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DOE OSTI2024

Transient Chemo‐Mechanical Model of Lithium Plating Impacted by External Pressure

Abstract Lithium anodes show great promise in commercial applications, but are hindered by lithium plating and dendrite growth which cause safety concerns during long‐term cell operation. Stack pressure is experimentally observed to improve cell lifetime; however, the relationship between stress and lithium deposition has remained difficult to elucidate. In this work, a transient, 3D, finite‐element model of the evolution of a lithium anode due to stripping and plating is developed. The evolution of a microscale protrusion on the anode surface is tracked over one charge‐discharge cycle with respect to stack pressure and lithium yield strength. Lithium plastic deformation, nonconformal anode‐separator contact, and separator porosity effects are accounted for. Over the course of several hours of stripping/plating, the anode surface evolves to a similar morphology under pressure regardless of the initial conditions due to lithium plastic deformation and hardening. The rate of this evolution highly depends on the applied pressure and assumed lithium yield strength.

25 ENERGY STORAGE↗
DOE OSTI1994

Nuclear Safety [Vol. 35, No. 2, July-December 1994]

Nuclear Safety is a journal that covers significant issues in the field of nuclear safety. Its primary scope is safety in the design, construction, operation, and decommissioning of nuclear power reactors worldwide and the research and analysis activities that promote this goal, but it also encompasses the safety aspects of the entire nuclear fuel cycle, including fuel fabrication, spent-fuel processing and handling, and nuclear waste disposal, the handling of fissionable materials and radioisotopes, and the environmental effects of all these activities. Table of Contents for this issue follows. GENERAL SAFETY CONSIDERATIONS: 179 Consideration of Postaccident Consequences in the Determination of Safety Objectives for Future Nuclear Power Plants in France, D. Queniart, A. Sugier, and J. Lochard; ACCIDENT ANALYSIS: 187 Nuclear Safety Research: The Phebus FP Severe Accident Experimental Program, P. von der Hardt, A. V. Jones, C. Lecomte, and A. Tattegrain; 205 Containment Performance Analysis of the Advanced Neutron Source Reactor at the Oak Ridge National Laboratory, S. H. Kim, R. P. Taleyarkhan, and V. Georgevich; 213 Assessment of Fission Product Deposits in the Reactor Coolant System: The DEVAP Program, G. Le Marois and M. Megnin; 222 Erratum to “A Review of the Available Information on the Triggering Stage of a Steam Explosion," Vol. 35, No. 1, CONTROL AND INSTRUMENTATION: 223 Effects of Normal Aging on Calibration and Response Time of Nuclear Plant Resistance Temperature Detectors and Pressure Sensors, H. M. Hashemian; DESIGN FEATURES: 235 Defense in Depth Against the Hydrogen Risk—A European Research Program, F. Fineschi; ENVIRONMENTAL EFFECTS: 246 Technical Note: A Preliminary Analysis of the Risks to Hong Kong Resulting from Potential Accidents of Daya Bay Nuclear Power Plant, Z. Shi and X. Wei; OPERATING EXPERIENCES: 253 Reactor Shutdown Experience, Compiled by J. W. Cletcher; SPECIAL SECTION ON TMI-2 VESSEL INVESTIGATION PROJECT: 256 Three Mile Island—New Findings 15 Years After the Accident A. M. Rubin and E. Beckjord; 269 Relocation of Molten Material to the TMI-2 Lower Head, J. R. Wolf, D. W. Akers, and L. A. Neimark; 280 Insight Into the TMI-2 Core Material Relocation Through Examination of Instrument Tube Nozzles, L. A. Neimark; 288 Physical and Radiochemical Examinations of Debris from the TMI-2 Lower Head, D. W. Akers and B. K. Schuetz; 301 Results of Metallographic Examinations and Mechanical Tests of Pressure Vessel Samples from the TMI-2 Lower Head, D. R. Diercks and G. E. Korth; 313 Margin-to-Failure Calculations for the TMI-2 Vessel, J. Rempe, L. Stickler, S. Chavez, G. Thinnes, R. Witt, and M. Corradini; U.S. NUCLEAR REGULATORY COMMISSION INFORMATION AND ANALYSES: 328 1993 Accident Sequence Precursor (ASP) Program Results, L. N. Vanden Heuvel, J. W. Cletcher, D. A. Copinger, J. W. Minarick, B. W. Dolan, and P. D. O’Reilley; RECENT DEVELOPMENTS: 339 Reports, Standards, and Safety Guides, D. S. Queener; 345 Proposed Rule Changes as of June 30, 1994; ANNOUNCEMENTS: 234 Thirty-First Annual Meeting of the National Council on Radiation Protection and Measurements; 356 1995 International Incineration Conference; 358 Fifth International Controls and Instrumentation Conference; 359 ANS International Topical Meeting on Safety of Operating Reactors; 359 Fifth International Conference on Nuclear Criticality Safety; 360 International Conference on Probabilistic Safety Assessment Methodology and Applications; 351 The Authors; 357 Reviewers of Nuclear Safety, Vol. 35.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2026

