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DOE OSTI2020

Monitoring Potential Transport of Radioactive Contaminants in Shallow Ephemeral Channels: FY2019

Desert Research Institute (DRI) conducted a field assessment of the potential for contaminated soil to be transported from the Smoky Site Contamination Area (CA) because of storm runoff. This activity supported U.S. Department of Energy (DOE) Environmental Management Nevada Program (EM NV) efforts to establish post-closure monitoring plans for the Smoky Site Soils Corrective Action Unit (CAU) 550. The work was intended to confirm the likely mechanism of transport and determine the meteorological conditions that might cause the movement of contaminated soils, as well as determine the particle size fraction most closely associated with transported radionuclide-contaminated soils. These data will facilitate the design of the appropriate post-closure monitoring program. In 2011, DRI installed a meteorological monitoring station on the west side of the Smoky Site CA and a hydrologic (runoff) monitoring station within the CA, near the east side. The meteorological station collected air temperature, wind speed, wind direction, relative humidity, precipitation, solar radiation, barometric pressure, soil temperature, and soil water content data. The maximum, minimum, and average or total values (as appropriate) for each of these parameters were recorded for each 10-minute interval. The maximum, minimum, and average water depth in the flume installed at the hydrologic station were also recorded for each 10-minute interval. This report presents the data collected from these stations during fiscal year (FY) 2019. During the FY2019 reporting period, the warmest months were June, July, and August and the coldest were December and February. The highest monthly solar radiation (i.e., sunshine) values were recorded in June, July, and August, whereas December through February had the lowest solar radiation values. Monthly mean wind speeds were highest in the spring (April) and early summer (June). Winds were predominantly from the north, except in February, July, August, and September when winds were mostly from the west. The monthly average relative humidity ranged from 17 percent to approximately 60 percent. Humidity was lowest in the summer and highest in the winter. Monthly total precipitation ranged from 0.0 during August and September to 2.22 inches (in) (56.39 millimeters [mm]) in February. Total precipitation for FY2019 was 7.83 in (198.88 mm). During the reporting period, a single, nonzero, flow event was recorded at the flume. This occurred over two days between March 6 and 7, 2019, in response to 1.16 in (29.46 mm) of precipitation falling within 9.3 hours on March 6, 2019. This event produced a peak water depth of 0.39 in (0.99 centimeters [cm]) in the flume, and runoff was measured for approximately 23.5 hours. However, the maximum recorded flow depth was less than the limit for flow discharge and velocity that can be calculated for the six-inch (15 cm) throat of a Parshall flume. The runoff event produced insufficient flow velocities through the natural channel to cause local erosion and transport of bedload materials. No bedload samples were collected for radiological analysis. Observing meteorological and environmental conditions that lead to storm runoff will help identify the parameters and threshold conditions that should be incorporated into post-closure monitoring plans for this and similar Soils CAU sites. Routine monitoring of meteorological and hydrologic parameters at the Smoky Site CA has been discontinued at the request of EM NV, effective at the conclusion of FY2019. Environmental data acquisition was completed and the meteorological and runoff monitoring stations were removed from the Smoky Site on October 15, 2019.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2023

Vertical distribution of boundary layer new particle formation and implications for nanoparticle growth mechanisms (Final Report)

New particles can form high above ground in the atmosphere before such formation events are observed by ground-based instruments. Once formed, these particles can take up significant amounts of water vapor, which has implications on the mechanisms by which nanoparticles grow and, ultimately, impact cloud formation processes. These observations motivated the research performed in this project using a combination of modeling, laboratory experiments, and the analysis of field observations. We hypothesized is that ground-based measurements do not always accurately represent the location and timing of new particle formation events, nor do they adequately characterize the dominant physical and chemical processes that are responsible for the subsequent growth of newly formed particles. Essentially, we wanted to study the new particle formation process under conditions that we expect may be more relevant to the actual location in the atmosphere where such events take place, which are often characterized by higher relative humidities, lower temperatures, and a broader range of precursors and oxidants compared to those observed at ground level. This project had two main objectives, each of which directly addressed our hypothesis. Our first is to investigate the timing, distribution, meteorological conditions, and nanoparticle properties associated with boundary layer new particle formation through the analysis of ARM field campaigns such as HI-SCALE and long-term observations and observations performed in other locales such as in China and India where atmospheric conditions could play a crucial role in determining the mechanisms of new particle formation. This activity provided a comprehensive description, both in time and in space, of the gases and nanoparticle properties that are responsible for these events. We also performed modeling studies to explore the vertical profile and timing of new particle formation events from these campaigns. Our second objective was to perform laboratory and process-level modeling studies to investigate the role that conditions such as low ambient temperature, high relative humidity, and different oxidants such as nitrate radical play in determining unique chemical pathways for nanoparticle growth. In doing so, we revisited the representation of nanoparticle growth in global models and updated assumptions of formation and growth based on the findings of the field, laboratory, and process-level-model work. Our research provides crucial insights into the most important regions of the atmospheric boundary layer for future observational and modeling studies. It also identifies the most relevant environmental conditions, precursors, and oxidants that are responsible for nanoparticle growth, which will aid in the design of laboratory studies and process-level model experiments. The unique pathways that we discovered can be incorporated into regional and global models, thereby improving predictions and attribution of the role of new particle formation in, e.g., air pollution formation and cloud properties.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2022

