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At least 541 records · Page 30
All sourcesNASA NTRSDOE OSTI
DOE OSTI2018

Lead exposure in young children over a 5-year period from urban environments using alternative exposure measures with the US EPA IEUBK model – A trial

Highlights: • IEUBK simulations of soil with petri dish dust (PDD), soil with handwipes, sweepings with PDD, sweepings with wipes. • Predicted blood lead levels (PbB) generally give good agreement with observed PbB in spite of differences in intake units for PDD and handwipes. • Analyses with dust loadings converted to concentration give higher predicted PbB. • Simulations on aggregated data for each child give similar results to age-stratified data. • Estimating house dust Pb from measured soil Pb concentrations (in the absence of measured house dust concentrations) results in over-prediction of PbB. The US Environmental Protection Agency (EPA) Integrated Exposure Uptake Biokinetic (IEUBK) model has been widely used to predict blood lead (PbB) levels in children especially around industrial sites. Exposure variables have strongly focussed on the major contribution of lead (Pb) in soil and interior dust to total intake and, in many studies, site-specific data for air, water, diet and measured PbB were not available. We have applied the IEUBK model to a comprehensive data set, including measured PbB, for 108 children monitored over a 5-year period in Sydney, New South Wales, Australia. To use this data set, we have substituted available data (with or without modification) for standard inputs as needed. For example, as an alternative measure for soil Pb concentration (μg/g), we have substituted exterior dust sweepings Pb concentration (μg/g). As alternative measures for interior dust Pb concentration (μg/g) we have used 1) 30-day cumulative petri dish deposition data (PDD) (as µg Pb/m{sup 2}/30days), or 2) hand wipe data (as μg Pb/hand). For comparison, simulations were also undertaken with estimates of dust Pb concentration derived from a prior regression of dust Pb concentration (μg/g) on dust Pb loading (μg/ft{sup 2}) as concentration is the unit specified for the Model. Simulations for each subject using observed data aggregated over the 5-year interval of the study, the most usual application of the IEUBK model, showed using Wilcoxon tests that there was a significant difference between the observed values and the values predicted by the Model containing soil with hand wipes (p < 0.001), and soil and PDD (p = 0.026) but not those for the other two sets of predictors, based on sweepings and PDD or sweepings and wipes. Overall, simulations of the Model using alternative exposure measures of petri dish dust (and possibly hand wipes) instead of vacuum cleaner dust and dust sweepings instead of soil provide predicted PbB which are generally consistent with each other and observed values. The predicted geometric mean PbBs were 2.17 ( ± 1.24) μg/dL for soil with PDD, 1.95 ( ± 1.17) μg/dL for soil with hand wipes, 2.36 ( ± 1.75) μg/dL for sweepings with PDD, and 2.15 ( ± 1.69) for sweepings with hand wipes. These results are in good agreement with the observed geometric mean PbB of 2.46 ( ± 0.99) μg/dL. In contrast to all other IEUBK model studies to our knowledge, we have stratified the data over the age ranges from 1 to 5 years. The median of the predicted values was lower than that for the observed values for every combination of age and set of measures; in some cases, the difference was statistically significant. The differences between observed and predicted PbB tended to be greatest for the soil plus wipes measure and for the oldest age group. Use of ‘default dust’ values calculated from the site-specific soil values, a common application of the IEUBK model, results in predicted PbB about 22% (range 0 to 52%) higher than those from soil with PDD data sets. Geometric mean contributions estimated from the Model to total Pb intake for a child aged 1–2 years was 0.09% for air, 42% for diet, 5.3% for water and 42% for soil and dust. Our results indicate that it is feasible to use alternative measures of soil and dust exposure to provide reliable predictions of PbB in urban environments.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2026

Illinois Storage Corridor - CarbonSAFE Phase III: Policy, Regulatory, Legal and Permitting Characteristics; Subtask 5.5

