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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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DOE OSTI2024

Uncertainty Propagation from Experiment Measurements to Modeling Approaches: A Case for SMR Steam Entrainment Testing

To license new and advanced reactor designs, regulators must be convinced that their unique safety cases—relative to existing large scale reactors—have been adequately addressed by the designed reactor protection systems. In water cooled small modular reactors (SMRs), droplet entrainment in steam flow has significant implications on the progression of accident scenarios due to its compact design features, which requires representative test data applicable to SMR designs. Computer code, modeling and simulation (M&S) tools and models require adequate verification, assessment, and qualification. This includes M&S results validation against scaled empirical data within allowable uncertainty bands to gain regulatory approvals during the various stages of reactor system design, demonstration, and commercialization. However, measurement uncertainty within the empirical datasets and test data applicability ranges requires careful consideration of M&S inputs (i.e., boundary conditions, and initial conditions), and verification and validation efforts. This study focuses on uncertainty quantification in designing scaled test facilities for SMR applications with appropriate measurements and a standard data-reduction method to estimate thermal hydraulics characteristics parameters that incorporate physics phenomena of interest. In addition, this study supports the evaluation model development and assessment process using M&S that interfaces with advanced computing tools and digital twin capabilities. This will allow synchronization between experiment and modeling approaches for droplet entrainment testing and analysis, improving diagnostics, prognostics, and decision-making to accelerate regulatory approval.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗
DOE OSTI2022

Exceptional Mineral Scaling Resistance from the Surface Gas Layer: Impacts of Surface Wetting Properties and the Gas Layer Charging Mechanism

Mineral scaling is a phenomenon that occurs on submerged surfaces in contact with saline solutions. In membrane desalination, heat exchangers, and marine structures, mineral scaling reduces process efficiency and eventually leads to process failure. Therefore, achieving long-term scaling resistance is beneficial to enhancing process performance and reducing operating and maintenance costs. While evidence shows that superhydrophobic surfaces may reduce mineral scaling kinetics, prolonged scaling resistance is limited due to the finite stability of the entrained gas layer present in a Cassie–Baxter wetting state. Additionally, superhydrophobic surfaces are not always feasible for all applications, but strategies for long-term scaling resistance with smooth or even hydrophilic surfaces are often overlooked. In this study, we elucidate the role of interfacial nanobubbles on the scaling kinetics of submerged surfaces of varied wetting properties, including those that do not entrain a gas layer. We show that both solution conditions and surface wetting properties that promote interfacial bubble formation enhances scaling resistance. In the absence of interfacial bubbles, scaling kinetics decrease as surface energy decreases, while the presence of bulk nanobubbles enhances the scaling resistance of the surface with any wetting property. The findings in this study allude to scaling mitigation strategies that are enabled by solution and surface properties that promote the formation and stability of interfacial gas layers and provide insights to surface and process design for greater scaling resistance.

calcite↗
DOE OSTI2021

Topical Report – Findings on Subtask 2.7 – Wet ESP and Aerosol Testing at Coal Creek Station

