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Fast Response Temperature by airborne measurements over BNF

The original data were collected during the AAF Engineering Flights (AEF2025) in the vicinity of the ARM Bankhead National Forest (BNF) Atmospheric Observatory (https://www.arm.gov/capabilities/observatories/bnf ) in northwestern Alabama in March 2025. The ARM Aerial Facility ArcticShark uncrewed aerial system (UAS, https://www.arm.gov/capabilities/observatories/aaf/uas) was based at the public-use airport of Posey Field, Alabama (FAA LID: 1M4, 34.28027778° N, 87.60055556° W, 283m MSL) from March 9 through March 24, 2025. The ArcticShark UAS performed nine flights, including eight research flights over the AMF3 (BNF Main Site) and Supplemental Facilities to measure atmospheric state, turbulence, surface IR temperature and imagery, and aerosol number concentration and size distribution. The current data set presents fast response temperature in the atmospheric boundary layer and lower free troposphere measured on the airborne platform throughout the field campaign. The primary instruments used to create the current data set were the fine wire thermocouple probe, the Aircraft Integrated Meteorological Measurement System (AIMMS-30), the Pitot-static system (part of UAS flight control), and the infrared gas analyzer sensor for H2O and CO2 (LI-840). All parameters used in temperature calculations (static pressure, True Air Speed, and absolute humidity in form of dew point temperature) were included in the data set. For user convenience, one additional parameter was also included: the type of flight flag (level, up, down, turn, and combination of thereof).

Air temperature, fast response↗

CHELAX-BNF: Fast Response Temperature by airborne measurements

The original data were collected on board the ARM Aerial Facility ArcticShark uncrewed aerial system (UAS; https://www.arm.gov/capabilities/observatories/aaf/uas ) during the “Characterizing HEterogeneous Land-Atmosphere eXchanges at BNF” field campaign (CHEAX-BNF; https://arm.gov/research/campaigns/aaf2025CHELAX-BNF ). The ARM Aerial Facility ArcticShark UAS was based at the public-use airport of Posey Field, AL (FAA LID: 1M4, 34.28027778° N, 87.60055556° W, 283m MSL) from May 28 to June 23, 2025. The ArcticShark UAS performed 5 flights, including 4 research flights over the BNF Main Site (ARM Mobile Facility 3, https://arm.gov/capabilities/observatories/amf ) and Supplemental Facilities to measure atmospheric state, turbulence, surface IR temperature and imagery, aerosol number concentration, and aerosol size distribution. The current data set presents fast response temperature in the atmospheric boundary layer and lower free troposphere measured on the airborne platform throughout the field campaign. The primary instruments used to create the current data set were the fine wire thermocouple probe, the Aircraft Integrated Meteorological Measurement System (AIMMS-30), the Pitot-static system (part of UAS flight control), and the infrared gas analyzer sensor for H2O and CO2 (LI-840). All parameters used in temperature calculations (static pressure, True Air Speed, and absolute humidity in the form of dew point temperature) were included in the data set. For user convenience, one additional parameter was also included: the type of flight flag (level, up, down, turn, and combination of thereof).

Air temperature, fast response↗

Eddy Correlation Flux Measurement System (ECOR) Instrument Handbook

The eddy correlation (ECOR) flux measurement system provides in situ, half-hour measurements of the surface turbulent fluxes of momentum, sensible heat, latent heat, and carbon dioxide (CO 2 ) (and methane at the U.S. Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) user facility’s North Slope of Alaska central facility [NSA Barrow], and at the ARM Mobile Facility (AMF) deployment at Oliktok Point). The fluxes are obtained with the eddy covariance technique, which involves correlation of the vertical wind component with the horizontal wind component, the air temperature, the water vapor density, and the CO 2 concentration. The instruments used are: a fast-response, three-dimensional (3D) wind sensor (sonic anemometer) to obtain the orthogonal wind components and the speed of sound (SOS) (used to derive the air temperature), an open-path infrared gas analyzer (IRGA) to obtain the water vapor density and the CO 2 concentration, and an open-path infrared gas analyzer (IRGA) to obtain methane density and methane flux at NSA Barrow and at the AMF deployment at Oliktok Point. The ECOR systems are deployed at the locations where other methods for surface flux measurements (e.g., energy balance Bowen ratio [EBBR] systems) are difficult to employ, primarily at the north edge of a field of crops. A surface energy balance system (SEBS) has been installed collocated with each deployed ECOR system in SGP, NSA, Tropical Western Pacific (TWP), and each of three ARM Mobile Facilities. The surface energy balance system consists of upwelling and downwelling solar and infrared radiometers within one net radiometer, a wetness sensor, and soil measurements. Finally, the SEBS measurements allow the comparison of ECOR sensible and latent heat fluxes with the energy balance determined from the SEBS and provide information on wetting of the sensors for data quality purposes.

