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DOE OSTI2017

Increasing atmospheric humidity and CO 2 concentration alleviate forest mortality risk

Climate-induced forest mortality is being increasingly observed throughout the globe. Alarmingly, it is expected to exacerbate under climate change due to shifting precipitation patterns and rising air temperature. However, the impact of concomitant changes in atmospheric humidity and CO 2 concentration through their influence on stomatal kinetics remains a subject of debate and inquiry. By using a dynamic soil–plant–atmosphere model, mortality risks associated with hydraulic failure and stomatal closure for 13 temperate and tropical forest biomes across the globe are analyzed. The mortality risk is evaluated in response to both individual and combined changes in precipitation amounts and their seasonal distribution, mean air temperature, specific humidity, and atmospheric CO 2 concentration. Model results show that the risk is predicted to significantly increase due to changes in precipitation and air temperature regime for the period 2050–2069. However, this increase may largely get alleviated by concurrent increases in atmospheric specific humidity and CO 2 concentration. The increase in mortality risk is expected to be higher for needleleaf forests than for broadleaf forests, as a result of disparity in hydraulic traits. These findings will further facilitate decisions about intervention and management of different forest types under changing climate.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2023

High-temperature low-humidity proton exchange membrane with “stream-reservoir” ionic channels for high-power-density fuel cells

The perfluorosulfonic acid (PFSA) proton exchange membrane (PEM) is the key component for hydrogen fuel cells (FCs). We used in situ synchrotron scattering to investigate the PEM morphology evolution and found a “stream-reservoir” morphology, which enables efficient proton transport. The short-side-chain (SSC) PFSA PEM is fabricated under the guidance of morphology optimization, which delivered a proton conductivity of 193 milliSiemens per centimeter [95% relativity humidity (RH)] and 40 milliSiemens per centimeter (40% RH) at 80°C. The improved glass transition temperature, water permeability, and mechanical strength enable high-temperature low-humidity FC applications. Performance improvement by 82.3% at 110°C and 25% RH is obtained for SSC-PFSA PEM FCs compared to Nafion polymer PEM devices. The insights in chain conformation, packing mechanism, crystallization, and phase separation of PFSAs build up the structure-property relationship. In addition, SSC-PFSA PEM is ideal for high-temperature low-humidity FCs that are needed urgently for high-power-density and heavy-duty applications.

25 ENERGY STORAGE↗

DOE OSTI2017

Ionic composition of a humid air plasma under ionizing radiation

A kinetic model is proposed for ion–molecular processes involving charged particles of a humid air plasma produced by a fast electron beam. The model includes more than 600 processes involving electrons and 41 positive and 14 negative ions, including hydrated ions H{sub 3}O{sup +} (H{sub 2}O){sub n} and O{sub 2}{sup −}(H{sub 2}O){sub n} with n = 1, 2, …, 12. The energy costs of production of electron–ion pairs and electronic and vibrational (for water molecules, also rotational) excitation of molecules are calculated in nitrogen, oxygen, water vapor, air, and humid air. A method is proposed for calculating the energy costs in mixtures by the calculation data in pure gases. The evolution of the plasma composition is studied by the numerical solution of a system of 56 time-dependent balance equations for the number of charged particles of plasma by the fourth-order Runge–Kutta method. The steady-state composition of plasma is determined by solving nonlinear steady-state balance equations for the ionization rates of humid air from 10 to 10{sup 16} cm{sup –3}/s and the fraction of water molecules from 10{sup –3}% to 1.5%. It is established that, for water vapor content (the ratio of the number density of water molecules to the total number density of air molecules) of 0.015–1.5% in air at atmospheric pressure and room temperature, the main ion species are two types of positive ions H{sub 3}O{sup +} (H{sub 2}O){sub n} with the number of water molecules n = 5, 6 and three species of negative ions O{sub 2}{sup −}(H{sub 2}O){sub n} with n = 5, 8, 9.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2023

Predicting fatal heat and humidity using the heat index model

A unique wet-bulb temperature of 35°C is often used as the threshold for human survivability, but recent experiments have shown that a person’s core temperature starts to rise at a wide range of critical wet-bulb temperatures. Here, it is shown that the model underlying the heat index correctly predicts those critical wet-bulb temperatures, explaining 95% of the variance in the values observed in laboratory heat-stress experiments. This is the first time the heat-index model has been validated against physiological data from laboratory experiments. For light and moderate exertion in an indoor setting, the heat index model predicts that the critical wet-bulb temperature ranges from 20 to 32°C, depending on the relative humidity, consistent with experimental results. Furthermore, for the same setting and exertion, the heat index model predicts fatal wet-bulb temperatures ranging from 24 to 37°C. Recent experiments have identified the critical combinations of heat and humidity, in an indoor setting, above which an individual is unable to maintain a standard core temperature, indicating severe heat stress. It is shown here why this state of severe heat stress cannot be predicted using the wet-bulb temperature. Instead, it is shown that the recently extended heat index model can explain nearly all of the variance in the observed critical combinations of temperature and humidity, and can be used to calculate fatal combinations.