Growing concerns over the impact of CO 2 emissions from combustion sources on global climate change have prompted numerous research and development projects aimed at developing cost-effective technologies for CO 2 capture. One family of technologies being demonstrated at pilot and full scale globally is postcombustion carbon capture (PCCC) systems that employ amine-based solvents. The captured CO 2 can be compressed and permanently stored underground or used for enhanced oil recovery. The proximity of North Dakota’s lignite-fired fleet of power plants to potential CO 2 storage options creates a unique atmosphere for PCCC within the state. However, the unique components present in lignite flue gas present a challenge for large-scale PCCC at North Dakota power plants by contributing to aerosol formation. Aerosols can negatively impact the long-term performance of amine-based solvents for CO 2 capture. Amine-based solvents are volatile, and flue gas particulate provides nucleation sites where amine vapors can condense as aerosols. Because aerosols cannot be easily captured at the column outlet using conventional technologies, the amine-laden aerosols escape the system and lead to accelerated solvent losses. Moreover, particulate components can chemically react with amines to form degradation products that can permanently deactivate the amine, cause fouling, and lead to hazardous emissions. Many of the elements that have been shown to catalyze solvent degradation are present in lignite coals and can exacerbate solvent replacement economics. Understanding this issue is critical to the implementation of solvent-based CO 2 capture systems as applied to lignite-fired generation systems. The Energy & Environmental Research Center (EERC) designed and carried out this project to fully characterize aerosol behavior with various control technologies installed to better optimize aerosol mitigation technology for CO 2 capture. To meet the goal of this project, the following objectives were identified: Determine the effectiveness of a wet electrostatic precipitator (WESP) on mitigating formation of problematic aerosols at Great River Energy’s Coal Creek Station, upstream of the PCCC system. Determine the effectiveness of the Mitsubishi Heavy Industries (MHI) proprietary amine emission reduction unit (AERU) as a postcapture solvent recovery system for reducing aerosol emissions and extending solvent life downstream of the PCCC system. Determine the impact of aerosols on the efficiency and degradation products of both commercial and advanced solvents within the PCCC system. Work was conducted at Coal Creek Station Unit 1 using a slipstream of flue gas from the outlet of the plant’s flue gas desulfurization (FGD) unit. Flue gas was routed through a pilot-scale FGD unit to remove SO 2 to very low levels (~1 ppm) and then through a direct contact cooler (DCC) to further cool the gas and to remove moisture. The gas exiting the DCC was then optionally routed through a WESP before passing to the CO 2 absorber columns. The MHI solvent was used to scrub CO 2 from the slipstream through a set of two absorber columns. The rich solvent was regenerated in a stripper column by heating to drive off captured CO 2 . Flue gas exiting the absorber column was routed to MHI’s proprietary AERU to recover entrained solvent. The system operated using a catch-and-release method where the CO 2 was separated to provide data on the process, but the captured CO 2 was released back into the host site stack. Particulate was measured, collected, and analyzed from multiple locations throughout the pilot-scale system. Unlike the performance observed in prior work, the inlet FGD and DCC did not remove significant particulate matter from the flue gas. This appears to be due to a difference in the nature of the particulate. The DCC seemed to increase particulate size and count, most likely owing to water condensing onto the surfaces of fly ash particles. When the WESP was operated, it achieved >95% particulate capture. Very little particulate matter or indications of solvent were detected at the AERU outlet. When operating with advanced KS 21 solvent, the particulate material at the AERU outlet was even further decreased. Solvent analysis showed that some species derived from flue gas and ash were slowly concentrating in the solvent over the duration of the test. The levels observed were reported to be within expected ranges and were not of concern to MHI. A high-level techno-economic assessment of installing CO 2 capture at Coal Creek Station suggested that, when using a standard monoethanolamine (MEA)-based solution with simple heat integration, the energy penalty to net generation would be 34%. The bulk of this was due to steam losses for regenerating solvent, followed by parasitic electrical demand for CO 2 compression and then by increased parasitic load for pushing flue gas through the absorber column. These demands could be decreased with a more advanced solvent that exhibits lower heat of regeneration and lower pressure drop than does a simple MEA solution. Further energy could be saved with more thorough heat integration to recover useful energy from the steam used for solvent regeneration. Installing a WESP was predicted to increase the cost of electricity by nearly $5/MWh. This would become cost-effective if solvent losses were roughly 10 times the baseline estimate when not using a WESP but could be returned to baseline by installing the WESP. Piping CO 2 for storage in more favorable geology could help with carbon capture and storage economics. Although storing off-site would necessitate construction of a CO 2 transport pipeline, the cost of this pipeline might be more than offset by reducing the number of wells required, the depths of the wells required, and the electrical demand for the CO 2 compressor. Additional factors that favor off-site storage costs include smaller expected CO 2 plume sizes, which translates to less monitoring and fewer landowner agreements. More detailed assessment of the specific geology in the region under and around Coal Creek Station would be needed to accurately assess the costs and benefits of different storage site options. This subtask was cofunded through the Energy & Environmental Research Center–U.S. Department of Energy Joint Program on Research and Development for Fossil Energy-Related Resources Cooperative Agreement No. DE-FE0024233. Nonfederal funding was provided by the North Dakota Industrial Commission.

Strege, Joshua↗
DOE OSTI2021

Characterizing major and trace element compositions in fallout melt glass from a near-surface nuclear test

We report the chemical and isotopic compositions of fallout melt glasses from nuclear tests contain a range of information constraining the physical conditions within the fireball and the mechanisms of fallout formation but historic studies tended to exclude the behavior of stable major and trace elements. Here, we present a large study specifically focused on major and trace element relationships within a population of macroscale fallout samples from a single event. We interpret these data to better constrain how fallout melt glass formation in near surface environments is influenced by that environment and demonstrate how major and trace element abundances can provide useful insights into chemical processes within the fireball. Data confirm that the uranium in the fallout glass population derives from two isotopically distinct endmembers: isotopically enriched uranium (presumably from the weapon), and natural composition uranium that may be a combination of anthropogenic and environmental materials from within the blast zone. The similarity between major and trace element concentrations in fallout and corresponding local soils from the event site confirm the local soils as the most probable source of entrained material into the fireball and the source of carrier material into which the bomb vapor was incorporated. The lack of correlation between major and trace element abundances with size indicates that volatility driven processes, such as condensation from the fireball, do not control the composition of macroscale fallout melt glass. Although the fallout has major and trace element chemical characteristics broadly similar to those of the local, associated soils, some systematic differences are observed between the two populations. Fallout melt glass is depleted in volatile elements such as K, Na, Tl and Pb, consistent with heating to temperatures above ~1000 °C for 3-10 s. This is supported by the results of laser heating experiments performed on rhyolitic soil at temperatures (1600-2200 °C) and timescales (1-120 s) that are broadly relevant to fallout formation conditions. Relative enrichments of metals such as Cu and Co do not correlate with the abundance of uranium, suggesting that fallout also records input of near field anthropogenic materials. Our observations suggest that major chemical features can be related to processing in the fireball and used to inform the thermal-chemical evolution of the system. Ultimately, these data are consistent with a fallout formation mechanism that involves rapid melting of surface materials to form carrier material melts with minor incorporation of bomb vapor and a degree of volumetric volatile loss due to heating.

