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At least 19 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2019

The dependence of radius on relative humidity and solute mass at high relative humidities up to and including 100%

This manuscript presents a rigorous examination of the equilibrium radius ratio of hygroscopic aerosol particles that are solution drops of ideal and actual inorganic solutes for a range of solute masses in the relative humidity range 99-100%. Analysis is presented first for ideal solutes over a range of solute masses for different hygroscopicities, providing a theoretical framework for the subsequent analysis of actual solutes. Dimensionless quantities are used to reduce the Kohler equation to one with no free parameters and an approximate solution is presented. Next analysis is presented for three common inorganic solutes of atmospheric importance: sodium chloride, ammonium sulfate, and sulfuric acid, with a range of solute masses considered for each substance. The extent to which non-ideality is important for these solutes over the ranges of relative humidities and solute masses considered is examined. A simple but accurate single-parameter expression is presented for the equilibrium radius ratio as a function of relative humidity that contains the dependenceso on solute mass and composition for these solutes. The accuracy of this expression is quantified and factors that limit this accuracy are discussed. The expression is accurate to within 5% over most of the range of mass-equivalent dry radii from 10 to 250 nm and relative humidities from below 99 up to 100%, over which the equilibrium radius ratio varies by more than a factor of five, and it remains finite at 100% relative humidity. Lastly, measurements of hygroscopic growth of aerosol particles in this relative humidity range are discussed.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2019

Effects of Porous Carbon Morphology, Agglomerate Structure and Relative Humidity on Local O 2 Transport Resistance

The morphology and ionomer distribution in a polymer electrolyte membrane fuel cell (PEMFC) cathode electrode are quantified with nano-scale resolution X-ray computed tomography (nano-CT). Using the nano-CT data, different shapes, sizes and compositions of agglomerates are extracted. Statistical information from multiple techniques, including transmission electron microscopy (TEM), ultra-small angle X-ray scattering (USAXS), and Brunauer-Emmett-Teller (BET) gas adsorption porosimetry are combined to reconstruct the high surface-area porous carbon (HSC) support, exterior (on the surface of carbon) and interior (inside carbon pores) catalysts, ionomer, and primary pores in the extracted agglomerates. Application of capillary condensation theory to the reconstructed agglomerate structure is shown to accurately represent the experimentally-observed relative humidity (RH) dependence of the electrochemically-active surface area (ECA). Direct numerical simulations show that the high local O 2 transport resistance ( R O 2 ) under dry conditions is mainly associated with the reduced ECA. We demonstrate that the agglomerate shape and size affect R O 2 only if the primary pores are poorly accessible (i.e., capillary-condensed water filled primary pores). We also evaluate the effect of transport to the interior catalyst particles on R O 2 .

agglomerate↗
DOE OSTI2018

Assessment of the combination of temperature and relative humidity on kidney stone presentations

Highlights: • Temperature and relative humidity have opposing effects on evaporative water loss. • Wet-bulb temperatures best predicted kidney stone presentations. • Differences in predictive capacity of temperature metrics were greatest in summer. Temperature and relative humidity have opposing effects on evaporative water loss, the likely mediator of the temperature-dependence of nephrolithiasis. However, prior studies considered only dry-bulb temperatures when estimating the temperature-dependence of nephrolithiasis. We used distributed lag non-linear models and repeated 10-fold cross-validation to determine the daily temperature metric and corresponding adjustment for relative humidity that most accurately predicted kidney stone presentations during hot and cold periods in South Carolina from 1997 to 2015. We examined three metrics for wet-bulb temperatures and heat index, both of which measure the combination of temperature and humidity, and for dry-bulb temperatures: (1) daytime mean temperature; (2) 24-h mean temperature; and (3) most extreme 24-h temperature. For models using dry-bulb temperatures, we considered four treatments of relative humidity. Among 188,531 patients who presented with kidney stones, 24-h wet bulb temperature best predicted kidney stone presentation during summer. Mean cross-validated residuals were generally lower in summer for wet-bulb temperatures and heat index than the corresponding dry-bulb temperature metric, regardless of type of adjustment for relative humidity. Those dry-bulb models that additionally adjusted for relative humidity had higher mean residuals than other temperature metrics. The relative risk of kidney stone presentations at the 99th percentile of each temperature metric compared to the respective median temperature in summer months differed by temperature metric and relative humidity adjustment, and ranged from an excess risk of 8–14%. All metrics performed similarly in winter. The combination of temperature and relative humidity determine the risk of kidney stone presentations, particularly during periods of high heat and humidity. These results suggest that metrics that measure moist heat stress should be used to estimate the temperature-dependence of kidney stone presentations, but that the particular metric is relatively unimportant.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2021

Printed hygroscopic electrodes for low-cost capacitive relative humidity sensors

A capacitive relative humidity sensor includes a first electrode and a second electrode, where at least the one of the electrodes is a water-permeable electrode. The electrodes act in conjunction with a water-sensitive hygroscopic dielectric material. The design enables low-cost and simple fabrication of fast-responding and stable relative humidity sensors using digital fabrication techniques.