47 OTHER INSTRUMENTATION↗

Impacts of Wildfire Aerosols on Global Energy Budget and Climate: The Role of Climate Feedbacks

Aerosols emitted from wildfires could significantly affect global climate through perturbing global radiation balance. In this study, the Community Earth System Model with prescribed daily fire aerosol emissions is used to investigate fire aerosols’ impacts on global climate with emphasis on the role of climate feedbacks. The total global fire aerosol radiative effect (RE) is estimated to be -0.78 ± 0.29 W m -2 , which is mostly from shortwave RE due to aerosol–cloud interactions (REaci; -0.70 ± 0.20 W m -2 ). The associated global annual-mean surface air temperature (SAT) change ΔT is -0.64 ± 0.16 K with the largest reduction in the Arctic regions where the shortwave REaci is strong. Associated with the cooling, the Arctic sea ice is increased, which acts to reamplify the Arctic cooling through a positive ice-albedo feedback. The fast response (irrelevant to ΔT) tends to decrease surface latent heat flux into atmosphere in the tropics to balance strong atmospheric fire black carbon absorption, which reduces the precipitation in the tropical land regions (southern Africa and South America). The climate feedback processes (associated with ΔT) lead to a significant surface latent heat flux reduction over global ocean areas, which could explain most (~80%) of the global precipitation reduction. The precipitation significantly decreases in deep tropical regions (5°N) but increases in the Southern Hemisphere tropical ocean, which is associated with the southward shift of the intertropical convergence zone and the weakening of Southern Hemisphere Hadley cell. Such changes could partly compensate the interhemispheric temperature asymmetry induced by boreal forest fire aerosol indirect effects, through intensifying the cross-equator atmospheric heat transport.

54 ENVIRONMENTAL SCIENCES↗

Rapid Load Transition for Integrated Solid Oxide Fuel Cell - Gas Turbine (SOFC-GT) Energy Systems: A Demonstration of the Potential for Grid Response

Rapid load transition is an essential requirement for integrated energy systems to maintain grid resilience as more renewable resources are added to the grid. Integrated solid oxide fuel cell - gas turbine (SOFC-GT) systems can provide high efficiency and low carbon emissions over a broad range of turndown. These hybrids also have the potential to enable rapid grid response. The challenge has been to demonstrate effective control strategies to manage load transitions. In the present study, a load transition of ~50% was achieved in 10 s using a novel but simple strategy. Power demand on the SOFC and the GT were ramped down concurrently. During this transition, the SOFC anode fuel was manipulated to maintain SOFC fuel utilization while the cathode inlet air flow and temperature were also manipulated to thermally protect the SOFC. This study was conducted using the Hybrid Performance (Hyper) facility at the National Energy Technology Laboratory (NETL) in a co-simulation environment with the Idaho National Laboratory (INL)'s grid-simulation. The load ramping strategy was tested using a hardware-based cyber-physical simulation methodology. The results demonstrate a high-fidelity representation of SOFC-GT hybrid dynamics and validation of the control strategy. Thermal and electrochemical transients indicated that the SOFC was well protected during rapid load turndown without violating operability constraints. This demonstration revealed the non-linear nature of tightly coupled SOFC-GT system components, especially the non-linear response of SOFC cathode air flow and inlet temperature controls. These results highlight the needs and challenges in developing adaptive automatic controls for autonomous rapid load transitions. This work demonstrates that SOFC-GT hybrids are a viable option to provide the fast-ramping characteristics essential to accommodate high levels of variable renewable power while maintaining grid resilience, reliability, and environmental performance. The results also demonstrate the utility of co-simulation in advancing the tightly-coupled integrated energy systems needed to meet goals for zero-carbon power generation.

