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At least 469 records · Page 26
All sourcesNASA NTRSDOE OSTI
DOE OSTI2013

Light absorption by secondary organic aerosol from α-pinene: Effects of oxidants, seed aerosol acidity, and relative humidity

It is well known that light absorption from dust and black carbon aerosols has a warming effect on climate while light scattering from sulfate, nitrate, and sea salt aerosols has a cooling effect. However, there are large uncertainties associated with light absorption and scattering by different types of organic aerosols, especially in the near-UV and UV spectral regions. In this paper, we present the results from a systematic laboratory study focused on measuring light absorption by secondary organic aerosols (SOAs) generated from dark α-pinene + O 3 and α-pinene + NO x + O 3 systems in the presence of neutral and acidic sulfate seed aerosols. Light absorption was monitored using photoacoustic spectrometers at four different wavelengths: 355, 405, 532, and 870 nm. Significant light absorption at 355 and 405 nm was observed for the SOA formed from α-pinene + O 3 + NO 3 system only in the presence of highly acidic sulfate seed aerosols under dry conditions. In contrast, no absorption was observed when the relative humidity was elevated to greater than 27% or in the presence of neutral sulfate seed aerosols. Organic nitrates in the SOA formed in the presence of neutral sulfate seed aerosols were found to be nonabsorbing, while the light-absorbing compounds are speculated to be aldol condensation oligomers with nitroxy organosulfate groups that are formed in highly acidic sulfate aerosols. Finally and overall, these results suggest that dark α-pinene + O 3 and α-pinene + NO x + O 3 systems do not form light-absorbing SOA under typical atmospheric conditions.

Song, Chen↗
DOE OSTI2017

Influence of humidity, temperature, and annealing on microstructure and tensile properties of electrospun polyacrylonitrile nanofibers

This study investigates the microstructure and mechanical properties of electrospun nanofibers from polyacrylonitrile (PAN)-dimethylformamide (DMF) solution at different relative humidity (RH) in the range from 14% to 60% and two different temperatures (20 °C and 40 °C). Nanofibers produced at low RH (22% or less at 20 °C) exhibit relatively smooth surface and solid core, whereas at higher RH (30% or higher at 20 °C) rough surface and porous core are observed. The resulting morphology is explained by means of H 2 O/DMF/PAN ternary phase diagram. At higher RH, the water diffusion into polymer-solution jet brings thermodynamic instability into the system leading to separation of polymer-rich phase and polymer-lean phase, where the later contributes to porosity. Higher process temperature (40 °C) yields larger miscibility area in the ternary phase diagram leading to formation of porous structure at relatively higher RH (40%). Tensile strength of nanofibrous yarns is found to vary from 80 MPa to 130 MPa depending on the processing temperature and RH. The amount of porosity is found to affect the tensile properties of nanofibers most significantly, although diameter and crystallinity play important role. Annealing is found to alleviate surface roughness and porosity and increase crystallinity. Furthermore, tensile strength of nanofibrous yarns is found to improve by up to 25% after annealing.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Changes in water vapor adsorption and water film thickness in clayey materials as a function of relative humidity

Abstract Soil water, with adsorbed water being an important component, plays an important role in fluid flow and chemical movement in the unsaturated zone. The adsorbed water consists of water film and interlayer water, and its content is related to the relative humidity (RH). This study theoretically and experimentally focuses on the variation in adsorbed water content in clayey materials as the RH changes. Based on a slit‐pore model, three types of water (water film, interlayer water, and capillary water) could be present in the water vapor adsorption process. The variation of water film is obtained from the analysis of interfacial forces, and then the total water content can be quantitatively subdivided into these three types of water for different RH values. The slit‐pore adsorption model was used with experimental measurements (water vapor adsorption and N 2 physisorption) to quantify the amounts and interrelationships of these three different types of water to six clayey materials, namely three clay minerals (kaolinite, montmorillonite, and illite–smectite mixed layer) and three clay‐rich sediments from the Jianghan Plain in China. The main results are that (a) the volumes of water vapor adsorption are much greater than those of N 2 adsorption except for kaolinite; (b) interlayer water largely dominates the growth of total water content in montmorillonite and results in a concentration of 0.090 ml g −1 at 95% RH; and (c) the minimum thickness of water film is calculated to be 0.23 nm, and the maximum value is one‐third of the pore width by considering the interfacial forces.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2022

