much of this information is already well-understood within the community. Applying a modest degree of subject matter expertise can often yield valuable predictions regarding how a battery will respond under certain conditions, such as grid emergencies, high or low-temperature days, Public Safety Power Shutoff (PSPS) events, and outages. The operational characteristics of batteries are well-documented, and their capabilities, including the risks associated with misoperation and the resulting consequences, are published and understood within the industry. CIE practices represent the next step in gaining functional assurance and providing an acceptable level of risk, regardless of whether a battery vendor can support a trusted and validated supply chain. While this issue has exacerbated supply chain challenges, it is not an isolated condition. This foreign supply route is the primary source of BESS for the U.S. market. Significant efforts are underway through the Bipartisan Infrastructure Law (BIL) to change that. Still, strategic short-term operational mitigations are needed to ensure the security of our operational technology (OT) systems, which are enhanced by instilling trust and are separate from vendors implementing CIE principles.

25 ENERGY STORAGE↗
DOE OSTI2026

Overview of design developments for Condensable Vapor Devices for ITER

The Condensable Vapor Devices (CVDs), which are part of the ITER Roughing Pump System (RPS), are designed to separate tritiated water content to protect downstream pumps and transfer the water to Tokamak Exhaust Processing (TEP) systems for further separation. CVDs operate on the principle that a cooling fluid, such as liquid nitrogen, cools the exhaust gas stream (process gas) from the Tokamak, allowing the water present in the process gas to condense and freeze, thereby trapping it in the CVDs. The CVDs once saturated with the ice are then regenerated to release the trapped water molecules, which are sent to the TEP. The present article will describe the technical requirements, challenges, and design progress made so far in the development of the CVDs.

Choukekar, Ketan [ORNL] (ORCID:0009000288016383)↗
DOE OSTI2024

Integrated photonic structures for photon-mediated entanglement of trapped ions

Trapped atomic ions are natural candidates for quantum information processing and have the potential to realize or improve quantum computing, sensing, and networking. These applications often require the collection of individual photons emitted from ions into guided optical modes, in some cases for the production of entanglement between separated ions. Proof-of-principle demonstrations of such photon collection from trapped ions have been performed using high-numerical-aperture lenses or cavities and single-mode fibers, but integrated photonic elements in ion-trap structures offer advantages in scalability and manufacturability over traditional optics. In this paper we analyze structures monolithically fabricated with an ion trap for collecting ion-emitted photons, coupling them into waveguides, and manipulating them via interference. We calculate geometric limitations on collection efficiency for this scheme, simulate a single-layer grating that shows performance comparable to demonstrated free-space optics, and discuss practical fabrication and fidelity considerations. Based on this analysis, we conclude that integrated photonics can support scalable systems of trapped ions that can distribute quantum information via photon-mediated entanglement.

Knollmann, Felix W.↗
DOE OSTI2026

Continuous Counter‐Current Microfluidic Liquid–Liquid Extraction Achieved Using a Pair of Wettable Screen Meshes

Continuous counter‐current microfluidic liquid–liquid extraction performs separations by flowing immiscible liquids in opposing directions within a single flow channel. In principle, this flow arrangement enables a large number of theoretical separation units in a small footprint, without using interstage valving, pumping, and phase separation. Despite its potential for excellent separation performance, this microfluidic scheme rarely appears in literature due to the requirement for capillary forces to be greater than hydrodynamic forces for stable flow. We present a novel microfluidic device and flow approaches that overcome this force‐balance challenge, enabling stable, long‐duration continuous counter‐current flow. Additionally, we cover a suite of methodologies for quantifying the performance of the microfluidic device, revealing the number of theoretical equilibrium stages achieved. The enabling technologies include a woven mesh screen‐based microfluidic device architecture that is easily fabricated outside of a clean room, surface functionalization strategies to promote conjugate (organic/aqueous) wettability, flow approaches to eliminate bubbles and carryover, and computer‐aided flow automation with optical measurement of extraction performance. The reported experiments lasted for over 36 h, terminated only at experiment conclusion, where the device still exhibited good performance. Automated Raman spectroscopy was used for solute quantitation of the ternary system tert‐butanol in a toluene/water matrix, a ternary system that was specifically chosen to analyze the device's performance with a small solute partition ratio and to enable in‐line Raman measurements of solute concentrations in both phases. The microfluidic device possessed a 55 mm contact length and a 38.5 µL internal volume. During counter‐current flow, we observed approximately 37 equilibrium stages (37 ± 13) based on a best‐fit of the solute fraction remaining in the aqueous phase using a Kremser Group Method analysis.