Pierre, Adrien↗
DOE OSTI2018

Lung function association with outdoor temperature and relative humidity and its interaction with air pollution in the elderly

Highlights: • We studied pulmonary effects of temperature and relative humidity in elderly. • Temperature and relative humidity were associated with decreased FEV1 and FVC. • The lag structure suggested that acute effects may last several days. • Effects of temperature and relative humidity were stronger on FVC than on FEV1. • Effects of temperature and relative humidity were amplified by black carbon exposure. While the effects of weather variability on cardio-respiratory mortality are well described, research examining the effects on morbidity, especially for vulnerable populations, is warranted. We investigated the associations between lung function and outdoor temperature (T in Celsius degrees (°C)) and relative humidity (RH), in a cohort of elderly men, the Normative Aging Study. Our study included 1103 participants whose forced vital capacity (FVC), forced expiratory volume in one second (FEV{sub 1}), and weather exposures were assessed one to five times during the period 1995–2011 (i.e. 3162 observations). Temperature and relative humidity were measured at one location 4 h to 7 days before lung function tests. We used linear mixed-effects models to examine the associations with outdoor T and RH. A 5-degree increase in the 3-day moving average T was associated with a significant 0.7% decrease (95%CI: −1.24, −0.20) in FVC and a 5% increase in the 7-day moving average RH was associated with a significant 0.2% decrease (95%CI: −0.40, −0.02) in FVC and FEV{sub 1}. The associations with T were greater when combined with higher exposures of black carbon with a 1.6% decrease (95%CI −2.2; −0.9) in FVC and a 1% decrease (95%CI −1.7; −0.4) in FEV{sub 1}. The relationships between T and RH and lung function were linear. No synergistic effect of T and RH was found. Heat and lung function are two predictors of mortality. Our findings suggest that increases in temperature and relative humidity are related to decreases in lung function, and such observations might be amplified by high black carbon levels.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2020

Hydration of α-UO 3 following storage under controlled conditions of temperature and relative humidity

Changes in chemical speciation of uranium oxides following storage under varied conditions of temperature and relative humidity are valuable for characterizing material provenance. In this study, subsamples of high purity α-UO 3 were stored under four sets of controlled conditions of temperature and relative humidity over several years, and then measured periodically for chemical speciation. Powder X-ray diffraction (XRD) analysis and extended X-ray absorption fine structure spectroscopy confirm hydration of α-UO 3 to a schoepite-like end product following storage under each of the varied storage conditions, but the species formed during exposure to the lower relative humidity and lower temperature condition follows different trends from those formed under the other three storage conditions (high relative humidity with high or low temperatures, and low relative humidity with a high temperature). Thermogravimetry coupled with XRD analysis was carried out to distinguish desorption pathways of water from the hydrated end products. Density functional theory calculations discern changes in the structure of α-UO 3 following incorporation of 1, 2 or 3 H 2 O molecules or 1, 2 or 3 OH groups into the orthorhombic lattice, revealing differences in lattice constants, U–O bond lengths, and U–U distances. The collective results from this analysis are in contrast to analogous studies that report that U 3 O 8 is oxidized and hydrated in air during storage under high relative humidity conditions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2017

Impact of Relative Humidity during Spin-Deposition of Metal Oxide Thin Films from Aqueous Solution Precursors

Relative humidity during the spin-processing of thin film solution precursors is often not controlled or measured, and its effect on film thickness is generally unappreciated. Herein, we report that the relative humidity during spin-processing has a marked impact on the film thickness of amorphous metal oxide (aluminum oxide and lanthanum zirconium oxide) and hafnium oxide-sulfate (HafSOx) thin films deposited from aqueous precursors. In the humidity range studied [20–95% relative humidity (RH)], film thicknesses varied by a factor of nearly 3, and this effect is independent of the metal precursor identity. Our data suggest that film thickness depends linearly on evaporation rate (100 – RH) for all systems studied, suggesting this effect is predominantly due to the unique characteristics of water as a solvent. In situ X-ray reflectivity studies of HafSOx films deposited under different humidities reveal that, while the thickness varies significantly with humidity, the density of the as-deposited films is similar, suggesting that humidity primarily affects the relative amount of material deposited. Because reproducible film thickness is critical for many applications, our data highlight the importance of controlling humidity during spin-processing.