Aqueous spray-drying synthesis of alluaudite Na 2+2x Fe 2–x (SO 4 ) 3 sodium insertion material: studies of electrochemical activity, thermodynamic stability, and humidity-induced phase transition

In pursuit of high-energy density sodium insertion materials, polyanionic frameworks can be designed with tuneable high-voltage operation stemming from inductive effect. Alluaudite Na 2 Fe 2 (SO 4 ) 3 polysulfate forms one such earth-abundant compound registering the highest Fe 3+ /Fe 2+ redox potential (ca. 3.8 V vs. Na/Na + ). While this SO 4 -based system exhibits high voltage operation, it is prone to thermal decomposition and moisture attack leading to hydrated derivatives, making its synthesis cumbersome. Also, the Na–Fe–S–O quaternary system is rich with (anhydrous to hydrated) phase transitions. Herein, we demonstrate scalable aqueous-based spray drying synthesis of alluaudite Na 2+2x Fe 2–x (SO 4 ) 3 sodium insertion material involving the formation of bloedite Na 2 Fe(SO 4 ) 2 ·4H 2 O as an intermediate phase. Moreover, a reversible phase transition from alluaudite to bloedite under controlled conditions of temperature and relative humidity is reported for the first time. Thermochemistry measurements revealed the enthalpies of formation (ΔH° f ) of alluaudite and bloedite are exothermic. Hydrated bloedite (ΔH° f = –117.16 ± 1.10 kJ/mol) was found to be significantly more energetically stable than anhydrous alluaudite (ΔH° f = –11.76 ± 1.25 kJ/mol). The calorimetric data support the observed synthesis and transformation (hydration-dehydration) pathways. Spray drying route led to spherical morphology delivering capacity ~80 mAh/g. Spray drying can be extended for rapid economic synthesis of sulfate class of battery materials.

25 ENERGY STORAGE↗
DOE OSTI2018

Recharge estimation from discrete water-table datasets in a coastal shallow aquifer in a humid subtropical climate

A time-series approach to the estimation of recharge rate in unconfined aquifers of highly variable water level is proposed. The approach, which is based on the water-table fluctuation method (WTF), utilizes discrete water-level measurements. Other similar techniques require continuous measurements, which makes them impossible to apply in cases where no data from automatic loggers are available. The procedure is deployed at the Ressacada Farm site, southern Brazil, on a coastal shallow aquifer located in a humid subtropical climate where diurnal water-level variations of up to 1 m can follow a precipitation event. The effect of tidal fluctuations on the groundwater levels is analyzed using a harmonic component builder, while a time-variable drainage term is evaluated through an independent analysis and included in the assessment. The estimated recharge values are compared with those obtained from the continuous measurements showing a good agreement with the approaches for discrete dataset intervals of up to 15 days. Subsequently, the estimated recharge rates are incorporated into a transient groundwater-flow model and the water levels are compared showing a good match. Henceforth, the approach extends the applicability of WTF to noncontinuous water-level datasets in groundwater recharge studies.