DIRECT ENERGY CONVERSION,POWER TRANSMISSION AND DI↗

Climate responses in China to domestic and foreign aerosol changes due to clean air actions during 2013–2019

In recent years, to improve air quality, significant efforts have been made to reduce regional aerosols including China, Europe and North America, which have potential impacts on climate. In this study, fast and slow climate responses in China to changes in domestic and foreign anthropogenic emissions of aerosols and precursors from 2013 to 2019 are investigated using the Community Earth System Model version 1 (CESM1). Aerosol emissions changes, especially reductions in China, North America and Europe, during 2013–2019 resulted in surface air temperature increases across the Northern Hemisphere. Global aerosol changes induce a regional warming of 0.2 °C in China, equally contributed by domestic and foreign emissions changes. China’s domestic emission reductions lead to a regional average temperature rise of 0.1°C, primarily driven by rapid atmospheric adjustments over eastern China. Foreign aerosol changes, particularly reductions in North America and Europe, also contributed to a 0.1°C warming in China through slow oceanic processes. This warming in China induced by foreign aerosol changes is due to a teleconnection between the aerosol-induced anomalous regional warming in Eastern U.S.-North Atlantic Ocean-Europe and the downstream East Asian climate through anomalous wave trains propagation. The comparable influence of domestic and foreign aerosol changes on climate in China underscores the importance of international collaboration in climate mitigation endeavors.

54 ENVIRONMENTAL SCIENCES↗

Effects of Atmosphere and Ocean Horizontal Model Resolution on Tropical Cyclone and Upper-Ocean Response Forecasts in Four Major Hurricanes

A coupled atmosphere–ocean model is necessary for tropical cyclone (TC) prediction to accurately characterize ocean feedback on atmospheric processes within the TC environment. Here, the ECMWF coupled global model is run at horizontal resolutions from 9 to 1.4 km in the atmosphere, as well as 25 and 8 km in the ocean, to identify how resolution impacts forecast accuracy of four observed major TCs in the Atlantic: Irma, Florence, Teddy, and Ida. Most of the resolutions used here are unprecedented for global models. GOES-16 and synthetic aperture radar (SAR) satellite images and best track data are used for atmospheric validation. Salinity and temperature observations from Air-Launched Autonomous Micro-Observer (ALAMO) floats are used to validate modeled upper-ocean response, including mixed layer deepening, sea surface cooling, and near-inertial waves in the wakes of TCs. Increasing atmospheric resolution leads to more realistic TC structure and stronger winds, significantly improving TC intensity forecasts and modestly improving track errors. Ocean resolution impacts the upper-ocean response but does not influence atmospheric forecasts for the fast-moving TCs considered here. Stronger mixing, sea surface cooling, and near-inertial oscillations are found for both higher atmosphere and ocean resolutions, provided the initial upper-ocean state is the same for the two ocean resolutions. Whether this agrees better with the ALAMO observations also depends on the realism of the initial upper-ocean state in the model, emphasizing the importance of ocean initialization for the accurate upper-ocean response. Overall, the model at all resolutions correctly predicts stronger mixing, surface cooling, and near-inertial oscillation amplitudes to the right of a TC center, as observed by ALAMO floats.