36 MATERIALS SCIENCE↗
DOE OSTI2018

Observational Relationship between Entrainment Rate and Environmental Relative Humidity and Implications for Convection Parameterization

Entrainment rate is a critical but highly uncertain quantity in convective parameterizations; especially, the effects of environmental relative humidity on entrainment rate are controversial, or even opposite, in different studies. Analysis of aircraft observations of cumuli from the RACORO and RICO field campaigns shows that entrainment rate is positively correlated with relative humidity. Physical analysis shows that higher relative humidity promotes entrainment by reducing buoyancy in the cloud cores and by weakening downdrafts near the cloud cores. The reduced buoyancy in the cloud cores and weakened downdrafts surrounding the cores further reduce updrafts in the cloud cores; the cloud cores with smaller updrafts are more significantly affected by their environment, resulting in larger entrainment rate. The relationship between entrainment rate and relative humidity is consistent with the buoyancy sorting concept widely used in convection parameterizations. The results provide reliable in situ observations to improve parameterizations of entrainment rate.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2020

Water adsorption on vanadium oxide thin films in ambient relative humidity

Here in this work, ambient pressure x-ray photoelectron spectroscopy (APXPS) is used to study the initial stages of water adsorption on vanadium oxide surfaces. V 2p, O 1s, C 1s, and valence band XPS spectra were collected as a function of relative humidity in a series of isotherm and isobar experiments. Experiments were carried out on two VO 2 thin films on TiO 2 (100) substrates, prepared with different surface cleaning procedures. Hydroxyl and molecular water surface species were identified, with up to 0.5 ML hydroxide present at the minimum relative humidity, and a consistent molecular water adsorption onset occurring around 0.01% relative humidity. The work function was found to increase with increasing relative humidity, suggesting that surface water and hydroxyl species are oriented with the hydrogen atoms directed away from the surface. Changes in the valence band were also observed as a function of relative humidity. The results were similar to those observed in APXPS experiments on other transition metal oxide surfaces, suggesting that H 2 O-OH and H 2 O-H 2 O surface complex formation plays an important role in the oxide wetting process and water dissociation. Compared to polycrystalline vanadium metal, these vanadium oxide films generate less hydroxide and appear to be more favorable for molecular water adsorption.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2018

The Effect of Environmental Relative Humidity on Carbonation and Oxidation in a Cementitious Waste Form - 18448

Cementitious material has been developed and used for the nuclear waste disposal. Cast Stone, a type of cementitious waste form, is considered for solidification and immobilization of part of low activity radioactive waste (LAW) at DOE Hanford Site in Richland, WA. During its life cycle, the waste form, which is produced from Portland cement, fly ash, blast furnace slag and liquid waste, is subject to reaction with carbon dioxide and oxygen, both in gaseous and dissolved form. The reactions may alter the physical and chemical properties of the waste form and thus change its retention ability for the radionuclides. Therefore, understanding the rate and the impact of oxidation and carbonation in the material is important for projecting the long-term performance of Cast Stone. However, the rate of carbonation and oxidation in Cast Stone closely depends on the moisture content in the material, which varies largely with the environmental relative humidity (RH). In this study, experiments are carried out to study the effect of environmental relative humidity on the carbonation and oxidation rate as well as the leaching of the constituents from Cast Stone. Cast Stone samples doped with Cr as a reaction indicator are aged for 16 to 32 weeks under N{sub 2}, air, and 2% CO{sub 2} (in nitrogen) environments with various relative humidities (15%, 40%, 68%, 100%). After aging, samples were tested for the pH-dependent leaching (EPA Method 1313) and mass transfer rate under diffusion-controlled leaching (EPA Method 1315) of constituents. The progress of the carbonation was measured for each condition to determine the rate of carbonation front ingress. The results show that environmental relative humidity strongly influences carbonation and oxidation in Cast Stone; however, the impact is different for the rate of reaction and for the extent of reactions. The former refers to the rate at which the reaction front ingresses, while the latter refers to the fraction of the material reacted. For both carbonation and oxidation, the largest impact of the reactions at the exposure surface is observed at intermediate relative humidity (68%). However, for carbonation, the reaction front evolves more rapidly under drier conditions, with the highest rate observed at 15% RH. As a result, carbonation and oxidation have different degree of impact on the leaching behavior of Cast Stone samples aged under various relative humidities. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2017

