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DOE OSTI2022

Composition, Emissions, and Air Quality Impacts of Hazardous Air Pollutants in Unburned Natural Gas from Residential Stoves in California

The presence of hazardous air pollutants (HAPs) entrained in end-use natural gas (NG) is an understudied source of human health risks. We performed trace gas analyses on 185 unburned NG samples collected from 159 unique residential NG stoves across seven geographic regions in California. Our analyses commonly detected 12 HAPs with significant variability across region and gas utility. Mean regional benzene, toluene, ethylbenzene, and total xylenes (BTEX) concentrations in end-use NG ranged from 1.6–25 ppmv–benzene alone was detected in 99% of samples, and mean concentrations ranged from 0.7–12 ppmv (max: 66 ppmv). By applying previously reported NG and methane emission rates throughout California’s transmission, storage, and distribution systems, we estimated statewide benzene emissions of 4,200 (95% CI: 1,800–9,700) kg yr –1 that are currently not included in any statewide inventories–equal to the annual benzene emissions from nearly 60,000 light-duty gasoline vehicles. Additionally, we found that NG leakage from stoves and ovens while not in use can result in indoor benzene concentrations that can exceed the California Office of Environmental Health Hazard Assessment 8-h Reference Exposure Level of 0.94 ppbv–benzene concentrations comparable to environmental tobacco smoke. This study supports the need to further improve our understanding of leaked downstream NG as a source of health risk.

42 ENGINEERING↗

NASA NTRS2000

BOREAS TGB-1 CH4 Concentration and Flux Data from NSA Tower Sites

The BOREAS TGB-1 team made numerous measurements of trace gas concentrations and fluxes at various NSA sites. This data set contains half-hourly averages of ambient methane (CH4) measurements and calculated fluxes for the NSA-Fen in 1996 and the NSA-BP and NSA-OJP tower sites in 1994. The purpose of this study was to determine the CH4 flux from the study area by measuring ambient CH 4 concentrations. This flux can then be compared to the chamber flux measurements taken at the same sites. The data are provided in tabular ASCII files.

Hall, Forrest G.↗

NASA NTRS1993

A two-dimensional model with coupled dynamics, radiative transfer, and photochemistry. 2: Assessment of the response of stratospheric ozone to increased levels of CO2, N2O, CH4, and CFC

The impact of increased levels of carbon dioxide (CO2), chlorofluorocarbons (CFCs), and other trace gases on stratospheric ozone is investigated with an interactive, two-dimensional model of gas phase chemistry, dynamics, and radiation. The scenarios considered are (1) a doubling of the CO2 concentration, (2) increases of CFCs, (3) CFC increases combined with increases of nitrous oxide (N2O) and methane CH4, and (4) the simultaneous increase of CO2, CFCs, N2O, and CH4. The radiative feedback and the effect of temperature and circulation changes are studied for each scenario. For the double CO2 calculations the tropospheric warming was specified. The CO2 doubling leads to a 3.1% increase in the global ozone content. Doubling of the CO2 concentrations would lead to a maximum cooling of about 12 C at 45 km if the ozone concentration were held fixed. The cooling of the stratosphere leads to an ozone increase with an associated increase in solar heating, reducing the maximum temperature drop by about 3 C. The CFC increase from continuous emissions at 1985 rate causes a 4.5% loss of ozone. For the combined perturbations a net loss of 1.3% is calculated. The structure of the perturbations shows a north-south asymmetry. Ozone losses (when expressed in terms of percent changes) are generally larger in the high latitudes of the southern hemisphere as a result of the eddy mixing being smaller than in the northern hemisphere. Increase of chlorine leads to ozone losses above 30 km altitude where the radiative feedback results in a cooler temperature and an ozone recovery of about one quarter of the losses predicted with a noninteractive model. In all the cases, changes in circulation are small. In the chlorine case, circulation changes reduce the calculated column depletion by about one tenth compared to offline calculations.

