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DOE OSTI2019

Fluid-based gating mechanism with tunable multiphase selectivity and antifouling behavior

A gating mechanism that uses a capillary stabilized liquid as a reversible, reconfigurable gate that fills and seals pores in the closed state, and creates a non-fouling, liquid-lined pore in the open state is disclosed. Theoretical modeling and experiments demonstrate that for each transport substance, the gating threshold—the pressure needed to open the pores—can be rationally tuned over a wide pressure range. This enables realizing in one system differential response profiles for a variety of liquids and gases, even letting liquids flow through the pore while preventing gas from escaping. These capabilities allow dynamic modulation of gas-liquid sorting and to separate multi-phase mixtures, with the liquid lining ensuring sustained antifouling behavior. Because the liquid gating strategy enables efficient short-term and long-term operation and can be applied to a variety of pore structures and membrane materials, and to nano, micro as well as macroscale fluid systems, the gating systems is useful in a wide range of applications.

36 MATERIALS SCIENCE↗

DOE OSTI2019

JOINING TECHNIQUES FOR NOVEL METAL POLY MER HYBRID HEAT EXCHANGERS

In the United States, over 50% of the unrecovered e nergy from industrial processes is in the form of low- grade heat (<220°C). Materials and maintenance co sts of common heat exchangers are typically too hig h to justify their usage. Polymers, though more afford able, are usually unsuitable for HX applications due t o their low thermal conductivity (~0.2 W/mK). Here, we show that metal-polymer hybrids may be attractiv e from both performance and cost perspectives. The use of polymers further increases the resistance to c orrosion by sulfuric and carbonic acids often present in flue gases. An ongoing work explores different co nfigurations of layered polyimide-copper macroscale hybrids for heat exchanger applications using numeri cal simulations. This paper explores a manufacturing pathway for producing such layered hybrid tubes tha t involves directly rolling and bonding tapes made of polymer and copper foil into tubes. A critical problem in the fabrication process is the bonding of metal and polymers. We explore approaches involving adhesiv es (epoxy, acrylic and silicone) for metal/polymer inte rfaces and direct welding (ultrasonic) for metal/metal interfaces that can be integrated into the manufacturi ng process. We report characterizations of the therm omechanical properties of these joining processes. T his work paves the way for realizing cost-effective m anufacturing of heat exchangers for low grade waste heat recovery.

Kuntumalla, Gowtham↗

DOE OSTI2021

Coupled Microbial-Conversion and Computational-Fluid-Dynamics (CFD) Models for Butanediol Production in Micro-Aerated Reactors