58 GEOSCIENCES↗
DOE OSTI2015

Reducing conditions, reactive metals, and their interactions can explain spatial patterns of surface soil carbon in a humid tropical forest

Humid tropical forests support large stocks of surface soil carbon (C) that exhibit high spatial variability over scales of meters to landscapes (km). Reactive minerals and organo-metal complexes are known to contribute to C accumulation in these ecosystems, although potential interactions with environmental factors such as oxygen (O 2 ) availability have received much less attention. Reducing conditions can potentially contribute to C accumulation, yet anaerobic metabolic processes such as iron (Fe) reduction can also drive substantial C losses. We tested whether these factors could explain variation in soil C (0–10 and 10–20 cm depths) over multiple spatial scales in the Luquillo Experimental Forest, Puerto Rico, using reduced iron (Fe(II)) concentrations as an index of reducing conditions across sites differing in vegetation, topographic position, and/or climate. Fine root biomass and Fe(II) were the best overall correlates of site (n = 6) mean C concentrations and stocks from 0 to 20 cm depth (r = 0.99 and 0.98, respectively). Litterfall decreased as reducing conditions, total and dead fine root biomass, and soil C increased among sites, suggesting that decomposition rates rather than C inputs regulated soil C content at the landscape scale. Strong relationships between Fe(II) and dead fine root biomass suggest that reducing conditions suppressed particulate organic matter decomposition. The optimal mixed-effects regression model for individual soil samples (n = 149) showed that aluminum (Al) and Fe in citrate/ascorbate and oxalate extractions, Fe(II), fine root biomass, and interactions between Fe(II) and Al explained most of the variation in C concentrations (pseudo R 2 = 0.82). The optimal model of C stocks was similar but did not include fine root biomass (pseudo R 2 = 0.62). In these models, soil C concentrations and stocks increased with citrate/ascorbate-extractable Al and oxalate-extractable Fe. However, soil C decreased with citrate/ascorbate-extractable Fe, an index of Fe susceptible to anaerobic microbial reduction. At the site scale (n = 6), ratios of citrate/ascorbate to oxalate-extractable Fe consistently decreased across a landscape O 2 gradient as C increased. Finally, we suggest that the impact of reducing conditions on organic matter decomposition and the presence of organo-metal complexes and C sorption by short-range order Fe and Al contribute to C accumulation, whereas the availability of an Fe pool to sustain anaerobic respiration in soil microsites partially attenuates soil C accumulation in these ecosystems.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2018

Corrosion Behavior of Weathering Steel Under Thin Electrolyte Layer at Different Relative Humidity

The corrosion behavior of weathering steel under thin electrolyte layer (TEL) at different relative humidity (RH) was investigated by cathodic polarization, electrochemical impedance spectroscopy, electrochemical noise, SEM/EDS, XRD and Raman spectroscopy. The results indicate that during the initial stage, the corrosion rate increases as the RH decreases when the initial thickness of TEL is above 100 μm. During the middle and final corrosion stages, the corrosion behavior of weathering steel is influenced by RH, the initial thickness of TEL and corrosion product. The TEL corrosion is divided into three types, and a weathering steel corrosion model under TEL and bulk solution is also proposed.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Exploring the Role of Humidity, Temperature, and Mixed Ionic and Electronic Conductivity on SOFC Anode Electrocatalysis

Infiltration of nanoscale electrocatalysts into Ni/yttria-stabilized zirconia (Ni-YSZ) cermets has been shown to improve the electrochemical performance of solid oxide fuel cell (SOFC) anodes. While infiltrated electrodes in SOFCs result in improved cell performance, long-term operation leads to coarsening of the infiltrated nanoparticles and negates the short-term performance improvements. This study explores the roles of humidity, temperature, and number of cycles of nanocatalyst infiltration in improving mixed conduction within the Ni-YSZ electrode. Two mixed conduction phases were studied: Gd 0.1 Ce 0.9 O 2-δ (GDC) as an infiltrant into Ni-YSZ electrodes, and Ni/transition metal doped-YSZ electrodes infiltrated with Ni. Analysis of impedance data from these cells shows improved electrochemical performance in infiltrated cells with mixed conduction compared with infiltrated cells containing purely ionic and electronic conducting phases. Improved anode performance is attributed to the availability of electronic pathways through predominantly ionic-conducting phases to connect distant Ni nanoparticles and/or Ni grains.