Schneider, Hans R.↗

DOE OSTI2025

Concentrations and Health Implications of As, Hg, and Cd and Micronutrients in Rice and Emissions of CH 4 From Variably Flooded Paddies

Abstract The flooded soil conditions under which rice is typically grown are beneficial for boosting yield and decreasing herbicide inputs but may pose a food safety and environmental health risk. Flooded soils lead to reducing conditions and anaerobic metabolisms of soil microorganisms, which mobilizes arsenic from soil into soil solution, where it can be absorbed by rice roots and transported to grain. These conditions also promote the production and emission of methane (CH 4 )—a potent greenhouse gas. To evaluate how water management affects metal(loid) grain concentrations and CH 4 emissions, we conducted a 2‐year field study in which rice paddy water was managed under a range of soil redox conditions that spanned from flooded to non‐flooded. We observed that growing rice under less flooded conditions decreased CH 4 emissions and concentrations of grain total As, grain inorganic As, grain total Hg, and grain inorganic Hg relative to flooded conditions, with more reductions observed as conditions were drier; grain organic As and Hg (MeHg) species also decreased with drier conditions particularly in Year 1. However, the driest conditions tested led to a 50%–97% increase in grain Cd concentrations that exceeded the CODEX limit and grain yield reductions as high as 25% and 40% in Year 1 and 2, respectively. While concentrations of toxic metal(loid)s could be manipulated by water management, micronutrient concentrations were similar or decreased with drier conditions, potentially increasing grain Cd bioaccessibility to humans. Because practices for rice water management are gaining momentum, more research should monitor grain Cd levels along with micronutrients.

Environmental Sciences & Ecology↗

DOE OSTI2026

Patch-level CO2 and CH4 fluxes and porewater concentrations in experimental wetlands, 5 and 10 PPT saltwater intrusion simulations, Louisiana 2023-2024

This dataset containes carbon dioxide (CO2) and methane (CH4) flux measurements collected from wetland vegetation patches dominated by Typha domingensis and Panicum hemitomon to assess greenhouse gas flux responses to experimental saltwater intrusion (SWI) pulses. Measurements were conducted before, during, and after simulated SWI events at target salinities of approximately 5 parts per thousand (ppt) with durations of 6, 10, and 17 days and 10 ppt with a duration of 48 days, alongside a control wetland (with no salinity added, flood manipulation only). These data were generated to evaluate how the magnitude and duration of SWI alter wetland carbon exchange and related biogeochemical and plant responses. This data package includes flux measurements from the wetland surface (i.e, soil/water surface and enclosed vegetation) and from the soil/water surface only; porewater and surface water concentrations of CO2 and CH4; salinity, pH, electrical conductivity collected in porewater (at 5, 10, and 20 cm soil depths) and in surface water; soil redox potential; leaf spectral indices, leaf vapor pressure deficit, stomatal conductance; water level, salinity, and photosynthetically active radiation; and aboveground biomass.

EARTH SCIENCE > AGRICULTURE > SOILS > SOIL RESPIRA↗

DOE OSTI2021

Review of Release Behavior of Hydrogen & Natural Gas Blends from Pipelines

Hydrogen can be used to reduce carbon emissions by blending into other gaseous energy carriers, such as natural gas. However, hydrogen blending into natural gas has important implications for safety which need to be evaluated. Hydrogen has different physical properties than natural gas, and these properties affect safety evaluations concerning a leak of the blended gas. The intent of this report is to begin to investigate the safety implications of blending hydrogen into the natural gas infrastructure with respect to a leak event from a pipeline. A literature review was conducted to identify existing data that will better inform future hazard and risk assessments for hydrogen/natural gas blends. Metrics with safety implications such as heat flux and dispersion behavior may be affected by the overall blend ratio of the mixture. Of the literature reviewed, there was no directly observed separation of the hydrogen from the natural gas or methane blend. No literature was identified that experimentally examined unconfined releases such as concentration fields or concentration at specific distances. Computational efforts have predicted concentration fields by modified versions of existing engineering models, but the validation of these models is limited by the unavailability of literature data. There are multiple literature sources that measured flame lengths and heat flux values, which are both relevant metrics to risk and hazard assessments. These data can be more directly compared to the outputs of existing engineering models for validation.