Climate Impact on CO2 Capture Efficiency and Levelized Cost of Liquid solvent-based DAC (Direct Air Capture) System

The transition towards net-zero emission poses economic, technical, and political challenges for the commercial-scale deployment of CO2 removal technologies by 2050. The opportunities for large-scale deployment will largely depend on the distinctive conditions found in the different locations of the world such as energy cost, carbon intensity of energy source, construction, transportation, and weather conditions. In this work, we focus on one of the promising negative emission technology, DAC (Direct Air Capture), and its response to different weather conditions. This work presents two potential operation scenarios: (i) natural gas standalone, (ii) grid electricity connected DAC plant. For the first time, we investigated the influence of temperature and RH (relative humidity) of the air on liquid-based DAC system and its response to carbon capture efficiency and levelized cost of carbon capture with operational sensitivity analysis. It is observed that the overall energy demand decreases from 11.1 to 8.3 GJ/ton-CO2 as the CO2 capture rate increases from 40 to 85%. We observed that a CO2 capture rate of 75% is only possible above 17°C even at 90% RH and this drops tremendously at lower temperatures. It is also observed that water evaporation in the air contactor is highest at dry and low RH as expected. The sensitivity analysis showed that weather conditions are insensitive to CO2 capture efficiency for the liquid-solvent based DAC plant for both scenarios. In addition, higher CO2 capture efficiency is achievable from lower upstream methane emissions and carbon intensity of grid electricity (for grid-connected scenario). Lastly, the levelized cost of natural gas standalone scenario varies from 239.7 to 408.8 $/t-CO2 is sensitive to temperature conditions more than relative humidity and compared to electricity grid-connected scenario, from 265.3 to 440.1 $/t-CO2.

An, Keju↗
DOE OSTI2020

Contrasting Scale Dependence of Entrainment-Mixing Mechanisms in Stratocumulus Clouds

The apparent turbulent entrainment-mixing mechanism between clouds and surrounding air is scale-dependent; however, such scale dependence has been rarely studied, hindering development of scale-aware entrainment-mixing parameterizations. Here we extend our previous study on cumulus clouds to investigate scale dependence of entrainment-mixing processes in stratocumulus clouds during ACE-ENA and RACORO. In contrast to previous studies, two opposite scale dependencies are found: entrainment-mixing can become more homogeneous or more inhomogeneous with increasing averaging scales, which is quantified by the difference between homogeneous mixing degree at the 100 m and 10 m resolutions. A new heuristic model and two new quantities are introduced. The observations and model show that microphysical properties near and far away from droplet-free air and relative humidity of entrained air determine both the sign and strength of scale dependence, while droplet-free air fraction only affects the strength. The results shed new light on developing scale-aware parameterizations of entrainment-mixing mechanisms.

Gao, Sinan↗
DOE OSTI2026

Meteorological Conditions in Urban Sites in Knoxville, USA. 2025

This 2025 dataset, which contains five csv files, reports hourly air temperature, wind speed, solar radiation, incident short wave, reflected short wave, incident long wave, emitted long wave, net radiation, and photosynthetically active radiation (PAR) data measured in urban parks in Knoxville, Tennessee, USA. The sites include Cumberland Estates Park (CEP), Socially Equal Energy Efficient Development (SEEED), West Hills Park (WHP), West View Park (WVP), and Victor Ashe Park (VAP). Air temperature, wind speed, and solar radiation data were obtained from a METER ATMOS 41 All-in-One Weather Station (Pullman, Washington, USA). Incident and emitted radiation (shortwave and longwave) measurements were made using an Apogee (Logan, Utah, USA) net radiometer (Model SN-500-SS). The SQ-521 Full-Spectrum Quantum sensor (Apogee Instruments, Inc) recorded the PAR. The measurement data for all the sites started on January 1, 2025. and all measurement ended on December 31, 2025. This work is a part of a larger study which investigates the impact of soil moisture and plant evapotranspiration on ambient temperature and relative humidity in several city parks in Knoxville, Tennessee.

Salvador, Christian [ORNL] (ORCID:0000000283287777↗
DOE OSTI2025

Meteorological Conditions in Urban Sites in Knoxville, USA. 2023

This 2023 dataset, which contains four csv files, reports hourly air temperature, wind speed, solar radiation, incident short wave, reflected short wave, incident long wave, emitted long wave, net radiation, and photosynthetically active radiation (PAR) data measured in urban parks in Knoxville, Tennessee, USA. The sites include Cumberland Estates Park (CEP), Socially Equal Energy Efficient Development (SEEED), West Hills (WHP), and Victor Ashe Park (VAP). Air temperature, wind speed and direction, and solar radiation data were obtained from a METER ATMOS 41 All-in-One Weather Station (Pullman, Washington, USA). Incident and emitted radiation (shortwave and longwave) measurements were made using an Apogee (Logan, Utah, USA) net radiometer (Model SN-500-SS). The SQ-521 Full-Spectrum Quantum sensor (Apogee Instruments, Inc) recorded the PAR. The measurement data for CEP, SEEED, and VAP started on July 1, 2023, while WHP started on August 26, 2023. All measurement ended on December 31, 2023. This work is a part of a larger study which investigates the impact of soil moisture and plant evapotranspiration on ambient temperature and relative humidity in several city parks in Knoxville, Tennessee.