The Illinois Storage Corridor (ISC) project aims to advance the commercial development and implementation of carbon capture and storage (CCS) technologies within a region in Illinois of suitable geology for carbon dioxide (CO 2 ) storage in deep saline aquifers. The project partners have annual emissions greater than 6.5 million tonnes per year; storage hubs are being explored at two sites—one near the One Earth Energy facility in east-central Illinois, and one near the Prairie State Generating Company campus in southwest Illinois. To implement the technology, legal, policy, and economic considerations must be explored. The United States Environmental Protection Agency (US EPA) administers the Underground Injection Control (UIC) program and is responsible for issuing Class VI permits to construct and operate CO 2 injection wells, i.e., a UIC Class VI well permit is required to inject CO 2 into the subsurface for geologic sequestration. The largest consideration of the Class VI well requirements is to protect underground sources of drinking water (USDWs). Additionally discussed are considerations for Class VI permits relating to public engagement. Besides permitting, property rights to storage sites, subsurface pore spaces, and areas for pipeline transportation must be secured. Pore space rights is still a novel concept being explored and not yet addressed by the Illinois legislature. It is believed that surface property rights are required for the subsurface pore space below, so long as there is not a separated mineral estate in the subsurface. Illinois legislature has addressed securing rights-of-way for CO 2 transportation, allowing for easements and the exercise of eminent domain to secure such rights. Economically, the incentives for CCS are ever-expanding. Recently, the federal government broadened the availability and increased the dollar-amounts for the § 45Q tax credits for geological storage of carbon oxides. Congress has also authorized the Advanced Industrial Facilities Development Program which allocates billions of dollars in funds to installing technology at industrial facilities to reduce greenhouse gas emissions. On the state level, Illinois has had its own incentives for CCS projects since 2009 and expanded its emission-related goals again in 2021. The law enacted in 2021 specifically creates a commission to explore implementing CCS at Prairie State Generating Company, a partner on the Illinois Storage Corridor project.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2017

Radon Vapor Intrusion Screening Level Calculator - 17041

The U.S. Environmental Protection Agency has produced a web-based calculator for the assessment of cancer risk from radon in soil, soil gas, and pore water seeping into above-ground buildings. Like the chemical vapor intrusion screening level (VISL) calculator, the radon VISL (RVISL) provides screening levels in subsurface soil and water that are protective of preliminary remediation goals (PRGs) for radon in air that are based on either cancer risk or Applicable or Relevant and Appropriate Requirements (ARARs). In addition to the screening levels calculated, the RVISL can also calculate the risk from radon concentrations in soil, water, and air. The exposure routes evaluated in the RVISL are inhalation and external exposure from submersion in radon. Two source term options are provided for the user: one without radioactive decay and one with decay. Sources continually generating radon (Rn-222 and Rn-220), such as below ground uranium, would best be modeled with the 'without decay' models. Radon is the second leading cause of lung cancer. Radon is released from the normal decay of uranium, thorium, and radium in rocks and soil. It is an invisible, odorless, tasteless gas that seeps up through the ground and diffuses into the air. In areas without adequate ventilation, such as underground mines, radon can accumulate to levels that substantially increase the risk of lung cancer. Radon can enter homes through cracks in floors, walls, or foundations, and collect indoors. It can also be released from building materials, or from water obtained from wells that contain radon. Radon levels can be higher in homes that are well insulated, tightly sealed, and/or built on soil rich in the elements uranium, thorium, and radium. Basement and first floors typically have the highest radon levels because of their closeness to the ground. The RVISL will also allow for the calculation of screening levels for thoron (Rn-220) and Rn-219. The RVISL will be useful in assessing the final cleanup goals for subsurface soils where direct contact is not assumed. These sites can be landfills, buried waste cells or naturally occurring. By calculating protective levels of radon in subsurface soils, the likelihood of exceeding CERCLA protective standards (either risk range or ARARs) can be reduced. (authors)

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2012

Sulfur Polymer Stabilization/Solidification Treatability Study of Mercury Contaminated Soil from the Y-12 Site