Iron surface corrosion in supercritical CO2 at atomic scale investigated by molecular dynamics simulations

Understanding the corrosion behavior of steels in supercritical carbon dioxide (S-CO2) is essential for ensuring the safe application of S-CO2 as a heat-transfer fluid in high-temperature energy systems, including advanced nuclear reactors. In this work, molecular dynamics (MD) simulations using ReaxFF potential are performed to explore the atomic-scale corrosion mechanisms of body-centered cubic iron (BCC-Fe) in S-CO2. The results show that CO2 molecules in S-CO2 decompose at the Fe surface, generating free C and O atoms that form Fe-C and Fe-O bonds and subsequently produce oxides and carbides. Concurrently, Fe atoms dissolve from the surface and diffuse into the S-CO2 region, resulting in interdiffusion of Fe, C and O atoms at the interface. The corrosion-layer thickness calculations show that high pressure and temperature induced by S-CO2 have stronger effects than surface orientation on the corrosion process. In addition, surface Fe atoms undergo substantial displacement under S-CO2 exposure, further accelerating corrosion. When a radiation-induced void is introduced near the Fe surface, the corrosion is enhanced. The void-matrix interface expands the reaction surface area and simultaneously induces corrosion reactions inside the bulk, resulting in a deeper penetration of C and O and thicker corrosion layers. All these results indicate that high-temperature, high-pressure and radiation-induced voids can seriously affect the corrosion of Fe in S-CO2, and must be considered to better use S-CO2 in nuclear facilities.

Li, Wenhua↗
DOE OSTI2024

Electrolyzer Integrated Modular Nano-Array Monolithic Catalytic Reactors

The project objective is to design and develop a new class of electrolyzer-integrated, modular, nanostructure array (nano-array) monolithic catalytic reactors for high-flux, robust and selective methanol synthesis. The modular reactor features metal oxide nano-array grown on an additively-manufactured channeled honeycomb monolith made of ceramic or metals; this low-pressure carbon dioxide hydrogenation reactor is fueled with hydrogen from a low-temperature water electrolyzer having reduced platinum group metal (PGM) content. Through these nanostructured monolithic reactors, methanol synthesis is enabled with cost-effective hydrogenation reactions under low-temperature (<200°C) and low-pressure (<10 atm) conditions, thus significantly reducing the energy demand of the entire process.

08 HYDROGEN↗
DOE OSTI2024

Electronic structure, magnetic correlations, and superconducting pairing in the reduced Ruddlesden-Popper bilayer La 3 Ni 2 O 6 under pressure: Different role of d 3 z 2 - r 2 orbital compared with La 3 Ni 2 O 7