59 BASIC BIOLOGICAL SCIENCES↗

DOE OSTI2021

Survival of Snow in the Melting Layer: Relative Humidity Influence

This study quantifies how far snow can fall into the melting layer (ML) before all snow has melted by examining a combination of in-situ observations from aircraft measurements in Lagrangian spiral descents from above through the ML and descents and ascents into the ML, as well as an extensive database of NOAA surface observer reports during the past 50 years. The airborne data contain information on the particle phase (solid, mixed, or liquid), population size distributions and shapes, along with temperature, relative humidity, and vertical velocity. A wide range of temperatures and ambient relative humidities are used for both the airborne and ground-based data. It is shown that an ice bulb temperature of 0°C, together with the air temperature and pressure (altitude), are good first order predictors of the highest temperature snowflakes can survive in the melting layer before completely melting. Particle size is also important, as is whether the particles are graupel or hail. If the relative humidity is too low, the particles will sublimate completely as they fall into the melting layer. Snow as warm as +7°C is observed from aircraft measurements and surface observations. Snow pellets survive to even warmer temperatures. Relationships are developed to represent the primary findings.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2016

Plant Growth Environments with Programmable Relative Humidity and Homogeneous Nutrient Availability

We describe the design, characterization, and use of “programmable”, sterile growth environments for individual (or small sets of) plants. The specific relative humidities and nutrient availability experienced by the plant is established (RH between 15% and 95%; nutrient concentration as desired) during the setup of the growth environment, which takes about 5 minutes and <1$ in disposable cost. These systems maintain these environmental parameters constant for at least 14 days with minimal intervention (one minute every two days). The design is composed entirely of off-the-shelf components (e.g., LEGO1 bricks) and is characterized by (i) a separation of root and shoot environment (which is physiologically relevant and facilitates imposing specific conditions on the root system, e.g., darkness), (ii) the development of the root system on a flat surface, where the root enjoys constant contact with nutrient solution and air, (iii) a compatibility with root phenotyping. We demonstrate phenotyping by characterizing root systems of Brassica rapa plants growing in different relative humidities (55%, 75%, and 95%). While most phenotypes were found to be sensitive to these environmental changes, a phenotype tightly associated with root system topology– the size distribution of the areas encircled by roots–appeared to be remarkably and counterintuitively insensitive to humidity changes. These setups combine many of the advantages of hydroponics conditions (e.g., root phenotyping, complete control over nutrient composition, scalability) and soil conditions (e.g., aeration of roots, shading of roots), while being comparable in cost and setup time to Magenta1 boxes.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2016

XPS Investigation on Changes in UO 2 Speciation following Exposure to Humidity

High purity UO 2 powder samples were subjected to accelerated aging under controlled conditions with relative humidity ranging from 34% to 98%. Characterization of the chemical speciation of the products was accomplished using X-ray photoelectron spectroscopy (XPS). A shift to higher uranium oxidation states was found to be directly correlated to increased relative humidity exposure. In addition, the relative abundance of O 2- , OH - , and H 2 O was found to vary with exposure time. Therefore, it is expected that uranium oxide materials exposed to high relative humidity conditions during processing and storage would display a similar increase in average uranium valence.

36 MATERIALS SCIENCE↗

DOE OSTI2014

Indoor Climate and Moisture Durability Performances of Houses with Unvented Attic Roof Constructions in a Mixed-Humid Climate