03 NATURAL GAS↗

NASA NTRS1995

Validation of Global Climatologies of Trace Gases Using NASA Global Tropospheric Experiment (GTE) Data

Methane is an important trace gas because it is a greenhouse gas that affects the oxidative capacity of the atmosphere. It is produced from biological and anthropogenic sources, and is increasing globally at a rate of approximately 0.6% per year [Climate Change 1992, IPCC]. By using National Oceanic and Atmospheric Administration/Climate Monitoring and Diagnostics Laboratory (NOAA/CMDL) ground station data, a global climatology of methane values was produced. Unfortunately, because the NOAA/CMDL ground stations are so sparse, the global climatology is low resolution. In order to compensate for this low resolution data, it was compared to in-situ flight data obtained from the NASA Global Tropospheric Experiment (GTE). The smoothed ground station data correlated well with the flight data. Thus, for the first time it is shown that the smoothing process used to make global contours of methane using the ground stations is a plausible way to approximate global atmospheric concentrations of the gas. These verified climatologies can be used for testing large-scale models of chemical production, destruction, and transport. This project develops the groundwork for further research in building global climatologies from sparse ground station data and studying the transport and distribution of trace gases.

Courchaine, Brian↗

NASA NTRS2001

Quantitative Species Measurements in Microgravity Combustion Flames

Flame-vortex interactions are canonical configurations that can be used to study the underlying processes occurring in complicated turbulent reacting flows. The elegant simplicity of the flame-vortex interaction permits the study of these complex interactions under relatively controllable experimental configurations, in contrast to direct measurements in turbulent flames. The ability to measure and model the fundamental phenomena that occur in a turbulent flame, but with time and spatial scales which are amenable to our diagnostics, permits significant improvements in the understanding of turbulent combustion under both normal and reduced gravity conditions. In this paper, we report absolute mole fraction measurements of methane in a reacting vortex ring. These microgravity experiments are performed in the 2.2-sec drop tower at NASA Glenn Research Center. In collaboration with Drs. Chen and Dahm at the University of Michigan, measured methane absorbances are incorporated into a new model from which the temperature and concentrations of all major gases in the flame can be determined at all positions and times in the development of the vortex ring. This is the first demonstration of the ITAC (Iterative Temperature with Assumed Chemistry) approach, and the results of these computations and analyses are presented in a companion paper by Dahm and Chen at this Workshop. We believe that the ITAC approach will become a powerful tool in understanding a wide variety of combustion flames under both equilibrium and non-equilibrium conditions.

Silver, Joel A.↗

NASA NTRS2016

Airborne In-Situ Measurements of Formaldehyde Over California: First Results from the Compact Formaldehyde Fluorescence Experiment (COFFEE) Instrument

Formaldehyde (HCHO) is one of the most abundant oxygenated volatile organic compounds (VOCs) in the atmosphere, playing a role multiple atmospheric processes. Measurements of HCHO can be used to help quantify convective transport, the abundance of VOCs, and ozone production in urban environments. The Compact Formaldehyde FluorescencE Experiment (COFFEE) instrument uses Non-Resonant Laser Induced Fluorescence (NR-LIF) to detect trace concentrations of HCHO as part of the Alpha Jet Atmospheric eXperiment (AJAX) payload. Developed at NASA GSFC, COFFEE is a small, low maintenance instrument with a sensitivity of 100 pptv and a quick response time (1 sec). The COFFEE instrument has been customized to fit in an external wing pod on the Alpha Jet aircraft based at NASA ARC. The instrument can operate over a broad range of altitudes, from boundary layer to lower stratosphere, making it well suited for the Alpha Jet, which can access altitudes from the surface up to 40,000 ft. Results of the first COFFEE science flights preformed over the California's Central Valley will be presented. Boundary layer measurements and vertical profiles in the tropospheric column will both be included. This region is of particular interest, due to its elevated levels of HCHO, revealed in satellite images, as well as its high ozone concentrations. In addition to HCHO, the AJAX payload includes measurements of atmospheric ozone, methane, and carbon dioxide. Formaldehyde is one of the few urban pollutants that can be measured from space. Plans to compare in-situ COFFEE data with satellite-based HCHO observations such as those from OMI (Aura) and OMPS (SuomiNPP) will also be presented.