25 ENERGY STORAGE↗
DOE OSTI2023

The effect of relative humidity on eddy covariance latent heat flux measurements and its implication for partitioning into transpiration and evaporation

While the eddy covariance (EC) technique is a well-established method for measuring water fluxes (i.e., evaporation or 'evapotranspiration’, ET), the measurement is susceptible to many uncertainties. One such issue is the potential underestimation of ET when relative humidity (RH) is high (> 70%), due to low-pass filtering with some EC systems. Yet, this underestimation for different types of EC systems (e.g. open-path or closed-path sensors) has not been characterized for synthesis datasets such as the widely used FLUXNET2015 dataset. Here, we assess the RH-associated underestimation of latent heat fluxes (LE, or ET) from different EC systems for 163 sites in the FLUXNET2015 dataset. We found that the LE underestimation is most apparent during hours when RH is higher than 70%, predominantly observed at sites using closed-path EC systems, but the extent of the LE underestimation is highly site-specific. We then propose a machine learning based method to correct for this underestimation, and compare it to two energy balance closure based LE correction approaches (Bowen ratio correction, BRC, and attributing all errors to LE). Our correction increases LE by 189% for closed-path sites at high RH (> 90%), while BRC increases LE by around 30% for all RH conditions. Additionally, we assess the influence of these corrections on ET-based transpiration (T) estimates using two different ET partitioning methods. Results show opposite responses (increasing vs. slightly decreasing T-to-ET ratios, T/ET) between the two methods when comparing T based on corrected and uncorrected LE. Overall, our results demonstrate the existence of a high RH bias in water fluxes in the FLUXNET2015 dataset and suggest that this bias is a pronounced source of uncertainty in ET measurements to be considered when estimating ecosystem T/ET and WUE.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2023

The role of oak species in long-term soil P loss in a humid river bottomland

There is a gap in our understanding of if and how bottomland forest type will affect long-term nutrient cycling and loss. This study aims to determine how different forests affect soil hydrologic variability and whole-soil P loss in a humid-subtropical setting. Here, we used replicate-sampling and measured soil physical, chemical, and mineralogical properties at 12 sites in two forest ecosystems, post oak (Quercus stellata) and cherry bark oak (Quercus pagoda) in Clarks River National Wildlife Refuge in Western Kentucky. We hypothesize that wetting–drying events in redox soils of forested bottomlands can cause positive feedback in whole-soil P loss. Trees with greater P demand (e.g., post oak) take up more water creating more frequent and pronounced episodes in swelling and shrinking of expandable clays. Repeated swelling and shrinking of clays occlude the surface of Fe-Mn oxides from further adsorption of P in acidic soil. This can lead to greater loss or plant uptake of available P. Our results show (i) a significant difference in mean whole-soil P loss between the oak species with more loss in soils underlying the post oak forest, and (ii) a difference in the total P found in the sap- and heartwood of the two oak species. Soil analysis reveals that the clay mineralogy of the post and cherry bark oak sites are similar, and thus, may only play a minor role in governing the whole-soil P loss difference. However, the leaf data analysis suggests that the post oak site could be P and nitrogen-limited, while the cherry bark is only nitrogen limited. Our study shows that differences in the oak forest ecosystem may affect the long-term balance in water and nutrient uptake and may alter the redistribution of nutrients in the canopy and the underlying soils.

58 GEOSCIENCES↗
DOE OSTI2023

The physics of desiccation cracks 1: Ductile fracturing and dependence on relative humidity

Ductile deformation is ubiquitously found in the shrinkage of geomaterials. The existence of ductility requires elastoplastic mechanics when analyzing the structure deformation under external stress. Here, in this work, we explore the physics of ductile fracturing based on the results from desiccation experiments and triaxial tests. By using the digital image correlation (DIC) method to generate the strain maps of samples undergoing desiccation cracking under different relative humidities, we obtain results showing the previously postulated Cnoidal Wave ductile failure patterns propagating under atmospheric condition-controlled crack velocities. We then correlate these observations with rate-dependent plasticity models calibrated through triaxial tests undergoing several unloading–reloading cycles and velocity stepping. This work demonstrates the necessity to consider ductility in soil cracking, indicating that the formation of crack patterns in soil desiccation is a slow and predictable process.