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

Prognostic simulations of mixed-phase clouds with model AC-1D v1.0: the impact of aerosol types and freezing parameterizations on ice crystal budgets

Mixed-phase clouds at high latitudes contribute to the uncertainty in predicting cloud feedbacks and climate sensitivity, mainly due to the complexity of microphysical processes that influence the partitioning between the supercooled liquid and ice phases, and hence, cloud radiative effects on regional scales. Particularly in Arctic mixed-phase clouds, the activation of ice-nucleating particles (INPs) from various aerosol populations remains a leading source of uncertainty. We developed an aerosol-cloud one-dimensional (AC-1D) model, which provides a novel framework to prognostically treat INP and ice crystal budgets while explicitly accounting for polydisperse and multicomponent aerosol that activate INPs following different freezing parameterizations. The AC-1D model is informed by large-eddy simulations to probe the impact of INP representation on predicted ice crystal number concentrations (N i ) and ice crystal budgets in mixed-phase Arctic stratus. We apply three immersion freezing (IMF) parameterizations, two time-independent (singular) and one time-dependent (classical nucleation theory), to predict the evolution of the INP reservoir and resulting ice crystal budget from polydisperse mineral dust, organic (humic-like substances), and sea spray aerosol particle size distributions. Our analysis focuses on how variations in aerosol number concentration and cloud system parameters such as cloud cooling rate, cloud-top entrainment rate, and ice crystal fall speed influence the INP reservoir and ice crystal budgets. Furthermore, this study investigates the competitive ice nucleation dynamics in mixed aerosol environments and provides a process-level quantification of the INP budget terms, which directly controls ice crystal budgets. For all studied case scenarios, the aerosol types and associated particle size distributions significantly impact INP and N i , and the choice between a time-dependent and a singular freezing description yields orders-of-magnitude differences in the predicted INP and N i over the 10 h simulation time, reflecting typical cloud lifetimes. Our results show that the influence of cloud cooling, INP entrainment, and sedimentation varies significantly depending on the chosen freezing parameterization. These findings underscore the critical need for robust IMF parameterizations and precise cloud system observations to enhance the accuracy of models in predicting mixed-phase cloud structure and evolution.

Arctic clouds↗
DOE OSTI2023

Technical Evaluation of Accelerated Basin De-Inventory Material Addition to Sludge Batch 11 (Rev. 1)