A sealed or unvented attic is an energy-efficient envelope component that can reduce the amount of energy a house consumes for space conditioning if the air handler and/or ducts are located in the attic. The attic is typically sealed by using spray foam on the underside of the roof deck and covering the soffit, ridge and gable vents to minimize air leakage from the attic to the outside. This approach can save up to 10% in space-conditioning energy when ducts are located in the attic (DOE 2013). Past research done by ORNL and Florida Solar Energy Center suggests that in more hot, humid climates, an unvented attic could potentially create a more humid, uncomfortable living environment than a vented attic (Colon 2011, Boudreaux, Pallin et al. 2013). Research showed that controlling the higher indoor humidity could reduce the energy savings from the sealed, unvented attic, which in turn would decrease the energy savings payback. Research also showed that the roof assembly (5.5 inches of open-cell foam, 1inch of closed-cell foam, OSB, felt paper, and asphalt shingles) stored moisture, thus acting as a moisture buffer. During the fall and winter, the roof assembly stored moisture and during the spring and summer it released moisture. This phenomenon is not seen in a vented attic, in which the air exchange rate to the outside is greater and, in the winter, helps to dehumidify the attic air. It was also seen that in a vented attic, the direction of water vapor diffusion is on average from the attic to the interior of the house. Air leakage from the attic to the interior also occurs during more of the year in a house with an unvented attic than in one with a vented attic. These discoveries show that the moisture dynamics in a house with an unvented attic are much different from those in a house with a vented attic. This study reports on a series of computer model investigations completed to determine the key variables impacting indoor comfort and the durability of roof assemblies against moisture. The key variables investigated were the leakage area from the attic to the outside, leakage area from the attic to the interior, leakage area from the interior to the outside, supply duct leakage in the attic, and interior moisture generation. These investigations are described in this report.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗

DOE OSTI2015

Fiberboard Humidity Data for 9975 Shipping Packages

The 9975 surveillance program is identifying a technical basis to support extending the storage period of 9975 packages in KAC beyond the currently approved 15 years. A key element of this effort is developing a better understanding of degradation of the fiberboard assembly under storage conditions. This degradation is influenced greatly by the moisture content of the fiberboard, which is not well characterized on an individual package basis. Two efforts have been undertaken to better understand the levels and behavior of moisture within the fiberboard assemblies of the 9975 shipping package. In the first effort, an initial survey of humidity and temperature in the upper air space of 26 packages stored in KAC was made. The data collected within this first effort help to illustrate how the upper air space humidity varies with the local ambient temperature and package heat load. In the second effort, direct measurements of two test packages are providing a correlation between humidity and fiberboard moisture levels within the package, and variations in moisture throughout the fiberboard assembly. This effort has examined packages with cane fiberboard and internal heat levels of 5 and 10W to date. Additional testing is expected to include 15 and 19W heat levels, and then repeat the same four heat levels with softwood fiberboard assemblies. This report documents the data collected to date within these two efforts.

36 MATERIALS SCIENCE↗

DOE OSTI2015

Fiberboard Humidity Data for 9975 Shipping Packages

36 MATERIALS SCIENCE↗

DOE OSTI2015

Fiberboard Humidity Data for 9975 Shipping Packages

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2021

Improved temperature control for measuring the humidity dependence of aerosol optical properties

Aerosols impact climate and cloud formation by their ability to take up water, which leads to changes in their optical properties. To better characterize the interactions of aerosol with water vapor, a humidification section has been added to the Cavity Attenuation Phase-shift Spectrometry (CAPS) instrument. The CAPS is a diode based method that provides simultaneous measurements of both aerosol total optical extinction and scattering in real-time. We are improving the humidity controlled sample line with new temperature controls. The current system suffers from particlelosses and poorly controlled humidity profiles, both of which were corrected for in the systems redesign. This improved wet-CAPS system has been integrated with a dry-CAPS to simultaneously measure the wet and dry aerosol optical properties. The two CAPS monitors were operated in a dry collection mode to ensure there were no biases between the instruments. Initial calibrations and data were collected to test the functionality of the dual CAPS system (wet + dry). The new two channel CAPS system improves our ability to measure the effects of humidity on aerosol optical properties.

58 GEOSCIENCES↗

DOE OSTI2018

On the role of aerosols, humidity, and vertical wind shear in the transition of shallow-to-deep convection at the Green Ocean Amazon 2014/5 site

Abstract. The preconditioning of the atmosphere for a shallow-to-deep convective transition during the dry-to-wet season transition period (August–November) is investigated using Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) GoAmazon2014/5 campaign data from March 2014 to November 2015 in Manacapuru, Brazil. In comparison to conditions observed prior to shallow convection, anomalously high humidity in the free troposphere and boundary layer is observed prior to a shallow-to-deep convection transition. An entraining plume model, which captures this leading dependence on lower tropospheric moisture, is employed to study indirect thermodynamic effects associated with vertical wind shear (VWS) and cloud condensation nuclei (CCN) concentration on preconvective conditions. The shallow-to-deep convective transition primarily depends on humidity, especially that from the free troposphere, which tends to increase plume buoyancy. Conditions preceding deep convection are associated with high relative humidity, and low-to-moderate CCN concentration (less than the 67th percentile, 1274 cm−3). VWS, however, shows little relation to moisture and plume buoyancy. Buoyancy estimates suggest that the latent heat release due to freezing is important to deep convective growth under all conditions analyzed, consistent with potential pathways for aerosol effects, even in the presence of a strong entrainment. Shallow-only convective growth, however, shows an association with a strong (weak) low (deep) level VWS and with higher CCN concentration.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2019