Atmosphere-ocean interaction↗

Performance of Scintillation Detectors Based on Quantum Dots in a Semiconductor Matrix (Final Technical Report)

InAs Quantum Dots (QDs) embedded into GaAs semiconductor waveguide have unique scintillation properties, valuable for nuclear security, medical imaging, and high energy physics. In this work, we developed thick (~25um) epitaxial heterostructres with high luminescence efficiency composed of self-assembled nano-engineered InAs QDs grown by molecular beam epitaxy. In this type of detector, the GaAs matrix acts as a stopping material for charged particles or photons generating electrons captured by the QDs acting as luminescence centers. The QD medium is designed to provide fast capture of electrons into QDs (few ps), high QD luminescence efficiency at room temperature (>50%), and strong red-shift of photoluminescence (PL) from the GaAs absorption edge (>250nm). Typical devices consist of a 10-25um thick GaAs layer with embedded sheets of modulation p-type doped InAs QDs and an InGaAs photodetector tuned to the QD emission wavelength. The thick GaAs layer acts also as a waveguide when layer-transferred onto a low-index substrate. Waveguiding and self-absorption (~1cm -1 ) were studied using photoluminescence with scanning laser excitation and modeled with ray optics approximation and geometrical coupling of high-index waveguide to a collection fiber. Scintillating signals from α-particles were analyzed with both an external photodiode (PD) and an integrated PD which provided an improved optical coupling. In the former case, the external InGaAs PD was air-coupled to the scintillator and had the light collection efficiency of about 1% corresponding to limited light extraction through a planar interface with air due to total internal reflection. The mean charge collected by the integrated PD was in the range of (3÷5)×10 4 photoelectrons per 1 MeV of deposited energy, or ~13-20% of the theoretically achievable light yield. Timing of the integrated device was measured by wire-bonding it to the input of an 8 GHz IC. The scintillation response shows an extremely fast 0.3-0.6 ns decay constant and about 40-70 ps time resolution, limited by the system noise. The combined light yield and decay time makes the InAs/GaAs QD heterostructures the fastest high yield scintillation material reported making it valuable for high energy physics and medical imaging applications.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

Enhanced ZIF-8-enabled colorimetric CO 2 sensing through dye-precursor synthesis

The accumulation of carbon dioxide (CO 2 ) within enclosed spaces, along with volatile organic compounds, under certain humidity, temperature, and ventilation conditions is associated with detrimental human health symptoms such as fatigue. Color-based chemical sensing is a promising approach to detect CO 2 levels relevant to indoor air quality through producing fast, quantifiable output visible to the naked eye. In a prior work, a colorimetric gas sensor was fabricated through synthesizing the metal-organic framework, ZIF-8, as the adsorbent, followed by post-synthetic mixing with a dye, phenol red (PSP), and primary amine, ethylenediamine (ED). While this sensor (termed PSP-ED/ZIF-8) maintained its structural integrity in atmospheric conditions and exhibited an increasing fuchsia-to-yellow color change with increasing CO 2 levels in dry environment, the colorimetric response greatly suffered in the presence of humid CO 2 . Here in this work, a significantly improved colorimetric CO 2 sensor (referred to as ED/PSP:ZIF-8) is accomplished through directly incorporating phenol red in the ZIF-8 metal and linker precursor solutions and then blending with ethylenediamine. MATLAB-generated color distributions and in-situ ultraviolet-visible (UV-Vis) spectroscopic studies quantitatively demonstrate an enhanced colorimetric gas response of ED/PSP:ZIF-8 compared to that of PSP-ED/ZIF-8 across an important range of CO 2 for indoor air quality monitoring (500 – 3500 ppm) and across a range of humidity. The new sensor also exhibits high selectivity to CO 2 compared to select volatile organic compounds, such as acetone and ethanol, which contribute to human health symptoms experienced indoors. The enhanced performance is attributed to the proposed incorporation of phenol red within ZIF-8, while maintaining the chemical stability of the MOF.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