The Accelerated Basin De-inventory (ABD) program involves discarding spent nuclear fuel that is currently stored in L-Basin to the Defense Waste Processing Facility (DWPF) for vitrification. The first ABD discards will occur during the preparation of Sludge Batch (SB) 11. Savannah River Mission Completion has requested that the Savannah River National Laboratory assess the technical gaps related to the increased gadolinium poisoning requirement and the impacts of performing the Low Temperature Aluminum Dissolution (LTAD) process in Tank 51 with H-Canyon discards present. The following summarizes the evaluation of the impacts of increasing the quantity of gadolinium (and related topics) from what was previously evaluated in the SRNL studies of gadolinium-poisoned ABD material solubility, the overall ABD flowsheet review, and increasing the fissile mass loading in glass: 1) Based on literature surveys, there is no indication that organic interactions with gadolinium will be significant at the high pH (typically >13) conditions of the Concentration, Storage, and Transfer Facilities. Any interactions of gadolinium with organics in DWPF are not expected to adversely impact DWPF or downstream facilities. Thus, there is little-to-no residual risk from organic interactions with gadolinium [Gap closed]; 2) Adding depleted uranium to ABD material, targeting 235 U enrichment of 4.90% within each transfer window, will mitigate potential impacts from an increase in soluble 235 U enrichment during sludge washing and LTAD. The plan to take advantage of previous transfers and allow 235 U enrichment of >5% during the final transfer window carries a risk that Tank 51 supernate will have a 235 U enrichment of >5%, which should be evaluated for acceptance; 3) Increasing the gadolinium mass ratio to 3.0:1 Gd: 235 U(eq SLU ) should lead to the same or higher partitioning of gadolinium into the solid phase within the DWPF Chemical Process Cell, resulting in both liquid and solid phases with expected partitioning of Gd consistent with the prior solubility study [Gap closed for SB11]; 4) There are no expected impacts on DWPF melt temperature and melter operations due to the minimal ~0.2 weight percent (wt%) increase in Gd concentration relative to previous sludge batches [Gap closed for SB11]; 5) As observed previously, Gd is expected to enter the off-gas system via physical entrainment, but at a slightly higher concentration than what was observed for SB9 melter off-gas pluggage deposits (0.07 wt%) [Gap closed for SB11] ; 6) There are no expected impacts on DWPF recycle or the Recycle Collection Tank glycolate destruction process. [Gap closed for SB11]; 7) Gd is projected to be a trace component in the SB11 glass (<0.5 wt%) and can be ignored for process control. Trace components do not significantly impact glass durability, thus the conclusions of the previous Product Consistency Test evaluation at a fissile mass loading of 2,500 g fissile/m3 glass still applies to SB11. The ~0.1 wt% increase in Gd2O3 concentration relative to the previous study will not impact the predictability of SB11 glass with the DWPF Product Composition Control System (PCCS) models for durability or the acceptability of glass according to the Waste Acceptance Product Specifications (WAPS) criterion for product consistency [Gap closed for SB11]; 8) No additional Toxicity Characteristic Leaching Procedure testing is necessary for SB11 and the hazardous waste specification of the SB11 DWPF waste form is unchanged after the addition of the ABD stream [Gap closed for SB11]. The following summarizes the evaluation of the impacts of adding two-thirds of the ABD material to Tank 51 prior to LTAD: 1) The addition of two-thirds of the ABD increases overall aluminum mass from 1.39×10 4 kg to 1.64×10 4 kg (15.5% ABD Al). The form of the insoluble portion of the Al resulting from ABD addition should be the more readily dissolved Al(OH) 3 and amorphous forms. The portion of the ABD aluminum that is processed by LTAD is expected to be completely soluble, thus requiring that less of the boehmite in the sludge be dissolved to reach the same Al target in the SB. [Gap closed for SB11]; The expected LTAD impact on other components, as related primarily to the components in ABD, are discussed. Gd is expected to remain insoluble during LTAD and not impact the solubility of other components. [Gap closed for SB11]; The addition of two-thirds of the ABD increases overall projected SB11 uranium mass from 4,740 kg to 13,100 kg (63% ABD U) and the projected plutonium mass from 86.0 kg to 89.5 kg (3.9% ABD Pu). The addition of all of the ABD increases overall projected SB11 uranium mass from 4,740 kg to 16,100 kg (70% ABD U) and the projected plutonium mass from 86.0 kg to 90.4 kg (5.3% ABD Pu). The 235 U enrichment will be ≤5%. The fissile uranium will be adequately poisoned by Gd and the fissile Pu will be adequately poisoned by Fe from the sludge. [Gap closed for SB11]; There is a low risk that ABD addition will impact the rheology or pumpability of the slurry. There is a low but higher risk of ABD addition prior to LTAD impacting the settling rate; Based on the evaluation of adding two-thirds of the ABD material and all of the ABD material prior to the LTAD process, there is no volume or mass limit that would need to be imposed on ABD additions prior to LTAD. [Gap closed for SB11]. Revision 1 of this report addresses a variation on the ABD additions and LTAD strategy where sodium hydroxide additions for LTAD may be performed intermittently or concurrently with an ABD addition window. The proposed change does not alter the conclusions of this evaluation.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2022

Off-Gas Design and Testing from Advanced Chlorination Process

Chlorination of Zr alloy cladding with sulfur-chloride reagents is being considered as a means of separating the main metal from alloying elements, imbedded U, actinides, and fission and activation products to purify the Zr. This would allow the Zr to be disposed of as low-level nuclear waste or possibly be recycled. A multistage process was developed that involves several steps and waste streams. Recycling of sulfur-chloride reagents S 2 Cl 2 and SOCl 2 is planned to minimize the waste stream. The generation of off-gas and entrainment of volatiles is anticipated to be minimized. However, given the complex nature of spent nuclear fuel (SNF), some volatile components will be generated, including the solvents themselves; Cl 2 used for the regeneration of S 2 Cl 2 ; volatile fission product chlorides, such as Sb and 3 H; and chlorinated alloying components, such as Sn, Nb, Fe, and Mo. This report discusses the chemical phenomena that might give rise to volatile species and their planned capture. The volatility of the transition metals will depend on their oxidation state and the compounds that are formed, such as Zr tritide. Loading radionuclides in the process off-gas will depend on the inputs to the process. For instance, processing separated Zr to reduce waste will have a much lower loading of radionuclides than if alternative chlorination were used for decladding SNF. Much of the volatile process streams will be part of the solvent recycling, which may involve online scrubbing. Generally, a caustic scrubber should be included in the off-gas to remove acidic vapors (e.g., Cl 2 , SOCl 2 ). The decontamination procedures for removing these species could involve pretreatment (i.e., heating) options or reduction by contact with H 2 . This report discusses these options along with a framework for testing these alternatives in future experiments. Technologies for off-gas capture will leverage those developed in the Materials Recovery and Waste Forms program.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2020

Frequency domain measurements of melt pool recoil force using modal analysis

Recoil pressure is a critical factor affecting the melt pool dynamics during Laser Powder Bed Fusion (LPBF) processes. Recoil pressure depresses the melt pool. When the recoil pressure is low, thermal conduction and capillary forces may be inadequate to provide proper fusion between layers. However, excessive recoil pressure can produce a keyhole inside the melt pool, which is associated with gas porosity. Direct recoil pressure measurements are challenging because it is localized over an area proportionate to the laser spot size producing a force in the mN range. This paper reports a vibrationbased approach to quantify the recoil force exerted on a part in a commercial LPBF machine. The measured recoil force is consistent with estimates from high speed synchrotron imaging of entrained particles, and the results show that the recoil force scales with applied laser power and is inversely related to the laser scan speed. These results facilitate further studies of melt pool dynamics and have the potential to aid process development for new materials.