The recent discovery of superconductivity in bilayer La 3 Ni 2 O 7 (327-LNO) under pressure stimulated much interest in layered nickelates. However, superconductivity was not found in another bilayer nickelate system, La 3 Ni 2 O 6 (326-LNO), even under pressure. To understand the similarities and differences between 326-LNO and 327-LNO, using density functional theory and the random phase approximation (RPA), we systematically investigate 326-LNO under pressure. The large crystal-field splitting between the e g orbitals caused by the missing apical oxygen moves the d 3z 2 -r 2 orbital farther away from the Fermi level, implying that the d 3z 2 -r 2 orbital plays a less important role in 326-LNO than in 327-LNO. This also results in a smaller bandwidth for the d x 2 -y 2 orbital and a reduced energy gap for the bonding-antibonding splitting of the d 3z 2 -r 2 orbital in 326-LNO, as compared to 327-LNO. Moreover, the in-plane hybridization between the d x 2 -y 2 and d 3z 2 -r 2 orbitals is found to be small in 326-LNO, while it is much stronger in 327-LNO. Furthermore, the low-spin ferromagnetic state is found to be the likely ground state in 326-LNO under high pressure. The weak interlayer coupling suggests that s ± -wave pairing is unlikely in 326-LNO. The robust in-plane ferromagnetic coupling also suggests that d-wave superconductivity, which is usually caused by antiferromagnetic fluctuations of the d x 2 -y 2 orbital, is also unlikely in 326-LNO. These conclusions are supported by our many-body RPA calculations of the pairing behavior. Additionally, contrasting with the cuprates, for the bilayer cuprate HgBa 2 CaCu 2 O 6 , we find a strong self-doping effect of the d x 2 -y 2 orbital under pressure, with the charge of Cu being reduced by approximately 0.13 electrons from 0 GPa to 25 GPa. In contrast, we do not observe such a change in the electronic density in 326-LNO under pressure, establishing another important difference between the nickelates and the cuprates.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Spall and subsequent recompaction of copper under shock loading

Research was undertaken to study spall and subsequent recompaction of oxygen-free high-thermal-conductivity copper using a single-stage large-bore light gas gun capable of planar impacts. Gun experiments were conducted that produced an initial spall in the target with a subsequent recompaction of the spall damage/layer by the use of layered impactors. Symmetric spall experiments at similar conditions were also conducted as a control to the recompaction experiments. Photonic Doppler velocimetry was used to obtain the velocity history of the target’s back surface; these velocity histories were analyzed, and the results were compared to numerical simulations. After recovery of selected samples, the microstructure was analyzed using optical imaging microscopy and electron backscatter diffraction. Recompaction waves were clearly observed in the time-resolved data obtained at the back surface of the targets. Two different series of experiments were performed to understand the effect of damage morphology on the stress required for spall recompaction. In the initial series, the peak pressure of the first shock was systematically increased to alter the amount of damage in the material. While in the second series, the peak pressure of the second shock was increased, keeping the magnitude of the first shock relatively constant to understand the effect of peak stress on the recompaction process. Findings clearly show that recompaction results in a perturbed band of the microstructure at the location of the expected spall plane in all cases except where the peak stress of the second shock is lower than the critical value.

, recompaction↗
DOE OSTI2021

Mathematical modeling and parameter estimation of MFI membranes for para/ortho‐xylene separation

Abstract A mathematical model of a membrane with a thin, oriented, and selective MFI layer, which also includes contributions from defects, pore blockages, support layer, and external mass transfer, was formulated based on the Maxwell‐Stefan equations. It was validated using reported (Kim et al., Angew Chemie Int Ed, 2018, 57:480–485; Jeon et al., Nature, 2017, 543:690–694) para/ortho‐xylene separation data from five MFI membranes. The diffusivities of the xylenes were considered to be the same for all membranes, while the thickness and the density of defects and pore blockage were treated as unique properties of each membrane, and their contributions were estimated by fitting the model to the corresponding separation data. The effects of these properties and the role of permeate pressure on the separation performance were subsequently analyzed. The proposed modeling, parameter estimation, and analysis framework allow one to quantitatively interpret the variation of separation performance, to understand separation bottlenecks, and to provide guidance for designing membranes with desired performance.