NPFTURBULENCE: Fast Response Temperature by Airborne Measurements

The original data were collected during the field campaign of the “Turbulent layers promoting New Particle Formation” experiment (NPFTURBULENCE; https://www.arm.gov/research/campaigns/aaf2024npfturbulence; https://www.arm.gov/publications/programdocs/doe-sc-arm-25-004.pdf ) over the Atmospheric Radiation Measurement (ARM) Southern Great Plains (SGP) Atmospheric Observatory (https://www.arm.gov/capabilities/observatories/sgp ) in north-central Oklahoma. The ARM Aerial Facility ArcticShark uncrewed aerial system (UAS, https://www.arm.gov/capabilities/observatories/aaf/uas) was based at Blackwell–Tonkawa Municipal Airport (IATA: BWL, ICAO: KBKN, FAA LID: BKN, 36.74475° N, 97.34918° W, 313.9 m MSL), for the field campaign from May 5 through May 29, 2024. The ArcticShark UAS performed 11 flights, including 10 research flights over the Central Facility of the ARM SGP to measure atmospheric state, turbulence, surface IR temperature and imagery, aerosol number concentration and size distribution. The current dataset presents fast response temperature in the atmospheric boundary layer and lower free troposphere measured on the airborne platform throughout the field campaign. The primary instruments used to create the current dataset were the fine wire thermocouple probe, Pitot-static system (part of the UAS control), and infrared gas analyzer sensor for H2O and CO2 (LI-840A). All parameters used in the temperature calculations (static and dynamic pressure, absolute humidity in form of dew point temperature) were included in the data set. For user convenience, one additional parameter was also included: the type of flight flag (level, up, down, turn, and combination of thereof).

Air temperature↗

Preliminary Development of Heat Transfer Model-Based Control Algorithms of Liquid Sodium Purification System: Advanced Sensors and Instrumentation Advanced Controls

Monitoring the operation of sodium purification system is essential for efficient operation of sodium fast reactors. In this work, a heat transfer model has been developed for monitoring the plugging meter and cold trap systems at the Mechanisms Engineering Test Loop (METL) liquid sodium facility at Argonne National Laboratory. The model of the purification system was developed by treating the respective aspects of the cold trap purification loop and plugging meter diagnostic loop as two separate control volumes using information from the METL piping and instrumentation diagram (P&ID). A model predictive controller was designed using first order differential equations with the specified boundary conditions. The system behavior was studied with a tuned optimized procedure using the internal cold trap temperature and plugging meter outlet temperature as control variables, and the air blower temperature as an independent variable respectively. Results of computer simulations obtained in this study compared favorably with experimental data showing very good reference tracking response with negligible overshoot as both plugging meter and cold trap physical models approach the setpoint.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

Fast Response of East Asian Precipitation in June 2020 to Local and Remote Aerosol Emission Reductions during COVID-19

Here, in this study, the fast response of East Asian summer precipitation to COVID-19–induced aerosol emission reductions is examined using the Community Earth System Model, version 2.2 (CESM2.2). The emission reductions decreased aerosol optical depth and cloud cover over northern China in June 2020. The troposphere became warmer, strengthening the land–sea thermal contrast and anomalous southerly winds. The subtropical westerly jet accelerated and shifted southward, favoring low-level convergence, upward air motions, and subsequent condensational heating over the Yangtze River basin (YRB). The feedback of condensational heating in return strengthened the convergence and ascent. The western North Pacific subtropical high was intensified, which further enhanced the moisture advection and convergence over the YRB. Both the enhanced moisture convergence and ascent increased precipitation over the YRB during June 2020. Furthermore, local and remote emission reductions show different impacts on convection and moisture transport over the YRB. The emission reductions over China caused stronger convective precipitation (1.15 vs 0.63 mm day −1 ) but weaker larger-scale precipitation (1.17 vs 2.24 mm day −1 ) than the emission reductions outside China. In addition to the emission reductions, the sea surface temperature (SST) anomalies in 2020 also play an important role in increasing precipitation over the YRB, contributing about 42.8%. The relative contribution of SST anomalies also increases under the COVID-19–induced emission scenario.

54 ENVIRONMENTAL SCIENCES↗

Merging flux-variance with surface renewal methods in the roughness sublayer and the atmospheric surface layer