42 ENGINEERING↗
DOE OSTI2022

Particle trapping, size-filtering, and focusing in the nonthermal plasma synthesis of sub-10 nanometer particles

Low-pressure nonthermal flowing plasmas are widely used for the gas-phase synthesis of nanoparticles and quantum dots of materials that are difficult or impractical to synthesize using other techniques. To date, the impact of temporary electrostatic particle trapping in these plasmas has not been recognized, a process that may be leveraged to control particle properties. Furthermore, we present experimental and computational evidence that, during their growth in the plasma, sub-10 nm silicon particles become temporarily confined in an electrostatic trap in radio-frequency excited plasmas until they grow to a size at which the increasing drag force imparted by the flowing gas entrains the particles, carrying them out of the trap. We demonstrate that this trapping enables the size filtering of the synthesized particles, leading to highly monodisperse particle sizes, as well as the electrostatic focusing of the particles onto the reactor centerline. Understanding of the mechanisms and utilization of such particle trapping will enable the design of plasma processes with improved size control and the ability to grow heterostructured nanoparticles.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2026

Understanding the causes of satellite–model discrepancies in aerosol–cloud interactions using near-LES simulations of marine boundary layer clouds

Aerosol–cloud interactions (ACI) remain the largest source of uncertainty in model estimates of anthropogenic radiative forcing, primarily because of deficiencies in representing aerosol–cloud microphysical processes that lead to inconsistent cloud liquid water path (LWP) responses to aerosol perturbations between observations and models. To investigate this discrepancy, we conducted a series of large-eddy-scale simulations driven by realistic meteorology over the eastern North Atlantic, and evaluated LWP susceptibility, precipitation processes, and boundary layer thermodynamics using satellite and ground-based observations. Simulated LWP responses show a strong dependence on cloud state. Non-precipitating thin clouds exhibit a modest LWP decrease with increasing cloud droplet number concentration (N d ), consistent in sign but weaker in magnitude than satellite estimates, reflecting enhanced turbulent mixing and evaporation. The largest model-observation discrepancy occurs in non-precipitating thick clouds, where simulated LWP susceptibilities are strongly positive (+0.32) while observations indicate large negative values (−0.69). This discrepancy stems from excessive precipitation driven by underestimated entrainment, overly active accretion, and overly broad drop-size distributions in polluted conditions. While our high-resolution setup mitigates the excessive drizzling common in coarser models and captures key regime transitions, these biases persist – highlighting that improved parameterizations of cloud-top processes, precipitation, and aerosol effects are needed beyond simply increasing model resolution. Additionally, misrepresented moisture inversions in reanalysis introduce a moist bias in cloud-top relative humidity, further amplifying positive LWP susceptibility. Our results also suggest that large negative N d –LWP relationships in observations may reflect internal cloud processes rather than true ACI effects.