Liu, Jingjun↗
DOE OSTI2023

Time dependent chlorination of CeO 2 , La 2 O 3 and Nd 2 O 3 by ZrCl 4 dissolved in eutectic LiCl–KCl

Partial chlorination of CeO 2 , La 2 O 3 , and Nd 2 O 3 was achieved using ZrCl 4 dissolved in molten LiCl-KCl at 450°C over a period of 4-5 hr. ZrCl 4 was pre-volatilized into an argon stream to maintain a constant vapor pressure for equilibration with the salt. This approach was effective at maintaining the ZrCl 4 concentration at the solubility limit of 1.3 mol% in the molten salt throughout the duration of two of the chlorination experiments and within about 60% of the solubility limit in the third experiment. Based on the analysis of salt samples, fractional conversion after four hours of reaction for CeO 2 , and five hours for La 2 O 3 , and Nd 2 O 3 were calculated to be 0.97, 0.28, and 0.65 respectively. Assuming a shrinking core diffusion-limited model, the diffusivity of ZrCl 4 through the hypothesized ZrO 2 layer was calculated for the chlorination of CeO 2 , La 2 O 3 , and Nd 2 O 3 were 1.76 x 10 -10 cm 2 /sec, 7.85 x 10 -12 cm 2 /sec, and 7.42 x 10 -12 cm 2 /sec, respectively. Given the extremely low values calculated for diffusivity, it was concluded that the process is chemical reaction rate limited and that a complete reaction of each rare earth oxide could be achieved. Furthermore, a chemically controlled shrinking core model was shown to also fit the experimental data closely.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2022

Defect Thermodynamics and Transport Properties of Proton Conducting Oxide BaZr 1–x Y x O 3–δ (x ≤ 0.1) Guided by Density Functional Theory Modeling

Density functional theory-based thermodynamic modeling was performed to determine the effect of humidity and H 2 /O 2 gas pressure on the defect chemistry and transport properties of proton conducting oxide BaZr 1-x Y x O 3-δ (x ≤ 0.1) in the temperature range of 800–1200K, relevant for solid oxide fuel/electrolysis cell applications. The first-principles charge defect analysis was carried out to obtain the defect energetic ensembles as a function of Fermi level as well as the dependence of the hydration and oxidation reaction energies on complex defect-dopant configurations. It is shown that oxygen vacancies introduced to compensate for the extra Ba vacancies may cause a slight increase in the concentration of hydroxyl and proton species upon hydration of Ba deficient BaZr 1-x Y x O 3-δ , while the overall proton diffusivity is predicted to decrease with increased proton hopping barriers upon trapping near the Ba vacancies. The developed defect model is further demonstrated to be able to describe the bulk defect chemistry and transport properties of BaZr 0.9 Y 0.1 O 3-δ under the solid oxide cell operating conditions. Finally, the theoretical framework developed in this work further allows the inclusion of configurational, energetic and electronic characteristics of the defects that can be used as a complementary tool to experimental measurements for testing various mechanistic pathways or to provide essential mechanistic data.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Types of spatter and their features and formation mechanisms in laser powder bed fusion additive manufacturing process

Spatter causes defect formation, powder redistribution and contamination in laser powder bed fusion (LPBF) additive manufacturing process. It is critical to distinguish different types of spatter and understand their features and formation mechanisms. This work reveals the features and formation mechanisms of five unique types of spatter during the LPBF process by in-situ high-speed, high-energy x-ray imaging. Spatters observed during LPBF testing are quantified by their speed, size, and direction. Distinct quantifiable characteristics for each type of spatter are identified. Finally, effects of the laser power, scan speed, and ambient pressure on spatter formation and features are unraveled. A spatter formation map for AlSi10Mg alloy is constructed.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Thermal hydraulic characteristics of liquid sodium and supercritical CO 2 in a diffusion bonded heat exchanger

Compact heat exchangers are being examined for use in advanced, high-temperature nuclear or concentrated solar power plants to improve thermal efficiencies and reduce capital costs. At the time of this work, no experimental investigation of liquid sodium in the popular diffusion-bonded heat exchanger design had been performed. Herein this paper describes the thermal-hydraulic and overall operations performance observed during testing of a 316/L stainless steel “zig-zag” microchannel heat exchanger operating between a (0.5 kg/s) sodium loop and a (0.3 kg/s) recuperated supercritical CO 2 system with outlet conditions up to 550 °C at 16 MPa. Observed pressure drop is presented in the form of an effective friction factor correlation which aligns closely with recent experimental data. The thermal performance of this heat exchanger, measured by its overall conductance under various flow conditions, was decomposed to examine the independent convection behaviors of both the CO 2 and sodium streams. These results are presented in the form of Nusselt correlations fitted to the experimental data. The sodium heat transfer correlation aligns closely with the widely accepted Lubarsky-Kaufman correlation, while the CO 2 heat transfer correlation lies between previous correlations developed by computational and experimental methods. This was the first long-duration use of sodium in a microchannels (~1.8 mm hydraulic diameter) heat exchanger. The use of an oxide control system enabled trouble-free operation of the heat exchanger for over 150 h of high-temperature operation. This first-of-a-kind demonstration using liquid sodium and supercritical carbon dioxide shows great promise for further application of this technology in advanced nuclear or solar power plants.