In this article, Two micrometeorological methods utilizing high-frequency sampled air temperature were tested against eddy covariance (EC) sensible heat flux (𝐻) measurements at three sites representing agricultural, agro-forestry, and forestry systems. The two methods cover conventional and newly proposed forms of the flux-variance (FV) and surface renewal (SR) schemes of differing complexities. The sites represent measurements in surface, roughness, and roughness to surface transitional layers. Regression analyzes against EC show that the most reliable FV and SR forms estimate 𝐻 with slopes within ±10% from unity and coefficient of determination 𝑅2 > 0.9 across all the three sites. The best performance of both FV and SR was found at the agricultural site with measurements well within the surface layer, while the worst was found for the tall forest with measurements within the roughness sublayer where its thickness needed to be additionally estimated. The main variable driving 𝐻 in FV is the temperature variance, whereas in SR, it is the geometry of ramp-like structures. Since these structures are also responsible for most of the temperature variance, a novel FV-SR approach emerging from combining the methods is proposed and evaluated against EC measurements and conventional FV and SR schemes. The proposed FV-SR approach requiring only a single fast response thermocouple is potentially independent of calibration and ameliorates some of the theoretical objections that arise when combining ramp statistics with similarity arguments. The combination of methods also provides new insights into the contribution of coherent structures to the temperature variance and its dependence on atmospheric stratification. Other potential utility of the new method is to include it in multi-tool assessments of surface energy fluxes, since a convergence or divergence of the results has a high diagnostic value.

54 ENVIRONMENTAL SCIENCES↗

Detonation Waves in High Explosives

A material at high temperature can react or decompose. For an energetic material, the reaction is exothermic and releases chemical energy that would further increase the temperature. Under some circumstances, when a reaction is triggered, such a reaction can propagate and the material rapidly releases a large amount of energy giving rise to an explosion. Examples of such materials are aerosols, suspensions of solid particles or liquid droplets in a gas; such as coal dust, grain dust and fuel-air explosions. Frequently, explosions are due to accidents. A spectacularly destructive example is the recent explosion of a large quantity of ammonium nitrate (thousands of tons) in Beirut, Lebanon (August 2020); see for example Beirut explosion. Ammonium nitrate is used as a fertilizer. It and the aerosols are not considered to be explosives due to the limited conditions for which an explosion can occur. An aerosol gets the oxidizer from the surrounding air. Burning requires diffusion of the oxidizer to the particle surface where the reaction occurs. A large density of small particles is required for a fast enough reaction to support an explosion. In contrast, an explosive is an energetic material with both fuel and oxidizer mixed on a molecular scale (either premixed gases or within molecules of a solid). This allows fast enough reactions over a wide range of conditions to support a self-propagating reactive wave known as a detonation wave. A detonation wave can be controlled and an explosive used for useful purposes such as in mining, construction, demolition, explosive welding, argon flash lamp, pulsed power using a magnetic flux generator [see also Goforth et al., 2015], jet cutter with shaped charge, explosive art, and generating conditions to study the response of materials at high strain rates and high pressures [see for example, Marsh, 1980]. Explosives are also used in conventional munitions and nuclear weapons. The focus of this book is on the theory and phenomenology of solid high explosives (HEs); in particular, plastic-bonded explosives (PBXs). Some aspects of detonation wave theory are needed to interpret explosive data. Hence, the theory is presented before the detonation wave phenomenology. A familiarity with fluid flow, specifically the notion of shock waves and the shock loci are assumed. In the remainder of this chapter we give a brief overview on the basic properties of detonation waves and PBXs.

36 MATERIALS SCIENCE↗

238 PuO 2 In Vitro Lung Dissolution Rate and Particle Size Determination for Material Involved in the June 8, 2020 Incident at the Los Alamos National Laboratory PF-4 Facility

As part of the LANL response to the June 8, 2020 238 PuO 2 inhalation exposure incident in PF-4, the Nuclear and Radiochemistry Group (C-NR) was asked to assist in determining the lung dissolution rate and particle size distribution of the airborne material. These material characteristics, along with urine and fecal bioassay data, are used by the Radiation Protection Services (RP-SVS) internal dosimetrists to refine dose estimates for exposed workers. Similar to previous studies, an in vitro lung dissolution rate study was performed to assess how fast 238 Pu is cleared from the lungs. Given that PuO 2 is a relatively insoluble material, it dissolves very slowly and requires in vitro studies of 100 or more days to estimate dissolution rates. This report details the results of a 100 day in vitro dissolution rate study and the particle size characteristics of 238 PuO 2 collected on an air filters during the incident. Results show that the 238 PuO 2 involved in this incident has behavior comparable to PuO 2 from previous in vitro studies, with approximately 1% of material dissolving quickly, and 99% of the material dissolving very slowly, with a half-time of approximately 120 years. This is somewhat slower than what was determined in a previous study of LANL 238 PuO 2 , which had an experimental dissolution half-time of 3 years, but significantly faster than 3000 years measured for 239 PuO 2 . Particle size distribution measurements indicate that particle sizes range from 0.10 µm – 6 µm, with most < 2 µm, which is reasonable based on our understanding of the process history of the 238 PuO 2 . Particle size, specific surface area, calcining temperature, specific activity, and age all are known factors that can impact the dissolution rate of refractory materials, however, there are too few studies to quantify the exact influence of these parameters on a measured dissolution rate. The results of this study add to that knowledge base, and provide new insights into the dissolution rates for this LANL process-specific 238 PuO 2 material.