Salvador, Christian [ORNL] (ORCID:0000000283287777↗
DOE OSTI2022

Product distribution, kinetics, and aerosol formation from the OH oxidation of dimethyl sulfide under different RO 2 regimes

Abstract. The atmospheric oxidation of dimethyl sulfide (DMS) represents a major natural source of atmospheric sulfate aerosols. However, there remain large uncertainties in our understanding of the underlying chemistry that governs the product distribution and sulfate yield from DMS oxidation. Here, chamber experiments were conducted to simulate gas-phase OH-initiated oxidation of DMS under a range of reaction conditions. Most importantly, the bimolecular lifetime (τbi) of the peroxy radical CH3SCH2OO was varied over several orders of magnitude, enabling the examination of the role of peroxy radical isomerization reactions on product formation. An array of analytical instruments was used to measure nearly all sulfur-containing species in the reaction mixture, and results were compared with a near-explicit chemical mechanism. When relative humidity was low, “sulfur closure” was achieved under both high-NO (τbi<0.1 s) and low-NO (τbi>10 s) conditions, though product distributions were substantially different in the two cases. Under high-NO conditions, approximately half the product sulfur was in the particle phase, as methane sulfonic acid (MSA) and sulfate, with most of the remainder as SO2 (which in the atmosphere would eventually oxidize to sulfate or be lost to deposition). Under low-NO conditions, hydroperoxymethyl thioformate (HPMTF, HOOCH2SCHO), formed from CH3SCH2OO isomerization, dominates the sulfur budget over the course of the experiment, suppressing or delaying the formation of SO2 and particulate matter. The isomerization rate constant of CH3SCH2OO at 295 K is found to be 0.13±0.03 s−1, in broad agreement with other recent laboratory measurements. The rate constants for the OH oxidation of key first-generation oxidation products (HPMTF and methyl thioformate, MTF) were also determined (kOH+HPMTF=2.1×10-11 cm3 molec.−1 s−1, kOH+MTF=1.35×10-11 cm3 molec.−1 s−1). Product measurements agree reasonably well with mechanistic predictions in terms of total sulfur distribution and concentrations of most individual species, though the mechanism overpredicts sulfate and underpredicts MSA under high-NO conditions. Lastly, results from high-relative-humidity conditions suggest efficient heterogenous loss of at least some gas-phase products.

Ye, Qing (ORCID:0000000337978988)↗
DOE OSTI2026

Characterizing the impact of water uptake on light absorption by aerosol particles

Absorbing aerosols (AA) have an important impact on the global radiation budget. The composition and properties of AA can vary substantially throughout the atmosphere, depending on the particle source and the influence of chemical aging. Uncertainties associated with the radiative effects of AA remain substantial. A key contributor to this uncertainty is understanding the extent to which water uptake alters absorption by AA particles and how this depends on particle composition. We have used new and existing experimental tools to systematically characterize the relationship(s) between AA chemical and physical characteristics, relative humidity, and mixing of AA with other aerosol components through a combination of laboratory and field measurements. We have developed fundamental understanding through laboratory experiments that will enable interpretation of field observations at DOE ARM sites and facilitate process-based improvements in the simulation of absorption by carbonaceous aerosols in climate models. In the laboratory experiments we have considered a variety of different AA types, including fullerene soot (a surrogate for refractory black carbon, or BC) and nigrosine (a surrogate for partially soluble brown carbon, or BrC). By examining a range of AA types we will develop insight into how the chemical and physical properties of AA particles (e.g. whether they are refractory or soluble) impact the influence of water uptake on absorption. These AA particles will also be mixed—both internally and externally—with compounds having a wide range of hygroscopic properties to establish how the impact of water uptake on absorption will vary with photochemical processing. These laboratory observations have been compared with commonly used theoretical models, enabling development of empirical models that will facilitate improved representation of absorption by AA particles in regional and global climate models. Overall, our study has contributed to the mission of the Atmospheric System Research program by quantifying how interactions between aerosols and radiation depend on relative humidity. Through this, our work will improve understanding and model representation of aerosol processes as they affect the Earth’s radiation budget.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2020

Utilizing ink composition to tune bulk-electrode gas transport, performance, and operational robustness for a Fe-N-C catalyst in polymer electrolyte fuel cell