ozone↗

NASA NTRS2016

Airborne In-Situ Measurements of Formaldehyde over California: First Results from the Compact Formaldehyde Fluorescence Experiment (COFFEE) Instrument

coffee↗

NASA NTRS2009

Effects of Temperature on Polymer/Carbon Chemical Sensors

Experiments were conducted on the effects of temperature, polymer molecular weight, and carbon loading on the electrical resistances of polymer/carbon-black composite films. The experiment were performed in a continuing effort to develop such films as part of the JPL Electronic Nose (ENose), that would be used to detect, identify, and quantify parts-per-million (ppm) concentration levels of airborne chemicals in the space shuttle/space station environments. The polymers used in this study were three formulations of poly(ethylene oxide) [PEO] that had molecular weights of 20 kilodaltons, 600 kilodaltons, and 1 megadalton, respectively. The results of one set of experiments showed a correlation between the polymer molecular weight and the percolation threshold. In a second set of experiments, differences among the temperature dependences of resistance were observed for different carbon loadings; these differences could be explained by a change in the conduction mechanism. In a third set of experiments, the responses of six different polymer/carbon composite sensors to three analytes (water vapor, methanol, methane) were measured as a function of temperature (28 to 36 C). For a given concentration of each analyte, the response of each sensor decreased with increasing temperature, in a manner different from those of the other sensors.

Manfireda, Allison↗

NASA NTRS2015

Quantitative Measurements of CH* Concentration in Normal Gravity and Microgravity Coflow Laminar Diffusion Flames

With the conclusion of the SLICE campaign aboard the ISS in 2012, a large amount of data was made available for the analysis of the effect of microgravity on laminar coflow diffusion flames. Previous work focused on the study of sooty flames in microgravity as well as the ability of numerical models to predict its formation in a simplified buoyancy-free environment. The current work shifts the investigation to soot-free flames, putting an emphasis on the chemiluminescence emission from electronically excited CH (CH*). This radical species is of significant interest in combustion studies: it has been shown that the CH* spatial distribution is indicative of the flame front position and, given the relatively simple diagnostic involved with its measurement, several works have been done trying to understand the ability of CH* chemiluminescence to predict the total and local flame heat release rate. In this work, a subset of the SLICE nitrogen-diluted methane flames has been considered, and the effect of fuel and coflow velocity on CH* concentration is discussed and compared with both normal gravity results and numerical simulations. Experimentally, the spectral characterization of the DSLR color camera used to acquire the flame images allowed the signal collected by the blue channel to be considered representative of the CH* emission centered around 431 nm. Due to the axisymmetric flame structure, an Abel deconvolution of the line-of-sight chemiluminescence was used to obtain the radial intensity profile and, thanks to an absolute light intensity calibration, a quantification of the CH* concentration was possible. Results show that, in microgravity, the maximum flame CH* concentration increases with the coflow velocity, but it is weakly dependent on the fuel velocity; normal gravity flames, if not lifted, tend to follow the same trend, albeit with different peak concentrations. Comparisons with numerical simulations display reasonably good agreement between measured and computed flame lengths and radii, and it is shown that the integrated CH* emission scales proportionally to the computed total heat release rate; the two-dimensional CH* spatial distribution, however, does not appear to be a good marker for the local heat release rate.

microgravity↗

NASA NTRS2012

Global Air Quality and Health Co-benefits of Mitigating Near-term Climate Change Through Methane and Black Carbon Emission Controls

Tropospheric ozone and black carbon (BC), a component of fine particulate matter (PM < or = 2.5 microns in aerodynamic diameter; PM2.5), are associated with premature mortality and they disrupt global and regional climate. Objectives: We examined the air quality and health benefits of 14 specific emission control measures targeting BC and methane, an ozone precursor, that were selected because of their potential to reduce the rate of climate change over the next 20-40 years. Methods: We simulated the impacts of mitigation measures on outdoor concentrations of PM2.5 and ozone using two composition-climate models, and calculated associated changes in premature PM2.5‑ and ozone-related deaths using epidemiologically derived concentration-response functions. Results: We estimated that, for PM2.5 and ozone, respectively, fully implementing these measures could reduce global population-weighted average surface concentrations by 23-34% and 7-17% and avoid 0.6-4.4 and 0.04-0.52 million annual premature deaths globally in 2030. More than 80% of the health benefits are estimated to occur in Asia. We estimated that BC mitigation measures would achieve approximately 98% of the deaths that would be avoided if all BC and methane mitigation measures were implemented, due to reduced BC and associated reductions of nonmethane ozone precursor and organic carbon emissions as well as stronger mortality relationships for PM2.5 relative to ozone. Although subject to large uncertainty, these estimates and conclusions are not strongly dependent on assumptions for the concentration-response function. Conclusions: In addition to climate benefits, our findings indicate that the methane and BC emission control measures would have substantial co-benefits for air quality and public health worldwide, potentially reversing trends of increasing air pollution concentrations and mortality in Africa and South, West, and Central Asia. These projected benefits are independent of carbon dioxide mitigation measures. Benefits of BC measures are underestimated because we did not account for benefits from reduced indoor exposures and because outdoor exposure estimates were limited by model spatial resolution.