Aerosol-cloud interaction↗
DOE OSTI2026

Dual-loop Solvent-based CCS for Net Negative CO 2 Emissions with Lower Cost

This final technical report details the successful design, construction, and operational validation of an innovative dual-loop CO 2 capture technology designed to achieve deep decarbonization (>99%) from Natural Gas Combined Cycle (NGCC) power plants that results in the electricity with carbon intensity of approximate 42 kg CO 2 -eq/MWh, less than the electricity produced by solar PV. The integrated process couples a primary aqueous solvent (in this project, a water lean solvent – WLS) absorption loop for bulk CO 2 removal with a secondary potassium hydroxide (KOH) polishing loop featuring electrochemical regeneration. This architecture leverages the higher exergy efficiency of the primary loop while utilizing the fastest kinetic of the secondary loop to capture dilute residual CO 2 , achieving an overall capture rate of 99.9% and co-producing pure hydrogen after moisture being condensed and dehydrated. Technical feasibility was established through a comprehensive 2,000-hour experimental campaign on a bench-scale fully-integrated unit (using 4” absorber and 4” stripper) with the feeding flue gas flowrate in the range of 8-20 cfm, confirming the attainment of Technology Readiness Level (TRL) 4. The project executed extensive parametric testing followed by 1,000 hours of continuous steady-state testing, demonstrating exceptional process stability with the electrochemical regenerator exhibiting less than a 10% reduction in electrical conductivity over the duration of the campaign. Operational characterization gathering on the bench unit revealed distinct energy profiles for the hybrid system: the primary loop required approximately 280 kJ mol -1 for bulk removal, while the polishing loop required approximately 1,600 kJ mol -1 specifically when reducing dilute CO 2 concentrations from ~740 ppm down to <50 ppm. (Please note those energy values/numbers can only be viewed as relative relationship and should not be extrapolated as absolute values required for CO 2 capture). Furthermore, dynamic testing validated the system’s flexibility for utility applications, demonstrating a rapid process response time of <30 minutes to changes in flue gas flowrate. Emission monitoring confirmed that the dual-loop architecture effectively mitigates solvent losses, utilizing a water wash to remove entrained aerosols to <1 ppm. The Techno-Economic Analysis (TEA) indicates a cost of capture of $\$$59.3/tonne and a Levelized Cost of Electricity (LCOE) of 71.7 $\$$/MWh at the overall capture efficiency of 99.8% of total carbon in the flue gas stream, with sensitivity analysis identifying an economic optimum when the primary loop captures 97% of the total CO 2 . A Life Cycle Assessment (LCA) confirms the technology’s potential for net-negative emissions, determining a Global Warming Potential (GWP) of 52 kg CO 2 -eq/MWh—significantly lower than the baseline—which further decreases to 42 kg CO 2 -eq/MWh when crediting the displacement of conventional hydrogen production.

03 NATURAL GAS↗
DOE OSTI2022

Ion Exchange Processing of AP-105 Hanford Tank Waste through Crystalline Silicotitanate in a Staged 2- then 3-Column System (Rev.1)

The Tank Side Cesium Removal (TSCR) system, under development by Washington River Protection Solutions LLC (WRPS), will send initial low-activity Hanford waste tank supernate feeds to the Hanford Waste Treatment and Immobilization Plant (WTP) Low-Activity Waste (LAW) Facility. In addition to entrained solids removal from the supernate, the primary goal of TSCR is to remove cesium-137 ( 137 Cs) by ion exchange, allowing contact handling of the liquid effluent product at the WTP. Crystalline silicotitanate (CST) ion exchange media, manufactured by Honeywell UOP, LLC (product IONSIVTM R9140-B), was selected as the ion exchange media at TSCR. CST is a non-elutable inorganic material that has demonstrated robust chemical, physical, and radiation tolerance while maintaining functionality. However, exchange kinetics of Cs onto CST is slow, resulting in low utilization of the CST Cs load capacity before unacceptable Cs breakthrough. Two process flow designs have been tested, as follows. 1. Lead-lag column processing: The lead column was removed after the lag column effluent reached the waste acceptance criteria (WAC) limit, the lag column was moved into the lead position, and a new lag column was installed. This format used ~52% Cs load capacity on the lead column. 2. Lead-lag-polish column processing: The processing was stopped when the polish column effluent reached the WAC limit. This format resulted in 81% Cs load capacity on the lead column. Testing with diluted feed from Hanford tank AP-105 (AP-105DF) incorporated a nuanced change to the lead-lag-polish column system where the polish column was inserted when the lag column effluent reached WAC limit. A 10.9-L volume of AP-105DF (diluted to 5.6 M Na) was processed through the Direct Feed Test Platform system, established at Pacific Northwest National Laboratory to support small-scale waste qualification efforts. The columns consisted of 10-mL CST beds (CST Lot 2002009604, sieved to screen out >30-mesh particles) placed in 1.5-cm-inner-diameter columns. Feed was processed at 1.83 bed volumes (BV) per hour; the flowrate, in terms of contact time with the CST bed, matched the expected flowrate at TSCR. The <30-mesh CST sieve cut was expected to provide appropriate performance scaling to a full-height column. The installation of the polish column later in processing (after processing 523 BVs) did not appear to fundamentally change the utilization of the lead column for Cs exchange nor did it extend the total feed processing volume when compared to the previous test with AP-107 feed. Table ES.1 and Figure ES.1 summarize the measured AP-105DF Cs load performance.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2020