63 RADIATION, THERMAL, AND OTHER ENVIRON. POLLUTAN↗

Extended Modeling of DOE Sealed Canisters with Updated Chemistry Models

Road-ready and final disposition packaging configurations for the advanced test reactor (ATR) fuel currently specifies storage within helium backfilled DOE sealed standard canisters. The aluminum cladding of the ATR fuel contains an oxyhydroxide layer of boehmite/bayerite that generates hydrogen when subjected to irradiation. Understanding the effect of this hydrogen buildup over time to important for long term storage considerations. Previous modeling efforts have built a coupled CFD-chemical model to simulate the temperature gas phase concentrations within the DOE sealed standard canisters. These models have coupled the temperature conditions to both the gas phase radiolysis chemistry and the surface chemistry associated with the oxyhydroxide layer. The previous iteration of the model utilized constant G-values for the hydrogen generation a 50-year period. This new iteration of the model utilizes new experimental data to update the hydrogen generation rate, as well as increase the simulated time to a 200-year period. Given the half-life assumed for the primary Cs-137 isotope responsible for gamma radiation in the ATR spent fuel, the 200-year period decreases the decay heat and dose rate of the spent fuel by a factor of 100, which combined with the updated chemistry substantially decreases new hydrogen generation. Continued experimental work has identified trends for aluminum surrogate samples with oxyhydroxide layers for tests done at higher dose rates. At low initial doses a fast generation rate of hydrogen occurs which starts to roll over to a lower generation as the total dose applied increase. A small-scale chemical model was built to replicate as mini-canister surrogate system at SRNL as well as for the smaller capsule tests performed at INL. A variety of chemical models to capture this effect were tested, and a back reaction of H radical absorbing onto the surface, or inhibition of the reaction by significant H 2 cover gas were both able to fit both the mini-canister and the small capsule test data. Both kinetic fits were used to generate data from the new 200-year simulation. As additional experiments continue, the kinetic fits may be adjusted to adapt to new data. However, updated data shows that hydrogen atmosphere has little effect on actual generation data, so the model was reverted to use a star-stepped G-value for low-dose and high-dose regions. For the undried fuel case, the three models differ significantly with an end concentration of 1% for back reaction, 4.2% for inhibition, and 13.1% for constant G-value for the nominal scenario. For the dried fuel case, the nominal cases showed end concentrations of 0.23% for back reaction, 1.9% for inhibition, and 4.2% for const G-value for the nominal scenario. For the constant G-value case that is less conservative than the other two, the pressure for undried fuel increases to 1.94 atm over 200 years for the nominal case and 2.11 atm for the high decay heat case. The total hydrogen concentration after 200 years is 4.92% for the low decay heat case and 27.4% for the high decay heat case for undried fuel and is 1.4% and 9.6% for low and high decay heat fuel for the dried fuel case. If small amount of residual air is present, the potential for nitric acid formation of 595, 1568, and 2816 ppm for the lower, nominal, and upper fuel decay heat can occur. At long-term timeframes no significant shift in major species present occurs, so no appreciable amount of oxygen is present in the system. The continued rate of hydrogen generation in the canister occurs at an increase of 0.04% by mole over the final 10 years. Increasing the model range out to 1000 years continues to drop the hydrogen generation rate through decreasing dose rate.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