air quality↗

NASA NTRS2005

Cassini-Huygens Probe Gas Chromatograph Mass Spectrometer (GCMS) Experiment: First Results

The Huygens Probe of the Cassini Huygens Mission entered the atmosphere of the moon Titan on January 14, 2005. The GCMS was part of the instrument complement on the probe to measure in situ the chemical composition of the atmosphere during the probe descent and to support the Aerosol Collector Pyrolyzer (ACP) experiment by serving as detector for the pyrolization products. The GCMS collected data from an altitude of 146 km to ground impact for a time interval of 2hours and 37minutes. The Probe and the GCMS survived the ground impact and collected data for 1hour and 9 minutes on the surface in the near surface environment until signal loss by the orbiter. The major constituents of the lower atmosphere were found to be N2 and CH4. The methane-mixing ratio was found to increase below the turbopause, about 35 km altitude, monotonically toward the surface to levels near saturation. After surface impact a steep increase of the mixing ratio was observed suggesting evaporation of surface condensed methane due to heating by the GCMS sample inlet heater. Other constituents were found to be in very low concentrations, below ppm levels. The presence of Argon 40 was confirmed. The results for the other noble gases are still being evaluated. Other hydrocarbons and nitriles were also observed and quantitative evaluation is in progress. Preliminary ratios for the major carbon and nitrogen isotopes were computed from methane and molecular nitrogen measurements. The instrument collected 5634 mass spectra during descent and 2692 spectra on the ground over a range of m/z from 2 to 141. Eight gas chromatograph samples were taken during the descent and two on the ground.

Niemann, H.↗

NASA NTRS2005

The Gas Chromatograph Mass Spectrometer (GCMS) Experiment on the Cassini-Huygens Probe: First Results

The Huygens Probe of the Cassini Huygens Mission entered the atmosphere of the moon Titan on January 14, 2005. The GCMS was part of the instrument complement on the Probe to measure in situ the chemical composition of the atmosphere during the probe descent and to support the Aerosol Collector Pyrolyzer (ACP) experiment by serving as detector for the pyrolization products. The GCMS collected data from an altitude of 146 km to ground impact for a time interval of 2 hours and 37 minutes. The Probe and the GCMS survived the ground impact and collected data for 1 hour and 9 minutes on the surface in the near surface environment until signal loss by the orbiter. The instrument collected 5634 mass spectra during descent and 2692 spectra on the ground over a range of m/z from 2 to 141. Eight gas chromatograph samples were taken during the descent and two on the ground. This is a report on work in progress. The major constituents of the lower atmosphere were found to be N2 and CH4. The methane-mixing ratio was found to increase below the turbopause, about 35 km altitude, monotonically toward the surface to levels near saturation. After surface impact a steep increase of the mixing ratio was observed suggesting evaporation of surface condensed methane due to heating by the GCMS sample inlet heater. Other constituents were found to be in very low concentrations, below ppm levels. The presence of Argon 40 was confirmed. The results for the other noble gases are still being evaluated. Other hydrocarbons and nitriles were also observed and quantitative evaluation is in progress. Preliminary ratios for the major carbon and nitrogen isotopes were computed from methane and molecular nitrogen measurements.