Initial Atmospheric Transport of Particles

A new version of the Initial Atmospheric Transport (IAT) model has been developed. This report fully characterizes the new model. IAT is designed to model heat release into the atmosphere that contains contaminated particles. The heat release forms a buoyant puff or plume. Buoyancy is quickly dissipated in 10's to 100's of seconds through drag and entrainment of ambient air. The final location of contaminant particles in the atmosphere after dissipation of abnormal heat is an important input to long term transportation codes such as the National Oceanic and Atmospheric Administration's (NOAA) Hybrid Single Particle Lagrangian Integrated Trajectory (HYSPLIT) code. Ultimately the settling of contaminants after long term transport provides a basis for estimating health consequences. In comparison to the old version, the new model includes explicit simulation of particles, newly formulated equations of motion for a rising puff, and a new plume model. The plume model releases many instances of a single puff along a single trajectory in a way that balances energy released over a longer period than would be appropriate for a single puff. The puff model has additions for vorticity, turbulence, virtual mass, drag, and entrainment. The particle model leads to direct interfacing between IAT and the long-term transport code HYSPLIT. Previously, particle locations were given a pattern based on IAT's puff trajectory with no particle simulation. Now, particles are explicitly simulated, and 3-D spatial distributions of particles are output based on final positions. Ballistic particles are thrown outward at high velocity from explosive events and tend to hit the ground before the end of the simulation. Non-ballistic particles tend to get pulled into the rising puff s ring of vorticity with some escaping to ambient conditions as buoyant energy dissipates. A new model verification and validation effort was made for the new plume model. The Wallops Island Solid Rocket Propellant (SRP) fire plume was extracted to a 3-D transient dataset. After calibration, the model performs better than previous single puff attempts. Even so, error levels in the process used to estimate location and ambient weather conditions approach 30%. This leads to the conclusion that unplanned photogrammetry evaluations of the IAT model are useful but not sufficiently accurate to quantify model parameters. Like previous attempts, the vertical motion entrainment parameters come out much too high in comparison to values for other studies in the literature. It is suspected that a new model of shear entrainment would alleviate this problem. Unfortunately, IAT already has more calibration parameters than the data comparisons thus far can resolve with statistical certainty. This underscores the need to verify and validate the IAT model using detailed CFD studies that allow ideal statistical comparison with the IAT model for hundreds of cases. Even so, validation by comparison to carefully planned experiments (i.e. with acceptable error levels) is also necessary because the dynamics of entrainment are at a sub-grid level for CFD. Though better validation and verification are most important, many new enhancements are still envisioned for future IAT development. These include particle rain out due to condensation and agglomeration of water, direct connection to the North American Mesoscale (NAM) weather dataset, dynamic weather conditions, including ambient particle entrainment into the puff, and detrainment at the puff to ambient mixing interface. In general, including detailed aerosol dynamics is the greatest coming challenge which will require an entire new sub-model in IAT. This is very important if contaminant particles change in such a way that they increase or decrease in their potential harm to the environment.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2023

Enabling Entrained-Flow Gasification of Blends of Coal, Biomass and Plastics (Final Report)

This project demonstrated the technical feasibility of gasifying blends of coal, biomass and mixed waste plastics in a high pressure entrained-flow gasifier for production of hydrogen. This was achieved by creating slurries of coal, biomass pyrolysis liquids and liquefied plastic oil. Specific objectives of the project included (1) determining compositions of coal-biomass-plastic mixtures that produce a stable slurry suitable for pumping to high pressure, (2) designing and testing a novel burner to effectively atomize the mixed feedstock slurry in a pressurized gasifier, and (3) acquiring first-of-a-kind performance data for pressurized, oxygen-blown entrained-flow gasification of slurried blends of coal, biomass and plastic. A key focus of the project was preparation of mixtures of coal, biomass and plastic. To facilitate easy pumping to high pressure, slurries were created using (i) bioliquid resulting from a well-established rapid thermal treatment pyrolysis process, (ii) oil produced from waste plastic via an available thermal conversion process, and (iii) ground coal. Lab-scale tests were conducted to evaluate viscosity and stability/propensity for the mixtures to separate over time. Larger batches of the most promising slurry compositions were prepared and subjected to pumping studies. It was found that mixtures containing less than about 40% coal and less than about 30% plastic oil were stable and of low enough viscosity to facilitate pumping to high pressure. A high-performance hot oxygen burner (HOB) was designed and fabricated for use in an existing 1 ton/day pressurized entrained-flow gasifier. Ex-situ testing demonstrated that the HOB provides excellent atomization of the slurries and creates a very uniform and robust flame. Performance of the HOB in the gasifier was exceptional and resulted in better conversion to syngas than any previous generation of burner. Fabricating the HOB for this project was challenging due to the relatively small scale of the gasifier. Performance in larger-scale systems is expected to be even better. Gasification of mixtures of coal, bioliquid and plastic oil proved to be relatively easy. The gasifier was able to be started up, pressurized and transitioned to the blended slurry feedstock with no technical difficulty. Syngas rich in CO and H 2 , with relatively low concentrations of CO 2 , was produced. During startup and at low gasification temperatures, soot formation was observed, as is typical for gasification of petroleum-based feedstocks. No slag buildup was observed under the conditions tested. The project was successful in demonstrating the technical feasibility of the concept. Future development should broaden the range of feedstocks under consideration, more deeply explore performance of the gasifier, and evaluate scale-up and implementation strategies.