With lower site density and turnover frequency, platinum group metal (PGM)-free catalysts based electrodes are often greater than 50 mu m thick in order to increase performance across the fuel cell operating range. Consequently, PGM-free electrodes have an additional bulk electrode transport resistance beyond the local or aggregate level transport in thin platinum-based electrodes. In parallel to the development of more active and durable PGM-free catalysts, advancements in understanding the interplay between PGM-free electrode fabrication, bulk-electrode transport, proton conductivity and performance are needed. Here, the relationship between ionic and gas phase transport through the electrode thickness is modified by adjusting electrocatalyst and ionomer flocculation/interaction at the ink level. The influence of the ink composition (water/n-propanol content) is examined via various in-situ electrochemical and ex-situ characterization techniques and the resulting electrode structure/performance relationship contrasted with electrode performance robustness across a range of relative humidity (RH). For the electrocatalyst examined here, a water-rich (82 wt% H2O) ink formulation was favorable for operation at high RH due to improved molecular diffusion through larger electrode pores. In contrast, the improved interactions between ionomer and electrocatalyst enabled a more robust electrode and higher performance during low RH operation for the 50 wt% H2O content ink.

08 HYDROGEN↗
DOE OSTI2022

Proton Conducting Sulfonated Poly(Ionic Liquid) Block Copolymers

Herein, we report the synthesis of proton-conducting sulfonated poly(ionic liquid) block copolymers (S-PILBCPs) containing one block with sulfonic acid (sulfonated styrene, SS) and the other with an IL moiety (vinylbenzylmethylimidazolium bis(trifluoromethylsulfonyl)imide, VBMIm-TFSI) using reversible addition–fragmentation chain-transfer (RAFT) polymerization and post-polymerization modifications (i.e., functionalization, anion exchange reactions, and sulfonation). The S-PILBCPs uniquely conjoin the SS block with mobile protons (H + ) and the PIL block with mobile anions (TFSI – ), where multiple highly desired properties, including high proton conductivity (from the SS block), and high IL-philicity and oxygen solubility (from the PIL block) can exist compartmentally within a microphase separated morphology (evidenced by differential scanning calorimetry (DSC) and small-angle X-ray scattering (SAXS)). High ion conductivity of 79.7 mS/cm at a PIL block composition of 21.6 mol % was observed at 80 °C and 90% relative humidity (RH) (comparable to the benchmark Nafion ionomer). This work successfully demonstrates the design of S-PILBCPs as a new material platform and showcases its promise as an ionomer for proton exchange membrane fuel cells (PEMFCs) as they simultaneously and compartmentally combine proton conductivity and oxygen solubility. Furthermore, these benefits have recently been leveraged to achieve substantial improvement in oxygen reduction reaction (ORR) activity and subsequently fuel cell performance.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