An XPS study on the impact of relative humidity on the aging of UO 2 powders

High resolution x-ray photoemission spectroscopy (XPS) was used to characterize the chemical speciation of high purity uranium dioxide (UO 2 ) powder samples following aging for periods of up to one year under controlled conditions with relative humidity ranging from 34% to 98%. A systematic shift to higher uranium oxidation states, and thus an increase in the mean uranium valence, was found to directly correlate with the dose of water received (i.e. the product of exposure time and relative humidity). Exposure duration was found to have a greater impact on sample aging than relative humidity. Lastly, the sample aged at 98% relative humidity was found to have unique structural differences for exposure time beyond 180 days when observed by scanning electron microscopy (SEM).

36 MATERIALS SCIENCE↗
DOE OSTI2012

Lead Research and Development Activity for DOE's High Temperature, Low Relative Humidity Membrane Program (Topic 2)

The Department of Energy’s High Temperature, Low Relative Humidity Membrane Program was begun in 2006 with the Florida Solar Energy Center (FSEC) as the lead organization. During the first three years of the program, FSEC was tasked with developing non-Nafion® proton exchange membranes with improved conductivity for fuel cells. Additionally, FSEC was responsible for developing protocols for the measurement of in-plane conductivity, providing conductivity measurements for the other funded teams, developing a method for through-plane conductivity and organizing and holding semiannual meetings of the High Temperature Membrane Working Group (HTMWG). The FSEC membrane research focused on the development of supported poly[perfluorosulfonic acid] (PFSA) – Teflon membranes and a hydrocarbon membrane, sulfonated poly(ether ether ketone). The fourth generation of the PFSA membrane (designated FSEC-4) came close to, but did not meet, the Go/No-Go milestone of 0.1 S/cm at 50% relative humidity at 120 °C. In-plane conductivity of membranes provided by the funded teams was measured and reported to the teams and DOE. Late in the third year of the program, DOE used this data and other factors to decide upon the teams to continue in the program. The teams that continued provided promising membranes to FSEC for development of membrane electrode assemblies (MEAs) that could be tested in an operating fuel cell. FSEC worked closely with each team to provide customized support. A logic flow chart was developed and discussed before MEA fabrication or any testing began. Of the five teams supported, by the end of the project, membranes from two of the teams were easily manufactured into MEAs and successfully characterized for performance. One of these teams exceeded performance targets, while the other requires further optimization. An additional team developed a membrane that shows great promise for significantly reducing membrane costs and increasing membrane lifetime.

08 HYDROGEN↗
DOE OSTI2012

Water radiolysis on plutonium dioxide: Initial results identifying a threshold relative humidity for oxygen gas generation

The radiolysis of water adsorbed onto the surface of high-purity plutonium dioxide powder is important for the safe storage and transportation of plutonium. Plutonium dioxide is the stable form of plutonium in air and plutonium dioxide readily adsorbs water from the atmosphere. The number of monolayers of water adsorbed is relative humidity dependent. Radiolysis of the adsorbed water can result in flammable conditions in sealed containers even if the atmosphere within the container has been flushed with an inert gas. The initial net rates of oxygen and hydrogen gas formation due to radiolysis of water associated with high-purity plutonium dioxide material are reported as a function of exposure relative humidity. A threshold relative humidity is observed for oxygen gas generation and a lower threshold appears to exist for hydrogen gas generation. Above their respective thresholds the net rates of oxygen and hydrogen gas generation increase rapidly. The net rates of formation are nearly linear with the number of monolayers above the threshold coverage. The net rates are also dependent upon specific surface area, but not linearly.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2023

Relative humidity threshold for oxygen generation by high-purity plutonium dioxides in 3013 containers

High-purity plutonium dioxide with adsorbed water in a sealed container can generate oxygen, but oxygen will not be generated in low water loading conditions. A threshold for oxygen generation has been observed in the hydrogen generation rate normalized by the specific power for high-purity plutonium dioxide. Normalized hydrogen generation rates above this threshold generate oxygen and below the threshold consume oxygen. The threshold rate is determined by the amount of water adsorbed onto the surface of the oxide. The relative humidity of the atmosphere that the oxide is in equilibrium with determines the amount of physisorbed water adsorbed on the surface. We calculate the relative humidity corresponding to the threshold rate as a function of mass and specific surface area of material stored in 3013 containers. Exceeding the calculated relative humidity may result in flammable gas mixtures of hydrogen and oxygen at some time during storage.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