Microbial conversion of substrates to macromolecules has been widely used in the synthesis of value-added products in pharmaceutical and biotechnology industries. These bioreactions are also being investigated in the production of low-value commodities such as biofuels [1]. Gas-liquid mass-transfer and transport-reaction coupling are important challenges when designing and scaling up these reactor systems. Experiments in wellmixed small-scale reactors have enabled characterization of microbial reactivity, while their coupling with macroscale transport remains relatively unexplored. In this work, we use a coupled metabolic-CFD model to study the action of a genetically engineered microbe Zymomonas mobilis [2] on sugars to produce 2,3-Butanediol (BDO). BDO is an important hydrocarbon intermediate that can be catalytically upgraded to several fuels and chemicals [3]. An important aspect to this particular microbial conversion is the need for micro-aerated environments as opposed to traditional aerobic fermentation. Slight variations in oxygen concentration can result in competing reaction pathways that disable BDO production. Hence, gas-liquid mass transfer and transport need to be optimized in large-scale reactors to maximize BDO production, for which CFD is a valuable tool. The aerobic-fermentation CFD model previously developed by the authors [5] for simulating bubble-column and airlift reactors at scale was used in this study. The Reynolds-averaged mass, momentum and energy transport equations for interpenetrating gas and liquid phase are solved in this model along with the transport and interphase mass transfer of oxygen. Our previous work used a phenomenological model for microbial oxygen uptake that neglected microbial growth and other reaction pathways. In this work, a detailed metabolic model enabled prediction of product formation and inhibition pathways. In order to manage computational cost, we used a subcycling technique [6] that takes advantage of the clear separation in transport (~ 200 sec) and reaction (~ 2-3 hours) timescales. The CFD model is first solved to steady state, after which the metabolic model is advanced at every cell in the computational domain using the local oxygen concentration. The CFD model is then run to achieve a new steady state that provides a new oxygen distribution for the metabolic model. This process, where reaction and fluid updates are interleaved together, is iterated until reactants are completely exhausted. This work will examine the performance of different reactor designs such as bubble column and airlift reactors at scale (250-500 m3). Oxygen mass-transfer coefficient and distribution are critically analyzed among reactors, and optimization studies pertaining to aeration is presented. Furthermore, it has been observed in experiments that high BDO production may be achieved by manipulating the aerobic environment over the course of reaction, such that oxygen concentration is high during the growth phase, and very low as sugar is depleted. This characteristic will be addressed by our simulations for which a timedependent scheduling strategy for aeration is presented that maximizes BDO production. [1] Humbird, D., Davis, R., and McMillan, J., Aeration costs in stirred-tank and bubble column bioreactors, Biochemical Engineering Journal, 127, 161—166, 2017 [2] Yang, S., Mohagheghi, A., Franden, M. A., Chou, Y.-C., Chen, X., Dowe, N., Himmel, M. E., and Zhang, M., Metabolic engineering of zymomonas mobilis for 2, 3-butanediol production from lignocellulosic biomass sugars. Biotechnology for biofuels, 9(1):189, 2016 [3] Kim, S. J., Sim, H. J., Kim, J. W., Lee, Y. G., Park, Y. C., and Seo, J. H., Enhanced production of 2,3-butanediol from xylose by combinatorial engineering of xylose metabolic pathway and cofactor regeneration in pyruvate decarboxylase-deficient Saccharomyces cerevisiae. Bioresource Technology, 245:1551–1557, 2017 [4] Weller, H., Tabor, G., Jasak, H. and Fureby, C., A tensorial approach to computational continuum mechanics using object-oriented techniques, Computers in physics, 12, 6, 620--631, 1998

29 ENERGY PLANNING, POLICY, AND ECONOMY↗

DOE OSTI2022

Hierarchical printed product and composition and method for making the same

Disclosed herein are embodiments of a printable composition that can be used to make printed products of a chosen material chemistry that have different levels of porosity within the printed product's structure Also disclosed herein are embodiments of a printed product that has multiple levels of porosity throughout its structure, which can include a macroscale level of porosity, a microscale level of porosity, a nanoscale level of porosity and any combination thereof. These printed products can be made using a 3-D printer and can be made from a single printable composition without the need to add different structural components during the production process. Also disclosed herein are embodiments of a method for making and using a printed product.

Lee, Matthew N.↗

DOE OSTI2022

A Study on Surface Texture and Wettability of Femtosecond Laser Treated Aluminum Alloys

This research aims to study the effects of femtosecond laser treatment on surface texture and wettability properties. The first portion of this research studies 2024-T3 aluminum alloy concerning surface texture (e.g., roughness), wettability, and surface free energy. SEM images help aid the researchers in detecting minuscule changes in surface texture. Profilometry extracts topographical data from the surface. A contact angle goniometer measures contact angle, which follows the sessile drop method. Owens, Wendt, Rabel, and Kaelble's method calculates the surface free energy in conjunction with the contact angle. Femtosecond laser modification produces relatively uniform surface morphology at the macroscale. When looking at the microscale, surface morphology differs depending on the interplay between material melting and self-assembly, where the surface becomes rougher after laser treatment. Contact angle results show that all but the control sample and sample 7 exhibit hydrophobic behavior, i.e., contact angle >90°, with Sample 1 having the most significant angle of 115°. The effects of laser parameters on surface energy is apparent. More work is needed to establish correlations among these three quantities: contact angle, surface energy, and laser parameters. The second portion of this research studies aluminum alloy 6061 as the subject material with the primary goal of creating a superhydrophobic surface. A central composite design creates the laser surface texturing design of experiments. SEM images help aid the researchers in detecting minuscule changes in surface texture. A 3D optical profiler extracts topographical data from the surface. The sessile drop method incorporates a contact angle goniometer to measure the contact angle. The response surface method builds a second-order polynomial model for the contact angle and obtains optimized parameters to maximize the contact angle. This research shows that laser surface texturing can generate a wide range of surface profiles and roughness values with geometric features ranging from hundreds of μm to submicron. All three laser parameters (pulse energy, pulse duration, repetition rate) affect surface roughness and contact angle to some degree. To quantify the relationship between the contact angle, pulse energy, and pulse repetition rate, a response surface model for Al 6061 is identified and used to find the optimal conditions of E=214 μJ, tp=10 ps, and fp=2427 Hz with a predicted maximum contact angle of 161°. A confirmation experiment produces a contact angle of 168°, in good agreement with the predicted value.