08 HYDROGEN↗
DOE OSTI2024

The Physics behind Precipitation Onset Bias in CMIP6 Models: The Pseudo-Entrainment Diagnostic and Trade-Offs between Lapse Rate and Humidity

Conditional instability and the buoyancy of plumes drive moist convection but have a variety of representations in model convective schemes. Vertical thermodynamic structure information from Atmospheric Radiation Measurement (ARM) sites and reanalysis (ERA5), satellite-derived precipitation (TRMM3b42), and diagnostics relevant for plume buoyancy are used to assess climate models. Previous work has shown that CMIP6 models represent moist convective processes more accurately than their CMIP5 counterparts. However, certain biases in convective onset remain pervasive among generations of CMIP modeling efforts. Here we diagnose these biases in a cohort of nine CMIP6 models with sub-daily output, assessing conditional instability in profiles of equivalent potential temperature θ e and saturation equivalent potential temperature θ es in comparison to a plume model with different mixing assumptions. Most models capture qualitative aspects of the θ es vertical structure, including a substantial decrease with height in the lower free troposphere associated with the entrainment of subsaturated air. We define a “pseudo-entrainment” diagnostic that combines subsaturation and a θ es measure of conditional instability similar to what entrainment would produce under the small-buoyancy approximation. This captures the trade-off between larger θ es lapse rates (entrainment of dry air) and small subsaturation (permits positive buoyancy despite high entrainment). This pseudo-entrainment diagnostic is also a reasonable indicator of the critical value of integrated buoyancy for precipitation onset. Models with poor θ e /θ es structure (those using variants of the Tiedtke Scheme) or low entrainment runs of CAM5, and models with low subsaturation, such as NASA-GISS, lie outside the observational range in this diagnostic.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2020

Summertime Post-Cold-Frontal Marine Stratocumulus Transition Processes over the Eastern North Atlantic

Abstract Marine boundary layer (MBL) cloud morphology associated with two summertime cold fronts over the eastern North Atlantic (ENA) is investigated using high-resolution simulations from the Weather Research and Forecasting (WRF) Model and observations from the Atmospheric Radiation Measurement (ARM) ENA Climate Research Facility. Lagrangian trajectories are used to study the evolution of post-cold-frontal MBL clouds from solid stratocumulus to broken cumulus. Clouds within specified domains in the vicinity of transitions are classified according to their degree of decoupling, and cloud-base and cloud-top breakup processes are evaluated. The Lagrangian derivative of the surface latent heat flux is found to be strongly correlated with that of the cloud fraction at cloud base in the simulations. Cloud-top entrainment instability (CTEI) is shown to operate only in the decoupled MBL. A new indicator of inversion strength at cloud top that employs the vertical gradients of equivalent potential temperature and saturation equivalent potential temperature, which can be computed directly from soundings, is proposed as an alternative to CTEI. Overall, results suggest that the deepening–warming hypothesis suggested by Bretherton and Wyant explains many of the characteristics of the summertime postfrontal MBL evolution of cloud structure over the ENA, thereby widening the phase space over which the hypothesis may be applied. A subset of the deepening–warming hypothesis involving warming initially dominating over moistening is proposed. It is postulated that changes in climate change–induced modifications in cold-frontal structure over the ENA may be accompanied by coincident changes in the location and timing of MBL cloud transitions in the post-cold-frontal environment.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2021

Low-Level Mesoscale and Cloud-Scale Interactions Promoting Deep Convection Initiation

Data from scanning radars, radiosondes, and vertical profilers deployed during three field campaigns are analyzed to study interactions between cloud-scale updrafts associated with initiating deep moist convection and the surrounding environment. Three cases are analyzed in which the radar networks permitted dual-Doppler wind retrievals in clear air preceding and during the onset of surface precipitation. These observations capture the evolution of (i) the mesoscale and boundary layer flow, and (ii) low-level updrafts associated with deep moist convection initiation (CI) events yielding sustained or short-lived precipitating storms. The elimination of convective inhibition did not distinguish between sustained and unsustained CI events, though the vertical distribution of convective available potential energy may have played a role. The clearest signal differentiating the initiation of sustained versus unsustained precipitating deep convection was the depth of the low-level horizontal wind convergence associated with the mesoscale flow feature triggering CI, a sharp surface wind shift boundary, or orographic upslope flow. The depth of the boundary layer relative to the height of the LFC failed to be a consistent indicator of CI potential. Widths of the earliest detectable low-level updrafts associated with sustained precipitating deep convection were ~3–5 km, larger than updrafts associated with surrounding boundary layer turbulence (~1–3 km wide). It is hypothesized that updrafts of this larger size are important for initiating cells to survive the destructive effects of buoyancy dilution via entrainment.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2021

Method for removing a foulant from a gas stream without external refrigeration

A process for removing a foulant from a gas stream is disclosed. The gas stream, containing a foulant, is cooled across a first heat exchanger and a second heat exchanger, producing a solid foulant entrained in cryogenic liquid as a foulant slurry, and a foulant-depleted gas stream. The foulant-depleted gas stream is passed through a cryogenic turbine and a first separation vessel, producing a light gas stream and further solid foulant. The solid foulants are recovered by a combination of pressurization, melting, and distillation to produce a liquid foulant product. Heat is recovered from the various streams in the various heat exchangers and the melter.

Baxter, Larry↗