NNSS Soils Monitoring: Plutonium Valley (CAU 366) FY2019

Desert Research Institute (DRI) conducted a field assessment of the potential for radionuclide-contaminated soil to be transported from the Plutonium Valley Dispersion Sites Contamination Area (CA) because of both wind and storm water runoff. This activity supported U.S. Department of Energy (DOE) Environmental Management Nevada Program (EM NV) efforts to establish post-closure monitoring plans for the Plutonium Valley Dispersion Sites Corrective Action Unit (CAU) 366. The DRI task was intended to identify the likely mechanism(s) of transport and determine the meteorological conditions that might cause the movement of radionuclide-contaminated soils. The emphasis of the work was on collecting sediment transported by channelized storm runoff and measuring airborne dust concentrations and associated wind conditions. These data will facilitate an appropriate post-closure monitoring program. In 2011, DRI installed meteorological monitoring stations north and south of the Plutonium Valley CA—known as Pu Valley North and Pu Valley South, respectively—as well as a fluvial sediment sampling station within the CA. Since installation, temperature, wind speed, wind direction, relative humidity, precipitation, solar radiation, barometric pressure, soil temperature, volumetric soil moisture content, and airborne particulate concentrations have been collected at both meteorological stations. The maximum, minimum, and average or total (as appropriate) for each of these parameters were recorded for each 10-minute interval. The sediment sampling station included an automatically activated sampling pump with collection bottles for suspended sediment, which was activated when sufficient flow was present in the channel, and passive traps for bedload material that was transported down the channel during runoff events. This report presents data collected from these stations during fiscal year (FY) 2019. During the FY2019 (October 1, 2018, through September 30, 2019) reporting period, the warmest month was July and the coldest month was February. Monthly total solar radiation was highest in June or July (depending on the station) and lowest in December. Monthly mean wind speeds were highest during February. At the Pu Valley North station, winds were commonly northerly, northwesterly, and southerly. At the Pu Valley South station, the wind direction was more variable and winds frequently came from most directions, excluding westerly and northwesterly winds. Winds above 15.0 miles per hour (mph) (24.1 kilometers per hour [km/hr]) were frequently southerly at both stations, and less-frequent strong winds were northerly (at the Pu Valley South station) or northwesterly (at the Pu Valley North station). Monthly average relative humidity ranged from 18 percent in August to 62 percent in January and February. Monthly total precipitation ranged from zero at both stations in September to 2.23 inches (in) (56.6 millimeters [mm]) during February at the Pu Valley South station and 2.09 in (53.1 mm) during March at the Pu Valley North station. From October 1, 2018, through September 30, 2019, the total precipitation was 8.23 in (209 mm) and 8.15 in (207 mm) at the Pu Valley South and Pu Valley North stations, respectively. The largest daily precipitation totals of 1.46 in (37.1 mm) and 1.14 in (29.0 mm) occurred at the Pu Valley South and Pu Valley North stations, respectively, on March 6, 2019. However, the ISCO autosampler was not activated during any storm event in FY2019 because the channel water depth measurements were insufficient for suspended sediment sample collection. Additionally, because no significant flow through the channel was indicated, no bedload samples were collected. Light breezes of 0.0 mph to 5.0 mph (0.0 km/hr to 8.0 km/hr) occurred most frequently (approximately 55 percent to 57 percent of the time). The frequency of occurrence diminished exponentially as the wind speed increased such that winds in excess of 25.0 mph (40.2 km/hr) occurred less than 0.01 percent of the time. Winds in excess of 15.0 mph (24.1 km/hr) were most commonly southerly, which is likely controlled by the topography of the valley because topographic highs define the east and west sides of the valley and converge toward the north.The concentrations of PM2.5 (particulate matter with an aerodynamic diameter ≤2.5 micrometers [μm]) and PM10 (particulate matter with an aerodynamic diameter ≤10 μm) in the air generally increase as wind speed increases. However, the particle profiler at the Pu Valley South station regularly malfunctioned, which resulted in poor data quality and a limited period of record within FY2019. Therefore, discussion of the annual dust observations is mostly limited to the Pu Valley North station. At the Pu Valley North station, significant increases in windblown dust concentrations were observed when wind speeds exceeded 15.0 mph (24.1 km/hr), especially during southerly winds. When all wind speeds were considered, high dust concentrations at the Pu Valley North station were frequently associated with northerly, northwesterly, or southerly winds. The majority of PM10 transport at the Pu Valley North station occurred when winds were blowing northerly and northwesterly because of the high frequency of winds up to 15.0 mph (24.1 km/hr). The ratio of PM10 to PM2.5 is a qualitative indicator of the proximity of dust sources to the observation point and the values of the PM10 to PM2.5 ratio tend to be higher nearer to the source. The PM10 to PM2.5 ratio increased from 1.2 to 2.8 with higher wind speeds at the Pu Valley North station. This increase suggests that some locally sourced PM10 was present in the air when local winds exceeded 15.0 mph (24.1 km/hr). Local dust suspension is interpreted during major dust events when peaks in the PM10 to PM2.5 ratio occur simultaneously with the maximum wind speed and the peak PM10 concentration. Analysis of the five major dust events in FY2019 revealed that northerly winds were dominant in three events and southerly winds were dominant in two events. Local suspension of dust within Plutonium Valley is suspected to have occurred during two of the five major events (April 9, 2019, and September 28 to 29, 2019), and a nonlocal source of dust is presumed for the three other major dust events (October 14, 2018; May 16, 2019; and September 2, 2019). The three suspected regional dust transport events exhibited winds that typically did not exceed the 15.0 mph (24.1 km/hr) wind speed threshold for local dust transport and featured PM10 to PM2.5 ratios that indicate large-scale regional dust transport. Similar event characteristics (e.g., wind speed and PM10 concentration) were observed at air monitoring stations approximately 70 mi (113 km) to the northwest within the Tonopah Test Range (TTR). Therefore, these three regional events may not reflect transport from the Plutonium Valley CA. Routine monitoring of meteorological and hydrologic parameters at Plutonium Valley has been discontinued at the request of EM NV, effective at the conclusion of FY2019. Environmental data acquisition has been completed, and both Pu Valley North and Pu Valley South meteorological stations within Plutonium Valley as well as the ISCO autosampler station within the CA were removed on October 14, 2019.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2023

Modeling the Impact of the Organic Aerosol Phase State on Multiphase OH Reactive Uptake Kinetics and the Resultant Heterogeneous Oxidation Timescale of Organic Aerosol in the Amazon Rainforest