Angell, Dakota↗

DOE OSTI2023

Microstructured ion-conducting composites and uses thereof

A composite membrane with nanostructured inorganic and organic phases is applied as an ion-selective layer to prove processability, prevent dendrite shorting, and increase power output of lithium-metal anodes through better Li-ion conductivity. Nanoconfinement, as opposed to macroscale confinement, is known to dramatically alter the properties of bulk materials. Control over a ceramic's size, shape, and properties is achieved with polymer templates. This is a new composition of matter and unique approach to composite membrane design.

Frischmann, Peter David↗

DOE OSTI2023

Low power sensor for NO x detection

Detection and capture of toxic nitrogen oxides (NO x ) is important for emissions control of exhaust gases and general public health. The low power sensor provides direct electrically detection of trace (0.5-5 ppm) NO 2 at relatively low temperatures (50° C.) via changes in the electrical properties of nitrogen-oxide-capture active materials. For example, the high impedance of MOF-74 enables applications requiring a near-zero power sensor or dosimeter, such as for smart industrial systems and the internet of things, with 0.8 mg MOF-74 active material drawing <15 pW for a macroscale sensor 35 mm 2 area.

Small, Leo J.↗

DOE OSTI2016

First-Principles Study of Surface Properties of U{sub 3}Si{sub 2} for Accident Tolerant Fuel

Due to the high thermal conductivity and uranium density compared to UO{sub 2} fuel used in current Light Water Reactors (LWRs), U-Si fuels, such as the U{sub 3}Si{sub 2} and U{sub 3}Si{sub 5} compounds, are currently under investigation for the development of accident tolerant fuels (ATF) in response to the Fukushima Daiichi accident in Japan. In order to perform meaningful mesoscale and macroscale fuel performance simulations, fundamental material properties of nuclear fuels should be known. One example is the simulations of fission gas bubble evolution and gas bubble-induced swelling in nuclear fuels using mesoscale methods, such as phase field and rate theory. To properly describe the gas bubble behavior in the fuel, it is crucial to know the surface energies of the fuel. Unfortunately, there is no study of the surface properties of U{sub 3}Si{sub 2} from both experiment and theory. To this end, we systematically investigate the surface properties of U{sub 3}Si{sub 2} using density functional theory (DFT) based first-principles calculations. Of several low index facets, we studied the (001) and (100) surfaces of tetragonal U{sub 3}Si{sub 2} with all the possible terminations. Since all the studied surfaces are not stoichiometric, we also investigated the effect of elemental chemical potentials on the formation of surface. We systematically investigate the surface properties of U{sub 3}Si{sub 2} using density functional theory calculations. Of several low-index facets, the (001) and (100) surfaces show similar averaged surface energies calculated using even number of layers. At the high Si chemical potential, the Si-terminated U{sub 3}Si{sub 2}(100) and U{sub 3}Si{sub 2}(001) surfaces show lower energies than those of the U-terminated surfaces, with U,Si-terminated U{sub 3}Si{sub 2}(001) as the most stable surface. The surface energies of all non-stoichiometric U{sub 3}Si{sub 2} are linearly dependent on the Si chemical potential. The surface energies of U-terminated surfaces decrease as Si potential decreases. The U{sub 2}-terminated U{sub 3}Si{sub 2}(100) surface becomes that the most stable surface at U-rich side. Based on the current results, an averaged surface energy of U{sub 3}Si{sub 2}, i.e., 1.45 J/m{sup 2}, is recommended for the description of the rounded facets of gas bubbles in U{sub 3}Si{sub 2} by mesoscale simulations. (authors)