Timescales of secondary organic aerosols to reach equilibrium at various temperatures and relative humidities

Abstract. Secondary organic aerosols (SOA) account for a substantial fraction of air particulate matter, and SOA formation is often modeled assuming rapid establishment of gas–particle equilibrium. Here, we estimate the characteristic timescale for SOA to achieve gas–particle equilibrium under a wide range of temperatures and relative humidities using a state-of-the-art kinetic flux model. Equilibration timescales were calculated by varying particle phase state, size, mass loadings, and volatility of organic compounds in open and closed systems. Model simulations suggest that the equilibration timescale for semi-volatile compounds is on the order of seconds or minutes for most conditions in the planetary boundary layer, but it can be longer than 1 h if particles adopt glassy or amorphous solid states with high glass transition temperatures at low relative humidity. In the free troposphere with lower temperatures, it can be longer than hours or days, even at moderate or relatively high relative humidities due to kinetic limitations of bulk diffusion in highly viscous particles. The timescale of partitioning of low-volatile compounds into highly viscous particles is shorter compared to semi-volatile compounds in the closed system, as it is largely determined by condensation sink due to very slow re-evaporation with relatively quick establishment of local equilibrium between the gas phase and the near-surface bulk. The dependence of equilibration timescales on both volatility and bulk diffusivity provides critical insights into thermodynamic or kinetic treatments of SOA partitioning for accurate predictions of gas- and particle-phase concentrations of semi-volatile compounds in regional and global chemical transport models.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2021

Toward closure between predicted and observed particle viscosity over a wide range of temperatures and relative humidity

Abstract. Atmospheric aerosols can exist in amorphous semi-solid or glassy phase states whose viscosity varies with atmospheric temperature and relative humidity. The temperature and humidity dependence of viscosity has been hypothesized to be predictable from the combination of a water–organic binary mixing rule of the glass transition temperature, a glass-transition-temperature-scaled viscosity fragility parameterization, and a water uptake parameterization. This work presents a closure study between predicted and observed viscosity for sucrose and citric acid. Viscosity and glass transition temperature as a function of water content are compiled from literature data and used to constrain the fragility parameterization. New measurements characterizing viscosity of sub-100 nm particles using the dimer relaxation method are presented. These measurements extend the available data of temperature- and humidity-dependent viscosity to −28 ∘C. Predicted relationships agree well with observations at room temperature and with measured isopleths of constant viscosity at ∼107 Pa s at temperatures warmer than −28 ∘C. Discrepancies at colder temperatures are observed for sucrose particles. Simulations with the kinetic multi-layer model of gas–particle interactions suggest that the observed deviations at colder temperature for sucrose can be attributed to kinetic limitations associated with water uptake at the timescales of the dimer relaxation experiments. Using the available information, updated equilibrium phase-state diagrams (-80∘C

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2017

A humidity-controlled fast integrated mobility spectrometer (HFIMS) for rapid measurements of particle hygroscopic growth

We present a Humidity-controlled Fast Integrated Mobility Spectrometer (HFIMS) for rapid particle hygroscopicity measurements. The HFIMS consists of a differential mobility analyzer (DMA), a relative humidity (RH) control unit and a water-based FIMS (WFIMS) coupled in series. The WFIMS (Pinterich et al., 2017) combines the Fast Integrated Mobility Spectrometer (Kulkarni and Wang, 2006a, b) with laminar flow water condensation methodologies (Hering & Stolzenburg 2005; Spielman et al. 2017). Inside the WFIMS, particles of different electrical mobilities are spatially separated in an electric field, condensationally enlarged and imaged to provide 1-Hz measurements of size distribution spanning a factor of ~3 in particle diameter, sufficient to cover the entire range of growth factor for atmopheric aerosol particles at 90 % RH. By replacing the second DMA of a traditional hygroscopicity tandem DMA (HTDMA) system with the WFIMS, the HFIMS greatly increases the speed of particle growth factor measurement. The performance of the HFIMS was evaluated using NaCl particles with well-known hygroscopic growth behavior, and further through measurements of ambient aerosols. Results show that HFIMS can reproduce, within 2 % the literature values for hygroscopic growth of NaCl particles. NaCl deliquescence was observed between 76 % and 77 % RH in agreement with the theoretical value of 76.5 % (Ming and Russell, 2001), and efflorescence relative humidity (43 %) was found to lie within the RH range of 41 % to 56 % reported in the literature. Ambient data indicate that HFIMS can measure the hygroscopic growth of five standard dry particle sizes ranging from 35 to 165 nm within less than three minutes, which makes it about an order of magnitude faster than traditional HTDMA systems.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2021