Niemann, H.↗

DOE OSTI2021

Soil gas probes for monitoring trace gas messengers of microbial activity

Abstract Soil microbes vigorously produce and consume gases that reflect active soil biogeochemical processes. Soil gas measurements are therefore a powerful tool to monitor microbial activity. Yet, the majority of soil gases lack non-disruptive subsurface measurement methods at spatiotemporal scales relevant to microbial processes and soil structure. To address this need, we developed a soil gas sampling system that uses novel diffusive soil probes and sample transfer approaches for high-resolution sampling from discrete subsurface regions. Probe sampling requires transferring soil gas samples to above-ground gas analyzers where concentrations and isotopologues are measured. Obtaining representative soil gas samples has historically required balancing disruption to soil gas composition with measurement frequency and analyzer volume demand. These considerations have limited attempts to quantify trace gas spatial concentration gradients and heterogeneity at scales relevant to the soil microbiome. Here, we describe our new flexible diffusive probe sampling system integrated with a modified, reduced volume trace gas analyzer and demonstrate its application for subsurface monitoring of biogeochemical cycling of nitrous oxide (N 2 O) and its site-specific isotopologues, methane, carbon dioxide, and nitric oxide in controlled soil columns. The sampling system observed reproducible responses of soil gas concentrations to manipulations of soil nutrients and redox state, providing a new window into the microbial response to these key environmental forcings. Using site-specific N 2 O isotopologues as indicators of microbial processes, we constrain the dynamics of in situ microbial activity. Unlocking trace gas messengers of microbial activity will complement -omics approaches, challenge subsurface models, and improve understanding of soil heterogeneity to disentangle interactive processes in the subsurface biome.

04 OIL SHALES AND TAR SANDS↗

DOE OSTI2022

Experimental validation of multiphysics model simulations of the thermal response of a cement clinker rotary kiln at laboratory scale

Abstract An increasing demand for buildings, transportation systems and civil infrastructure development has driven expansion of cement consumption world‐wide, producing a significant increase in related global energy demand. With approximately 7% of the world‐wide industrial energy consumption (10.7 exajoules [EJ]), the cement industry is the third most energy intensive industrial processes and a key component for concrete, the most consumed composite material in the global construction industry. In cement manufacturing, the cement kiln accounts for most of the energy consumption in the production process. As the heart of a cement plant, the cement kiln is where the kiln feed primarily containing calcium oxide (CaO), silica (SiO 2 ), alumina (Al 2 O 3 ), and iron (Fe 2 O 3 ) are thermally and chemically transformed into clinker minerals. The presented work developed a multiphysics model, designed and built a laboratory‐scale rotary cement clinker kiln, and produced cement clinker at laboratory‐scale. The model was developed to study the interaction between the various thermal, fluid dynamic and chemical interactions involved in the sintering process used to form Portland cement clinker in an effort to reduce energy use. The analytical model was validated through experimental testing using a unique laboratory‐scale rotary cement kiln developed during the investigation. Also demonstrated was the feasibility of producing clinker at laboratory scale. This modeling and lab scale tests were designed to better understand the clinker sintering process so that operational and quality decisions can be made to optimize energy consumption without compromising cement clinker quality. The computational fluid dynamics modeling was developed in COMSOL Multiphysics 6.0. The characteristics of the combustion fluid flow, concentration of species, temperature and heat transfer were studied for a turbulent flow of methane (CH 4 ) gas and oxygen (O 2 ). Theory suggests that heat transfer impacts the cement production process but the multiphysics model more accurately describes the convection, conduction, and radiant heat transfer in the kilning process and thus allows for a better understanding of the energy exchange driving the chemical reactions that produce Portland cement. Clinker minerals were formed because of appropriate burning conditions implemented during experimental model validation.

Tabares, Juan David↗

NASA NTRS1975

Ambient Atmospheric Hydrocarbon Content as Determined by Gas Chromatographic Techniques from Rural Tidewater Virginia in Late Spring 1974

In an attempt to ascertain the naturally generated hydrocarbon contribution to the air quality of the Hampton Roads region of Tidewater Virginia, a series of 27 air samples was obtained in two rural locations during late spring of 1974. These samples were analyzed for their hydrocarbon content (carbon number range C5 to C10) using gas chromatographic techniques. The thirty different hydrocarbon species were identified and monitored in the experiment. Preliminary analysis of the data indicates an average concentration of 397 parts per billion by weight (carbon) for the total non-methane hydrocarbon loading for C5 to C10 during the experiment. This value exceeds the National Primary Air Quality Standards as set by the Environmental Protection Agency.

Copeland, G. E.↗