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2016

High Energy X-ray Applications for the Characterization of Metallic Uranium Alloys

Uranium-based metallic alloys are both candidates for fuels in high performance research and test reactors, as well as in fast spectrum reactors as nuclear transmutation fuels that can be utilized to burn long-lived minor actinides and fission products. Uranium-molybdenum (UMo) alloys are under development for the use in research and test reactors. Whereas, uranium-zirconium (U-Zr) alloys represent one of the types of fuels that are under consideration for use within the fast spectrum reactors. Both of these types of metallic fuels have been studied for over five decades in various types of reactors. Many of the previous studies had focused on performance-based aspects. However, recent advances in characterization tools and techniques, as well as short-term (low fluence) neutron irradiation facilities have contributed to a more in-depth understanding of nuclear fuel and material behavior following irradiation. This knowledge is crucial to the enhancement of current modeling and simulation techniques, particularly with respect to parameterization and validation. This paper focuses on the use of high energy x-rays to characterize metallic nuclear fuel. The specimens were composed of depleted uranium (DU) alloyed with either Zr or Mo, where DU-xZr (x = 10, 15, or 20 wt.%) and DU-yMo (y = 7 or 10 wt.%). The geometries of the specimens were 3 mm TEM disks that were ∼200 μm in thickness. The fuel alloys were initially prepared via an arc melting process. The samples were irradiated at the Advanced Test Reactor at Idaho National Laboratory (INL) using the hydraulic rabbit system. The hydraulic rabbit system allows for well-controlled, short term irradiations (less than one cycle), hence resulting in low fluences. The U-based alloys were irradiated to doses of 0.01 and 0.1 dpa. The irradiation temperature of the specimens ranged from 150 deg. C to 800 deg. C. Synchrotron characterization techniques can be used to provide insight into material microstructure ranging a multitude of spatial scales, from the atomic scale to the macroscale. High-energy x-rays at the National Synchrotron Light Source II (NSLS II) and the Advanced Photon Source (APS) have been utilized to understand the microstructural changes in these metallic alloys, specifically with respect to phase identification, phase fractions, chemical bonding, strain, and dislocation density through the use of diffraction and X-ray Absorption Spectroscopy (XAS). These experiments utilized a robot for specimen exchange during the diffraction measurements, allowing for remote handling of radioactive materials. This is an example of another recent advancement in characterization techniques that enables research with nuclear materials. Detailed results of the analyses of the microstructural changes are pending.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2020

Determination of Elastic Coefficients for a Composite with Crossing Steel - 20086

For a composite material with an embedding of crossing reinforcement bars, the elastic coefficients are calculated by solving a boundary-value problem (elastostatic problem). The background material is concrete whereas the bars are made of steel. The bars cross each other horizontally at a right angle. The boundary-value problem is solved numerically by using 3-D quadratic basis functions in ABAQUS{sup R}. Under external shear loading conditions, the effective elastic coefficients on the macroscale are quite larger for a cross-section in which the bars are immediately below the ones in the cross-section normal to it. The shear modulus in the off-plane direction is about one and half times larger than that in the in-plane direction. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2016

Theoretical Modeling of Radiation Damaged Polyethylene

The insulation around the electrical cables in nuclear power plants is made of ethylene propylene rubber and cross-linked polyethylene. The insulation is subjected to environmental and radiation damage. We wish to develop methods to evaluate the degradation of the insulation with the hope of predicting the performance and lifetime. Here we present a series of calculations aimed at identifying the features in IR and Raman spectra that can be used as a means of evaluating the insulation around cabling. Further we develop molecular dynamics calculations to examine the macroscale mechanical properties of the insulation material. (authors)

36 MATERIALS SCIENCE↗

DOE OSTI2022

Development of Lightweight Structural Materials with Improved Properties for Fission Batteries