Accurate predictions of chemical lifetime, i.e., oxidation timescale and change in the mass of organic aerosols (OAs) in atmospheric models, are critical to quantify the impacts of OA on aerosol–cloud interactions, radiative forcing, and air quality. The heterogeneous oxidation of OA by hydroxyl (OH) radicals is a key process governing OA mass changes during their oxidation. Recently, laboratory observations of the OH uptake coefficient (γ OH ) and heterogeneous reaction rate (k het,OH ) for different OA systems with varying phase states have been combined to develop a new parameterization of γ OH and k het,OH as a function of the OA phase state, i.e., viscosity (η OA ). Here, in this work, we use a recently published viscosity prediction framework to analyze the new γ OH and k het,OH parameterization with a box model. Subsequently, we implement this box model to predict γ OH and k het,OH over the Amazon rainforest in the dry-to-wet transition season with both significant biomass burning and biogenic influences. Relevant parameters within our box model are specified based on detailed regional model simulations over the Amazon using the Weather Research and Forecasting model coupled with Chemistry (WRF-Chem). η OA is predicted as a function of species volatility, OA composition (including water uptake) along with ambient relative humidity (RH), and temperature. Based on ambient conditions simulated by WRF-Chem over the entire atmospheric column, we use the box model to predict the upper bounds of the heterogeneous oxidation timescale of OA. Based on previous laboratory measurements, we assume that this heterogeneous OH oxidation causes fragmentation (carbon loss) of OA, followed by the evaporation of the fragmented molecules that results in the exponential decay of OA. We predict that the oxidation timescale of OA is ~1 month near the Earth’s surface in the pristine Amazonian background because of low OH concentrations. But OA is oxidized more rapidly within urban and wildfire plumes near the Earth’s surface with an order of magnitude higher OH concentrations compared to the pristine background, causing the simulated oxidation timescale of OA to be much shorter, ~3–4 days. At 3–5 km altitudes where biomass burning OA is predicted to be semisolid, the heterogeneous oxidation timescale is estimated as ~6 days to 3 weeks and decreases with increasing OH concentrations within plumes. We show that the simulated mass loss of OA is strongly size-dependent, where smaller particles oxidize more rapidly compared to larger particles due to their greater per-particle surface area-to-volume ratio. Increasing urbanization and deforestation in the Amazon in the future might increase OH concentrations in the background Amazon, causing faster oxidation of OA. At higher altitudes above liquid clouds, especially in the upper troposphere where temperatures approach ~250 K, future measurements are needed to reduce the uncertainties related to the mass loss of OA at colder temperatures and low relative humidity conditions due to its heterogeneous OH oxidation.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Fluidization of Group A Glass Particles: Experiments and Preliminary Validation

This work is aimed at providing reliable high-quality data from fluidization experiments. Geldart Group A glass beads are used as bed material. The fluidizing medium is air at atmospheric pressure which enters the system at 40% relative humidity. The air inlet velocity is varied over a broad range from 2 U mf to 26 U mf , where the minimum fluidization velocity, U mf , is 0.608 cm/s. There is not a significant change in the mean values of differential pressure; however, there are noticeable trends in their standard deviation values. Preliminary validation studies are performed using the open-source software Multiphase Flow with Interphase eXchanges (MFiX) developed by the National Energy Technology Laboratory (NETL). The results from Eulerian-Eulerian (MFiX-TFM, two-fluid model) and Eulerian-Lagrangian (MFiX-PIC, particle-in-cell) formulations are compared. The work presented in this report highlights the applicability of MFiX-PIC for large-scale applications, and reveals that PIC simulation offers a suitable alternative to TFM simulation when effects due to multiple components or polydispersity are significant. PIC modeling provides a readily extendible framework for such systems. However, PIC models do rely on an empirical closure for inter-particle stress. Some solution discrepancies were evident in MFiX-PIC predictions which require further analysis. As such, the study underlines the need for a systematic approach to quantify the sources of numerical uncertainty within the PIC model. However, even with known empiricism, MFiX-PIC has demonstrated considerable potential in analyzing gas-solid systems. The results obtained are encouraging and warrant further investigation to improve the predictive capability of MFiX-PIC.

36 MATERIALS SCIENCE↗
DOE OSTI2020

AATTENUATION—The Atmospheric Attenuation Model for CSP Tower Plants: A Look-Up Table for Operational Implementation

Attenuation of solar radiation between the receiver and the heliostat field in concentrated solar power (CSP) tower plants can reduce the overall system performance significantly. The attenuation varies strongly with time and the average attenuation at different sites might also vary strongly from each other. If no site specific attenuation data is available, the optimal plant design cannot be determined and rough estimations of the attenuation effect are required leading to high uncertainties of yield analysis calculations. The attenuation is caused mainly by water vapor content and aerosol particles in the lower atmospheric layer above ground. Although several on-site measurement systems have been developed during recent years, attenuation data sets are usually not available to be included during the plant project development. An Atmospheric Attenuation (AATTENUATION) model to derive the atmospheric transmittance between a heliostat and receiver on the basis of common direct normal irradiance (DNI), temperature, relative humidity, and barometric pressure measurements was developed and validated by the authors earlier. The model allows the accurate estimation of attenuation for sites with low attenuation and gives an estimation of the attenuation for less clear sites. However, the site-dependent coefficients of the AATTENUATION model had to be developed individually for each site of interest, which required time-consuming radiative transfer simulations, considering the exact location and altitude, as well as the pre-dominant aerosol type at the location. This strongly limited the application of the model despite its typically available input data. In this manuscript, a look-up table (LUT) is presented which enables the application of the AATTENUATION model at the site of interest without the necessity to perform the according complex radiative transfer calculations for each site individually. This enables the application of the AATTENUATION model for virtually all resource assessments for tower plants and in an operational mode in real time within plant monitoring systems around the world. The LUT also facilitates the generation of solar attenuation maps on the basis of long-term meteorological data sets which can be considered during resource assessment for CSP tower plant projects. The LUTs are provided together with this manuscript as supplementary files. The LUT for the AATTENUATION model was developed for a solar zenith angle (SZA) grid of 1°, an altitude grid of 100 m, 7 different standard aerosol types and the standard AFGL atmospheres for mid-latitudes and the tropics. The LUT was tested against the original version of the AATTENUATION model at 4 sites in Morocco and Spain, and it was found that the additional uncertainty introduced by the application of the LUT is negligible. With the information of latitude, longitude, altitude above mean sea level, DNI, relative humidity (RH), ambient temperature (Tair), and barometric pressure (bp), the attenuation can be now derived easily for each site of interest.