Rapid measurement of RH-dependent aerosol hygroscopic growth using a humidity-controlled fast integrated mobility spectrometer (HFIMS)

Abstract. The ability of aerosol particles to uptake water (hygroscopic growth) is an important determinant of aerosol optical properties and radiative effects. Aerosol hygroscopic growth is traditionally measured by humidified tandem differential mobility analyzers (HTDMA), in which size-selected dry particles are exposed to elevated relative humidity (RH), and the size distribution of humidified particles is subsequently measured using a scanning mobility particle sizer. As a scanning mobility particle sizer can measure only one particle size at a time, HTDMA measurements are time consuming, and ambient measurements are often limited to a single RH level. Pinterich et al. (2017b) showed that fast measurements of aerosol hygroscopic growth are possible using a humidity-controlled fast integrated mobility spectrometer (HFIMS). In HFIMS, the size distribution of humidified particles is rapidly captured by a water-based fast integrated mobility spectrometer (WFIMS), leading to a factor of ∼10 increase in measurement time resolution. In this study we present a prototype HFIMS that extends fast hygroscopic growth measurements to a wide range of atmospherically relevant RH values, allowing for more comprehensive characterizations of aerosol hygroscopic growth. A dual-channel humidifier consisting of two humidity conditioners in parallel is employed such that aerosol RH can be quickly stepped among different RH levels by sampling from alternating conditioners. The measurement sequence is also optimized to minimize the transition time between different particle sizes. The HFIMS is capable of measuring aerosol hygroscopic growth of six particle diameters under five RH levels ranging from 20 % to 85 % (30 separate measurements) every 25 min. The performance of this HFIMS is characterized and validated using laboratory-generated ammonium sulfate aerosol standards. Measurements of ambient aerosols are shown to demonstrate the capability of HFIMS to capture the rapid evolution of aerosol hygroscopic growth and its dependence on both size and RH.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2017

A Humidity-controlled Fast Integrated Mobility Spectrometer (HFIMS) for rapid measurements of particle hygroscopic growth

We present a Humidity-controlled Fast Integrated Mobility Spectrometer (HFIMS) for rapid particle hygroscopicity measurements. The HFIMS consists of a differential mobility analyzer (DMA), a relative humidity (RH) control unit and a water-based FIMS (WFIMS) coupled in series. The WFIMS (Pinterich et al., 2017) combines the Fast Integrated Mobility Spectrometer (Kulkarni and Wang, 2006a, b) with laminar flow water condensation methodologies (Hering and Stolzenburg, 2005; Spielman et al., 2017). Inside the WFIMS, particles of different electrical mobilities are spatially separated in an electric field, condensationally enlarged and imaged to provide 1-Hz measurements of size distribution spanning a factor of ~ 3 in particle diameter, sufficient to cover the entire range of growth factor for atmospheric aerosol particles at 90 % RH. By replacing the second DMA of a traditional hygroscopicity tandem DMA (HTDMA) system with the WFIMS, the HFIMS greatly increases the speed of particle growth factor measurement. The performance of the HFIMS was evaluated using NaCl particles with well-known hygroscopic growth behavior, and further through measurements of ambient aerosols. Results show that HFIMS can reproduce, within 2 % the literature values for hygroscopic growth of NaCl particles. NaCl deliquescence was observed between 76 % and 77 % RH in agreement with the theoretical value of 76.5 % (Ming and Russell, 2001), and efflorescence relative humidity (43 %) was found to lie within the RH range of 41 % to 56 % reported in the literature. Ambient data indicate that HFIMS can measure the hygroscopic growth of five standard dry particle sizes ranging from 35 to 165 nm within less than three minutes, which makes it about an order of magnitude faster than traditional HTDMA systems.

54 ENVIRONMENTAL SCIENCES↗