Fission batteries require lightweight structural materials that demonstrate structural resilience when subjected to repeated shutdown, transportation, startup cycles, and certain external conditions, including rare events such as seismic vibrations and tsunamis. The objectives of this project are (1) to produce lightweight structural materials whose strength-to-weight ratios and fatigue resistance exceed those of current widely used structural materials such as 316 stainless steels (SS316), and (2) to enhance radiation tolerance of structural materials over a suitable service temperature range. To achieve these, (1) a lattice structure will be produced, (2) advanced modeling and simulation tools will be employed to design lattice structures (e.g., a gyroid structure) that reduce stress concentrations and thus increase fatigue resistance, and (3) one-dimensional (1-D) carbon nanotubes will be added to enhance radiation resistance. To validate our solution, high-temperature tensile and fatigue testing, in combination with microstructure characterization, will be conducted on wrought materials, additively manufactured solid materials, and the designed lightweight lattice structure material. Ion irradiation, microstructure characterization, and nanoindentation will be carried out to investigate the effect of 1-D carbon nanotubes on radiation tolerance. Successful completion of this project will deliver a material to serve as a substitute for current SS316 using the same chemistry but with lighter weight and improved mechanical properties. In addition, a material with carbon nanotubes can be designed for improved radiation tolerance over a suitable service temperature range. This project will establish new techniques in innovative materials/lattice design, advanced macroscale properties prediction, and the application of state-of-the-art processes.

36 MATERIALS SCIENCE↗

DOE OSTI2024

When and Where Lithium Plating Occurs, Its Correlation with Microstructure Heterogeneity, and the Mechanisms That Initiate and Self-Regulate Electrochemical Heterogeneity (A02-0444)

A microstructure scale electrochemical LIB model was used to investigate lithium plating onset, material non-uniform utilization, and in-plane heterogeneities for an NMC-graphite full cell. Model predicts active material particle surface roughness and size distribution (respectively, non-uniform curvature within and between particles) initiate in-plane heterogeneity, and that particle size heterogeneity at the separator interface controls the lithium plating preferential deposition ("Where"). These in-plane heterogeneities are then exacerbated by through-plane heterogeneities induced at fast charge as electrolyte depletion occurs and concentrates intercalation reaction near the anode-separator interface. Also, magnitude and occurrence of lithium plating is controlled by effective, or macroscale, microstructure parameters ("When"). As local states of charge start to diverge between nearby active material regions, overpotential differences induced by OCP difference kick in and contribute to reduce these SOC local heterogeneities. However, for staged materials such as graphite, with OCP profile alternating between plateaus and varying regions, this balancing mechanism is, respectively, inactive and active. This leads to a dynamic, non-monotonic, in-plane heterogeneity time evolution for state of charge and Faraday current density, for which their respective in-plane heterogeneity magnitude alternates. Such behavior has been modeled both for the whole electrode at the microstructure scale and at the particle scale. In-plane heterogeneities are usually considered to be detrimental, as they result in material non-uniform utilization (i.e., under and over stressed regions) and earlier degradations. However, this work provides a more granular approach as it discriminates between a harmful in-plane heterogeneity (non-uniform curvature) that triggers SOC in-plane heterogeneity, and a beneficial in-plane heterogeneity (Faraday current density) that contributes to reduce SOC in-plane heterogeneity. This work comprehensively explains the mechanisms that initiate, exacerbate, and regulate heterogeneity at the microstructure scale, while providing some design suggestions to reduce both in-plane and through-plane heterogeneities, as summarized in the graphical abstract.

ADVANCED PROPULSION SYSTEMS↗

DOE OSTI2010

Encapsulated Nanoparticle Synthesis and Characterization for Improved Storage Fluids: Preprint

Nanoparticles are typically composed of 50--500 atoms and exhibit properties that are significantly different from the properties of larger, macroscale particles that have the same composition. The addition of these particles to traditional fluids may improve the fluids' thermophysical properties. As an example, the addition of a nanoparticle or set of nanoparticles to a storage fluid may doubleits heat capacity. This increase in heat capacity would allow a sensible thermal energy storage system to store the same amount of thermal energy in half the amount of storage fluid. The benefit is lower costs for the storage fluid and the storage tanks, resulting in lower-cost electricity. The goal of this long-term research is to create a new class of fluids that enable concentrating solarpower plants to operate with greater efficiency and lower electricity costs. Initial research on this topic developed molecular dynamic models that predicted the energy states and transition temperatures for these particles. Recent research has extended the modeling work, along with initiating the synthesis and characterization of bare metal nanoparticles and metal nanoparticles that areencapsulated with inert silica coatings. These particles possess properties that make them excellent candidates for enhancing the heat capacity of storage fluids.