14 SOLAR ENERGY↗
DOE OSTI2024

Uncertainty-informed selection of CMIP6 Earth System Model subsets for use in multisectoral and impact models

Earth system models (ESMs) and general circulation models (GCMs) are heavily used to provide inputs to sectoral impact and multisector dynamic models, which include representations of energy, water, land, economics, and their interactions. Therefore, representing the full range of model uncertainty, scenario uncertainty, and interannual variability that ensembles of these models capture is critical to the exploration of the future co-evolution of the integrated human–Earth system. The pre-eminent source of these ensembles has been the Coupled Model Intercomparison Project (CMIP). With more modeling centers participating in each new CMIP phase, the size of the model archive is rapidly increasing, which can be intractable for impact modelers to effectively utilize due to computational constraints and the challenges of analyzing large datasets. In this work, we present a method to select a subset of the latest phase, CMIP6, featuring models for use as inputs to a sectoral impact or multisector dynamics models, while prioritizing preservation of the range of model uncertainty, scenario uncertainty, and interannual variability in the full CMIP6 ensemble results. This method is intended to help impact modelers select climate information from the CMIP archive efficiently for use in downstream models that require global coverage of climate information. This is particularly critical for large-ensemble experiments of multisector dynamic models that may be varying additional features beyond climate inputs in a factorial design, thus putting constraints on the number of climate simulations that can be used. We focus on temperature and precipitation outputs of CMIP6 models, as these are two of the most used variables among impact models, and many other key input variables for impacts are at least correlated with one or both of temperature and precipitation (e.g., relative humidity). Besides preserving the multi-model ensemble variance characteristics, we prioritize selecting CMIP6 models in the subset that preserve the very likely distribution of equilibrium climate sensitivity values as assessed by the latest Intergovernmental Panel on Climate Change (IPCC) report. This approach could be applied to other output variables of climate models and, possibly when combined with emulators, offers a flexible framework for designing more efficient experiments on human-relevant climate impacts. It can also provide greater insight into the properties of existing CMIP6 models.

Snyder, Abigail C.↗
DOE OSTI2020

Accelerated Aging Humidity Chamber for Nuclear Grade HEPA Filter Media

A unique accelerated aging humidity chamber for simulating the natural aging process of nuclear grade high efficiency particulate air (HEPA) filter media is being designed, implemented, and tested. The nuclear industry currently lacks information regarding the shelf life and service life of HEPA filter media. The Department of Energy recommends disposing of HEPA filters 10 years after the manufacture date for filters operated under dry conditions. Studies have shown the tensile strength and water repellency of HEPA filter media diminish with age. The chamber's principal function is to sustain an elevated relative humidity condition for an extended duration specified by the Arrhenius aging model. To accomplish this, various design parameters were established: (1) consistently achieve uniform humidity conditions within the chamber to equally expose media sheets, (2) ensure the chamber is sufficiently sealed to mitigate the uncontrolled infiltration of air, (3) confidently secure the media sheets to avert the introduction of unnecessary stressing/creasing, (4) fabricate the chamber from clear polycarbonate material to allow inspection of the media sheets, (5) provide a safe and ergonomic design for personnel, (6) ensure the chamber design is replicable and relatively easy to fabricate/assemble. A humidity source, fan, PID controller, humidity and temperature transmitters, and data loggers are required for proper operation and control of the chamber. The humidity source must accommodate target values up to 95% relative humidity throughout the chamber. The three humidity and temperature transmitters are strategically spaced throughout the chamber to ensure uniform conditions. The 10 cubic feet per minute (CFM) fan selected intends to accomplish the desired air change rate inside the chamber of approximately 20 air changes per hour (ACH). The 2 plenums on the upper and lower portions of the chamber utilize a perforated design to uniformly distribute air, promote air mixing, and control the air velocity entering the chamber. Industrial blueprint hanging clamps are being retrofitted to be seated within the chamber drawers and firmly secure the nuclear grade filter media. The aged media will be evaluated using autopsy methodology, and the results obtained intend to help clarify the useful life of nuclear grade HEPA filters. Nuclear grade high efficiency particulate air (HEPA) filters are defined as disposable, extended-media, dry-type filters with a rigid casing enclosing the full depth of the pleats and have a minimum particle removal efficiency of 99.97%. [1] - HEPA filters are constantly exposed to stressors and subsequently have been shown to degrade as the filter ages. Properties such as tensile strength and water repellency, along with others, are negatively impacted. [2] - Due to the scarcity of naturally aged HEPA filters available, it is crucial to develop accelerated aging methods which effectively mimic the natural degradation effects. - After accelerated aging, the filters are subject to testing in the Axial Flow Large Scale Test Stand (ALSTS) and other analysis techniques such as the same qualification tests performed directly after being manufactured. - Quality data is necessary for future decisions regarding the lifetime of nuclear grade HEPA filters. - The objective is to develop a prototype accelerated aging humidity chamber for nuclear grade HEPA filter media. The chamber should expose the media to commonly occurring stressors to expedite the degradation process caused by aging. PID yields reliable and reproducible results: - CFD model correlates well with actual performance; - Further analysis is needed to complete characterization; - Future work for the chamber is still to be completed. The data shown in Figure 5 and Table 1 indicate the system is functioning as designed. As can be determined from the system response evaluation in Table 1, the PID controller is yielding reliable and reproducible results at each set point. As the set point increases, the time constant and 20% settling time increase accordingly. From the results in Table 1, it stands to reason that the CFD model correlates well with the actual performance of the system. Each system response parameter for the 90%RH* CFD model is slightly lower than the parameters collected from the physical model tested at an equivalent set point. This is to be expected considering the inlet in the CFD model is a constant supply of water vapor, whereas the physical model uses a PID controller to monitor the amount of water vapor needed and reacts accordingly. More analysis is still to be done on the prototype chamber. A pressure test will be conducted in order to determine the hourly leak rate of the chamber. This test will involve constant air flow into the chamber until the desired pressure is reached. A uniformity test will also be conducted in order to ensure each filter medium is being exposed to equivalent relative humidity levels. This test will involve an array of humidity meters strategically oriented inside the chamber to record any possible gradients. Future work for the chamber includes dehumidification abilities, tests while fully loaded with filters, and temperature control. Once completed, the autopsy team at Institute of Clean Energy Technology will conduct necessary accelerated aging studies as needed.