58 GEOSCIENCES↗
DOE OSTI2019

A new approach for drying moist air: The ideal Claridge-Culp-Liu dehumidification process with membrane separation, vacuum compression and sub-atmospheric condensation; Une nouvelle approche pour assécher l’air humide: Le procédé idéal de déshumidification Claridge-Culp-Liu avec séparation membranaire, compression sous vide et condensation sous-atmosphérique

The Claridge-Culp-Liu Dehumidification Process is a novel and efficient approach to removing water vapor from air using a combination of membrane separation, vacuum compression and sub-atmospheric condensation. The basic theory of this process is to separate water vapor from moist air flowing across one side of a membrane by applying a partial vacuum to the opposite side of the membrane and then compressing the water vapor to its saturation pressure at the wet-bulb temperature of the ambient air so as to facilitate condensation. We report this process has a fundamental efficiency limit that approximates the Carnot limit, but for eight different ideal dehumidification-only cases examined herein, the process requires only 26–56% the energy required by a Carnot vapor-compression system. Furthermore, the limiting energy required by an ideal 5-stage membrane system is 16–31% that of a Carnot system for the same cases. Of special importance, the ideal Claridge-Culp-Liu Dehumidification Process requires less than 5% of the energy required by an ideal desiccant process for all cases treated. The Claridge-Culp-Liu Dehumidification Process can also be combined with evaporative cooling to provide dehumidification and sensible cooling with the temperature and humidity controlled independently. Of special importance, this system uses no HFC refrigerants, and it generates pure water as a by-product.

42 ENGINEERING↗
DOE OSTI2016

PEDOT:PSS/QCM-based multimodal humidity and pressure sensor

A room-temperature multimodal sensor composed of PEDOT:PSS deposited on an AT-cut quartz crystalmicrobalance (QCM) crystal has been fabricated. The nonlinear resistive and frequency sensor responses aredeconvolved using an articial neural network (ANN), which allows the single sensor to function simultane-ously as a relative humidity (RH) sensor and a pressure sensor using only two electrodes. We demonstratethat the predictive ability of the sensor is highly inuenced by the data used to train the ANN. When trainingsets are tailored to resemble the operating conditions of the sensor, the sensor achieves an average resolutionof < 3% RH from 0-100% RH, even after H 2 O saturation occurs on the surface. Our results indicate thatANNs show strong promise for improving the resolution of low cost gas sensors and for expanding the rangeof environmental conditions in which a given sensor can operate.

47 OTHER INSTRUMENTATION↗
DOE OSTI2019

Quantifying the Role of the Relative Humidity-Dependent Physical State of Organic Particulate Matter in the Uptake of Semivolatile Organic Molecules

The uptake of gas-phase dicarboxylic acids to organic particulate matter (PM) was investigated to probe the role of the PM physical state in exchange processes between gas-phase semivolatile organic molecules and organic PM. A homologous series of probe molecules, specifically isotopically labeled 13C-dicarboxylic acids, was used in conjunction with aerosol mass spectrometry to obtain a quantitative characterization of the uptake to organic PM for different relative humidities (RHs). The PM was produced by the dark ozonolysis of unlabeled α-pinene. The uptake of 13C-labeled oxalic, malonic, and α-ketoglutaric acids increased stepwise by 5 to 15 times with increases in RH from 15 to 80%. The enhanced uptake with increasing RH was explained primarily by the higher molecular diffusivity in the particle phase, as associated with changes in the physical state of the organic PM from a nonliquid state to a progressively less-viscous liquid state. At high RH, the partitioning of the probe molecules to the particle phase was more associated with physicochemical interactions with the organic PM than that with the co-absorbed liquid water. Additionally, uptake of the probe molecules also increased with a decrease in volatility along the homologous series. This study quantitatively shows the key roles of the particle physical state in governing the interactions of organic PM with semivolatile organic molecules.