42 ENGINEERING↗
DOE OSTI2023

Sustainable ammonia synthesis from nitrogen wet with sea water by single-step plasma catalysis

Ammonia synthesis at ambient conditions employing intermittent distributed green sources of energy and feedstocks is globally sought to replace the centralized Haber-Bosch (H-B) process operating at high temperature and pressure. We report herein for the first time an effective and sustainable ammonia synthesis pathway from N 2 wet with seawater vapor over spherical SiO 2 and M/SiO 2 (M: Ag, Cu, and Co) catalysts driven by non-thermal plasma (NTP). Experimental results indicate that the presence of a catalyst is required for ammonia production from seawater vapor and N 2 . The Co/SiO 2 catalyst delivered the highest ammonia synthesis rate (r NH 3 ) of 3.7 mmol g cat -1 h -1 and energy yield of 3.2 g NH 3 ∙kW -1 ∙h -1 at a relatively low input power of 2 W. The extraction of H atoms from H 2 O molecules plays an important role in the ammonia synthesis from seawater vapor. Finally, this work unfolds a novel platform for the subsequent optimization of sustainable ammonia production from endless resources such as seawater and N 2 through catalytic non-thermal plasma potentially powered by renewable sources.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2026

An experimental and kinetic modeling study of the ignition of 2-methyl decane

Ignition delay times (IDTs) of 2-methyl decane (C 11 H 24 -2) are measured in a high-pressure shock tube and in a rapid compression machine at equivalence ratios in the range 0.5–2.0 at 90 % dilution, at temperatures in the range 600–1430 K and at pressures of 15 and 30 bar. To clarify the effect of the branched methyl group on fuel oxidation, IDTs of n-undecane (nC 11 H 24 ) are also measured at similar conditions to those measured for C 11 H 24 -2. A new chemical kinetic mechanism, using C3MechV4.0.1 as the core chemistry, is developed and validated against the new experimental data. The thermodynamic properties of the fuel (RH), alkyl (Ṙ), alkyl peroxy (RȮ 2 ), hydroperoxy-alkyl (Q̇OOH), and peroxy hydroperoxy alkyl (Ȯ 2 QOOH) radicals are updated in both the C 11 H 24 -2 and nC 11 H24 models using THERM25. A reaction path flux analysis for C 11 H 24 -2 at different temperatures was conducted. Compared to nC 11 H 24 , C 11 H 24 -2 shows slower reactivity. At low and intermediate temperatures, the chain propagation pathway Q̇OOH ↔ C 11 cyclic ether + ȮH is favored for C 11 H 24 -2, while the chain branching pathway Q̇OOH ↔ Ȯ 2 QOOH ↔ C 11 carbonyl hydroperoxide (KHP) + ȮH is suppressed, leading to lower reactivity compared to nC 11 H 24 . At high temperatures, the presence of the branched methyl group inhibits the direct decomposition of the fuel, resulting in reduced C 2 H 4 formation, which in turn suppresses the reactivity of the fuel.