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

Variability in observed stable water isotopes in snowpack across a mountainous watershed in Colorado

In this study, isotopic information from 81 snowpits was collected over a 5-year period in a large, Colorado watershed. Data spans gradients in elevation, aspect, vegetation, and seasonal climate. They are combined with overlapping campaigns for water isotopes in precipitation and snowmelt, and a land-surface model for detailed estimates of snowfall and climate at sample locations. Snowfall isotopic inputs, describe the majority of δ18O snowpack variability. Aspect is a secondary control, with slightly more enriched conditions on east and north facing slopes. This is attributed to preservation of seasonally enriched snowfall and vapour loss in the early winter. Sublimation, expressed by decreases in snowpack d-excess in comparison to snowfall contributions, increases at low elevation and when seasonal temperature and solar radiation are high. At peak snow accumulation, post-depositional fractionation appears to occur in the top 25 ± 14% of the snowpack due to melt-freeze redistribution of lighter isotopes deeper into the snowpack and vapour loss to the atmosphere during intermittent periods of low relative humidity and high windspeed. Relative depth of fractionation increases when winter daytime temperatures are high and winter precipitation is low. Once isothermal, snowpack isotopic homogenization and enrichment was observed with initial snowmelt isotopically depleted in comparison to snowpack and enriching over time. The rate of δ18O increase (d-excess decrease) in snowmelt was 0.02‰ per day per 100-m elevation loss. Isotopic data suggests elevation dictates snowpack and snowmelt evolution by controlling early snow persistence (or absence), isotopic lapse rates in precipitation and the ratio of energy to snow availability. Hydrologic tracer studies using stable water isotopes in basins of large topographic relief will require adjustment for these elevational controls to properly constrain stream water sourcing from snowmelt.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2021

Long-term thermal aging of parylene conformal coating under high humidity and its effects on tin whisker mitigation

Usage of pure tin (Sn) or Sn-rich alloy in electronics industry is growing, which makes them more susceptible to the spontaneous growth of tin whiskers. The risk of having these whiskers can be dramatically mitigated by applying a conformal coating provided that it not only possesses excellent mechanical and adhesion properties but also maintains these properties throughout their service. Parylene C is commonly used as a conformal coating because of its favorable mechanical and physical properties, as well as superior conformal coverage. The purpose of this paper is to investigate the degradation of parylene C coating during the thermal aging in high humidity environment (85°C/85% relative humidity for up to 5000hrs) and its effect on the tin whisker mitigation capacity. It was observed that during aging at high temperature and high humidity (HTHH) environment, the oxidation occurs at early times, followed by bond scission, resulting in the loss of strength of the coating. Thinner parylene coating (12.5-μm-thick) had better coating adhesion on the silane-treated tin surface, so provided the better protection for tin whisker penetration than the thicker counterpart (25-μm-thick). After 2500hrs of aging, due to the degradation of the silane agent at the tin/parylene interface, the adhesion of the parylene coating was significantly weakened on the tin surface, which resulted in extensive corrosion of the tin solderpads. The loss of adhesion of the coating, along with the corrosion of the tin surface facilitated the tin whisker nucleation at the interface while the loss of mechanical strength and the brittleness made the coating easily penetrated by the growing whiskers. Tin whiskers with a smaller diameter were buckled and grew along the delaminated region while those with a larger diameter penetrated and continued to grow through the coating. Hence, the effectiveness of the parylene coatings on tin whisker mitigation is significantly reduced under long exposure to such high temperature and high humidity.

36 MATERIALS SCIENCE↗