36 MATERIALS SCIENCE↗
DOE OSTI2025

First-Principles Molecular Dynamics Simulations of Ammonia Adsorption onto MFI Zeolite Nanosheets

MFI zeolite nanosheet membranes are promising candidates for ammonia separation from nitrogen and hydrogen gases, yet questions remain on the origin of their high selectivity. Silanols, Si–OH, are present in high concentration at the surface of zeolite nanosheets, and force-field-based simulations indicate that surface adsorption at the silanols contributes to selectivity. Acidic silanol groups can chemically react with ammonia via transfer of a proton to form ammonium ions, which may further contribute to the ability of zeolite nanosheet membranes to separate ammonia from other gases. In this work, we used first-principles molecular dynamics techniques to simulate ammonia’s behavior within stacked MFI zeolite nanosheets. We found that at 523 K and a loading corresponding to 35 bar, conditions desired for the ammonia separation, about 30% of ammonia reacts with surface silanols. Our work explored H-bonding and proton transfer within this system.

ammonia↗
DOE OSTI2025

First Principles Molecular Dynamics Simulations of Ammonia Adsorption onto MFI Zeolite Nanosheets

MFI zeolite nanosheets membranes are promising candidates for ammonia separation from nitrogen and hydrogen, yet questions remain on the origin of their high selectivity. Silanols, Si-OH, are present in high concentration at the surface of zeolite nanosheets, and force-field-based simulations indicate that surface adsorption at the silanols contributes to selectivity. Silanols can chemically react with ammonia, which may further contribute to the ability of zeolite nanosheet membranes to separate it from other gases. In this work, we use first-principles molecular dynamics techniques to simulate ammonia’s behavior within stacked MFI zeolite nanosheets. We find that at 523 K and a loading corresponding to 35 bar, conditions desired for the ammonia separation, about 30% of ammonia reacts with surface silanols. Our work explores H-bonding and proton transfer within this system.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Solvent Polarity Independent Symmetry-Breaking Charge Separation in a Slip-Stacked Covalent Terrylene Monoimide Dimer

The design of organic materials capable of efficient photoinduced charge separation in low-polarity environments is a critical challenge for advancing organic photovoltaics. Symmetry-breaking charge separation (SB-CS) offers a promising route to efficient charge separation with minimal energy loss; however, in conventional organic materials this process typically relies on polar solvents to stabilize the charge-separated state. Here, we investigate a slip-stacked terrylene monoimide dimer (TMI 2 ) engineered with intrinsic electronic asymmetry to circumvent this limitation. We demonstrate through a comprehensive suite of ultrafast spectroscopic techniques that TMI 2 undergoes remarkably efficient SB-CS regardless of solvent polarity enabled by the permanent dipole moment of TMI and the accessible intramolecular charge-transfer (ICT) character of its monomer units. Furthermore, analysis of vibronic coherences reveals that the initial state mixing is actively driven by a 193 cm –1 intermolecular mode, while the final SB-CS state is marked by a distinct vibrational fingerprint of the radical ion pair product. Our findings reveal how the intrinsic electronic asymmetry of the TMI monomers that constitute TMI 2 creates an efficient charge separation pathway that precludes the need for external stabilization from a polar solvent. Here, this work establishes a powerful molecular design principle for leveraging intrinsic monomeric asymmetry to achieve efficient charge separation in low-dielectric environments, with significant implications for the development of next-generation organic optoelectronic materials.

Aromatic compounds↗
DOE OSTI2025

High gas-pressure apparatus for nonlinear X-ray propagation and reshaping via stimulated X-ray Raman scattering

Abstract We describe an experimental setup for non-linear interaction and propagation of ultrashort and intense x-ray free-electron laser (XFEL) pulses in a dense gas. It allows one to provide high, but adjustable, target-gas pressures of up to 6 bar within a vacuum environment of 3∙10 − 3 mbar or better. The setup enables investigation of intense x-ray propagation in an optically thick medium with minimal absorption loss of the unfocused beam outside of the target. As an application, we demonstrate the amplification of spectrally-resolved stimulated x-ray Raman scattering (SXRS) in dense neon gas, where the most intense inner part of the beam is almost completely absorbed. As a result, in the inner part of the beam, the SXRS signal exceeds the residual XFEL pulse by a factor of around two. In principle, this reshaping effect allows for a spatial separation of the two spectral components, i.e., the driving pulse and the SXRS signal.

Magunia, Alexander↗