42 ENGINEERING↗
DOE OSTI2024

Dynamics of Electric Polarization and Relaxation of Ions at Humid Calcite Surfaces

Mobile ions at mineral surfaces can respond to an applied electric field, adopting a new distribution that effectively represents polarization of the electrical double layer. When the field is released, the ions relax to their equilibrium distribution. In both cases, the dynamics are characteristic of the interface. However, current models of electrokinetic phenomena are not sufficiently robust to accurately predict collective ion dynamics at structurally and chemically specific mineral–water interfaces. Here, in this study, we use electrostatic force microscopy (EFM) to investigate the dynamics of ion relaxation at hydrated calcite (104) surfaces at controlled relative humidity (RH). Electrically biased probes are used to polarize the distributions of calcium and carbonate ions that are intrinsic to this interface across a range of RH values. Polarization kinetics are tracked by monitoring the tip–sample force gradient during charging, and EFM imaging is used to characterize the spatial relaxation dynamics after the applied field is released. Electrostatic finite element modeling of the sample/probe system across length-scales from nanometers to millimeters reproduces the observed stretched exponential charging response. Together, these results allow us to estimate the ion diffusivities at the interface across a wide range of RH values. These diffusivities increase by roughly 5 orders of magnitude as the RH is increased from 5 to 90%, highlighting the critical role of adsorbed water for surface ion solvation that enables ion mobility.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2016

Dissociation of sarin on a cement analogue surface: Effects of humidity and confined geometry

Here, first-principles molecular dynamics simulations were used to investigate the dissociation of sarin (GB) on the calcium silicate hydrate (CSH) mineral tobermorite (TBM), a surrogate for cement. CSH minerals (including TBM) and amorphous materials of similar composition are the major components of Portland cement, the binding agent of concrete. Metadynamics simulations were used to investigate the effect of the TBM surface and confinement in a microscale pore on the mechanism and free energy of dissociation of GB. Our results indicate that both the adsorption site and the humidity of the local environment significantly affect the sarin dissociation energy. In particular, sarin dissociation in a low-water environment occurs via a dealkylation mechanism, which is consistent with previous experimental studies.

36 MATERIALS SCIENCE↗
DOE OSTI2017

Structural Stability of N -Alkyl-Functionalized Titanium Metal–Organic Frameworks in Aqueous and Humid Environments

Here, we show that the highly photoredox active metal–organic framework (MOF) MIL-125-NHCyp exhibits crystalline and porosity stability in humid environments for more than 30 days as well as increased hydrophobicity compared to the unfunctionalized framework. This improved stability, in synergy with its high photocatalytic activity, makes this MOF an enticing candidate for large-scale applications in CO 2 photoreduction.

36 MATERIALS SCIENCE↗
DOE OSTI2018

Iodine Adsorption in Metal Organic Frameworks in the Presence of Humidity

Used nuclear fuel (UNF) reprocessing represents a unique challenge when dealing with radionuclides such as isotopes of 85 Kr and 129 I 2 , due to their volatility and long half-life. However, efficient capture of 129 I 2 (t 1/2 = 15.7 x 10 6 years) from the nuclear waste stream can help to reduce the risk of releasing I 2 radionuclide into the environment and mitigate concerns about human health problems. Metal organic frameworks (MOFs) have been reported to be potential I 2 adsorbents: but the effect of water vapor, generally present in the reprocessing off-gas stream is rarely taken into account. Moisture stable porous MOFs, which can selectively adsorb I 2 in presence of water vapor is thus of great interest. Herein, the I 2 adsorption performance of two microporous MOFs is reported in presence of different humidity. I…π phenyl ring interactions are mainly responsible for the adsorption as revealed by single crystal XRD

Iodine↗