2-methyl decane↗
DOE OSTI2022

Experimental results of a magnetically coupled piezoelectric actuator to relieve microchannel heat exchanger maldistribution

Refrigerant maldistribution is a common issue in microchannel heat exchangers. Refrigerant maldistribution can have significant negative effects on the heat transfer performance and increase the pressure drop, leading to increased superheat temperature at the outlet and increased compressor work, lowering system efficiency. In this work, a novel piezoelectric-driven magnetic actuator (PEDMA) was fabricated and inserted into the inlet header of the microchannel evaporator, with the goal of improving the non-uniformity of the flow distribution by regulating the flow in the header to the microchannels. Two prototype PEDMA designs were tested and showed significant impact on the refrigerant flow in the region of actuation. In the first design, the experimental data showed superheat reductions up to 9 °C when the individual channel temperatures were measured. The second design redistributed the refrigerant such that a 1% increase in capacity was calculated for the whole heat exchanger without significantly impacting the heating efficiency. The experimental results demonstrate the successful operation of the PEDMA devices and represent a new method of active flow distribution control which is based on a simple design with minimal additional energy consumption, and which can be inserted into microchannel heat exchanger headers to potentially relieve the refrigerant maldistribution.

42 ENGINEERING↗
DOE OSTI2023

A Membrane Contactor Enabling Energy-Efficient CO 2 Capture from Point Sources with Deep Eutectic Solvents

We demonstrate a scalable and energy-efficient hollow fiber membrane contactor (HFMC)-based process using a green solvent for CO 2 capture. This process uses a deep eutectic solvent (DES) in an HFMC to provide close interfacial interactions and contact between the DES and CO 2 . This approach overcomes disadvantages associated with direct absorption in DES and could potentially be applied to a variety of solvent-based CO 2 capture methods. Commercial low-cost polymer hollow fiber membranes (e.g., microporous polypropylene) were evaluated for CO 2 capture with reline, a prototypical DES. Single-gas measurements showed that the DES-based polypropylene HFMC can capture and separate CO 2 while rejecting N2. From a mixed gas containing 50 mol % N 2 and 50 mol % CO ν , the DES-based HFMC separated CO 2 with a purity of 96.9 mol %. The effect of several process parameters including solvent flow rate, pressure, and temperature on the CO 2 separation performance was studied. The flux of the recovered CO 2 was 67.43 mmole/m 2 /h at a feed pressure of 4 bar. In situ Fourier transform infrared (FTIR) measurements combined with density functional theory (DFT)-based molecular dynamics simulations revealed that reline absorbs CO 2 by physical absorption without forming a new chemical compound, and CO 2 separation by reline occurs via the pressure swing mechanism. This research provides fundamental insights about physical solvent-based separation processes and a pathway toward practical deployment.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Laser-Assisted Synthesis of Monolayer 2D MoSe 2 Crystals with Tunable Vacancy Concentrations: Implications for Gas and Biosensing

We report tuning the structural and electronic properties of atomically thin two-dimensional (2D) materials via defect and vacancy engineering is the key to enabling their potential use in various applications, including electronics, energy, and sensing devices. Vacancies are, for instance, becoming highly promising for the enhanced interaction of gases and biomolecules with 2D materials in energy and sensing applications. However, the deterministic generation of desirable vacancies with tunable concentrations remains a challenge in 2D materials due to the limitations in the current growth methods, such as the complex reaction chemistries and gas flow dynamics. Therefore, engineering defects and vacancies in 2D materials have been mainly limited to destructive top-down processes such as heating, ion bombardments, and laser postprocessing. Here, we introduce a single-step bottom-up synthesis approach for the growth of monolayer MoSe 2 crystals with tunable vacancy concentrations. This method utilizes the spatiotemporal properties and adjustable power densities of the lasers to control the vaporization dynamics of the stoichiometric MoSe 2 powders. Such a mechanism in the vaporization allows us to grow tunable stoichiometry monolayer MoSe 2–x crystals on the substrates. The localized and time-controlled (250 ms to 2 s) vaporization of the MoSe 2 powder by a CO 2 laser enables the formation of monolayer crystals with controlled vacancy concentrations ranging from ~1 to 20%. The effects of laser power, laser irradiation time, and background pressure on the tuning range and subsequent properties of the crystals are investigated and quantified using Raman and photoluminescence spectroscopy, scanning transmission electron microscopy (STEM), and time-correlated single-photon counting (TCSPC). This bottom-up synthesis is a promising approach that allows the deterministic vacancy tuning for future electronics and, in particular, gas and biosensing applications without the need for further postprocessing and potential structural disruption of the crystals.

2D materials↗