14 SOLAR ENERGY↗

DOE OSTI2020

Correlation of Spatiotemporal Dynamics of Polarization and Charge Transport in Blended Hybrid Organic–Inorganic Perovskites on Macro- and Nanoscales

Progress in flexible organic electronics necessitates a full understanding of how local inhomogeneities impact electronic and ionic conduction pathways and underlie macroscopic device characteristics. In this work, we used frequency- and time-resolved macro- and nanoprobe measurements to study spatiotemporal characteristics of multiscale charge transport dynamics in a series of ternary-blended hybrid organic inorganic perovskites (HOIPs) (MA 0.95– x FA x Cs 0.05 PbI 3 ). We show that A-site cation composition defines charge transport mechanisms across broad temporal (10 2 –10 –6 s) and spatial (millimeters–picometers) scales. Ab initio molecular dynamic simulations suggest that insertion of FA results in a dynamic lattice, improved ion transport, and dipole screening. We demonstrate that correlations between macro- and nanoscale measurements provide a pathway for accessing distribution of relaxation in nanoscale polarization and charge transport dynamics of ionically conductive functional perovskites.

36 MATERIALS SCIENCE↗

DOE OSTI2024

Macroscopic modeling of gas permeability in hierarchical micro/nanoporous media: A unified characterization of rarefaction using Klinkenberg theory and equivalent diameter

Estimating gas transport through a hierarchical micro/nanoporous system is challenging due to non-equilibrium gas dynamics. The primary difficulty lies in determining the rarefaction level, because identifying a representative flow dimension in a complex porous system with multiple pore scales is not straightforward. Our study performed a pore-level analysis for gas permeability in dual-scale porous media with varying porosity, throat size, and secondary pore size under different rarefaction conditions. We found that secondary porosity negatively affects permeability due to increased friction forces, with this influence growing as the secondary pore size and porosity increase until the secondary pore becomes comparable to the throat. However, rarefaction reduces the effects of secondary pores due to boundary slip. Traditional Knudsen number (Kn) calculations based on Darcy-defined height failed to accurately describe the rarefaction effects on gas permeability. Instead, we introduced an equivalent diameter to calculate the Kn, which provided an accurate normalization of apparent gas permeability independent of pore geometry. Furthermore, the extended Kozeny–Carman–Klinkenberg model developed in our previous study successfully yielded a macroscopic model for apparent gas permeability in hierarchical micro/nanoporous systems as a function of the traditional Darcy height and porosity.

04 OIL SHALES AND TAR SANDS↗

DOE OSTI2011

Multi-Summer Climatology of Cumuli at SGP site: Vertical Structure

We perform a case study for estimating the impact of the vertical distribution of cloud fraction on the normalized cloud radiative forcing (CRF) using a decade-long (2000-2009) high resolution dataset of cloud macrophysical and radiative properties. This dataset is developed for fair-weather cumuli (FWC) observed at the U.S. Department of Energy's Atmospheric Radiation Measurement (ARM) Southern Great Plains (SGP) site. The design of the case study reduces effects associated with non-cloud factors, such as the diurnal changes of aerosol loading and solar zenith angle. The results of the case study suggest that the impact of the vertical cloud structure can be substantial. Therefore, taking into account the vertical distribution of clouds would be beneficial for more comprehensive parameterizations aimed to portray the complex interactions between clouds and radiation more accurately

54 ENVIRONMENTAL SCIENCES↗

NASA NTRS2015

ARTEMIS Lunar Orbit Insertion and Science Orbit Design Through 2013

As of late-July 2011, the ARTEMIS mission is transferring two spacecraft from Lissajous orbits around Earth-Moon Lagrange Point #1 into highly-eccentric lunar science orbits. This paper presents the trajectory design for the transfer from Lissajous orbit to lunar orbit insertion, the period reduction maneuvers, and the science orbits through 2013. The design accommodates large perturbations from Earth's gravity and restrictive spacecraft capabilities to enable opportunities for a range of heliophysics and planetary science measurements. The process used to design the highly-eccentric ARTEMIS science orbits is outlined. The approach may inform the design of future planetary moon missions.

lunar orbiters↗