As a result of past operations, the Department of Energy’s (DOE) Oak Ridge Y-12 National Security Complex (Y-12 Plant) has extensive mercury-contamination in building structures, soils, storm sewer sediments, and stream sediments, which are a source of pollution to the local ecosystem. Because of mercury’s toxicity and potential impacts on human health and the environment, DOE continues to investigate and implement projects to support the remediation of the Y-12 site. URS and #9122;CH2M Oak Ridge LLC (UCOR) under its prime contract with DOE has cleanup responsibilities on the DOE Oak Ridge Reservation and is investigating potential mercury-contaminated soil treatment technologies through an agreement with Babcock and Wilcox (B and W) Y-12, the Y-12 operating contractor to DOE. As part of its investigations, UCOR has subcontracted with Brookhaven National Laboratory (BNL) to conduct laboratory-scale studies evaluating the applicability of the Sulfur Polymer Stabilization/Solidification (SPSS) process using surrogate and actual mixed waste Y-12 soils containing mercury (Hg) at 135, 2,000, and 10,000 ppm. SPSS uses a thermoplastic sulfur binder to convert Hg to stable mercury sulfide (HgS) and solidifies the chemically stable product in a monolithic solid final waste form to reduce dispersion and permeability. Formulations containing 40 – 60 dry wt% Y-12 soil were fabricated and samples were prepared in triplicate for Environmental Protection Agency Toxicity Characteristic Leaching Procedure (TCLP) testing by an independent laboratory. Those containing 50 and 60 wt% soil easily met the study criteria for maximum allowable Hg concentrations (47 and 1 ppb, respectively compared with the TCLP limit of 200 ppb Hg). The lowest waste loading of 40 wt% yielded TCLP Hg concentrations slightly higher (240 ppb) than the allowable limit. Since the Y-12 soil tended to form clumps, the improved leaching at higher waste loadings was probably due to reduction in particle size from friction of the soil mixing, which creates more surface area for chemical conversion. This was corroborated by the fact that the same waste loading pre-treated by ball milling to reduce particle size prior to SPSS processing yielded TCLP concentrations almost 30 times lower, and at 8.5 ppb Hg was well below EPA limits. Pre-treatment by ball milling also allowed a reduction in the time required for stabilization, thus potentially reducing total process times by 30%.Additional performance testing was conducted including measurement of compressive strength to confirm mechanical integrity and immersion testing to determine the potential impacts of storage or disposal under saturated conditions. For both surrogate and actual Y-12 treated soils, waste form compressive strengths ranged between 2,300 and 6,500 psi, indicating very strong mechanical integrity (a minimum of greater than 40 times greater than the NRC guidance for low-level radioactive waste). In general, compressive strength increases with waste loading as the soil acts as an aggregate in the sulfur concrete waste forms. No statistically significant loss in strength was recorded for the 30 and 40 wt% surrogate waste samples and only a minor reduction in strength was measured for the 43 wt% waste forms. The 30 wt% Y-12 soil did not show a significant loss in strength but the 50 wt% samples were severely degraded in immersion due to swelling of the clay soil. The impact on Hg leaching, if any, was not determined.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2013

Uranium Fate and Transport Modeling, Guterl Specialty Steel Site, New York - 13545

The Former Guterl Specialty Steel Corporation Site (Guterl Site) is located 32 kilometers (20 miles) northeast of Buffalo, New York, in Lockport, Niagara County, New York. Between 1948 and 1952, up to 15,875 metric tons (35 million pounds) of natural uranium metal (U) were processed at the former Guterl Specialty Steel Corporation site in Lockport, New York. The resulting dust, thermal scale, mill shavings and associated land disposal contaminated both the facility and on-site soils. Uranium subsequently impacted groundwater and a fully developed plume exists below the site. Uranium transport from the site involves legacy on-site pickling fluid handling, the leaching of uranium from soil to groundwater, and the groundwater transport of dissolved uranium to the Erie Canal. Groundwater fate and transport modeling was performed to assess the transfer of dissolved uranium from the contaminated soils and buildings to groundwater and subsequently to the nearby Erie Canal. The modeling provides a tool to determine if the uranium contamination could potentially affect human receptors in the vicinity of the site. Groundwater underlying the site and in the surrounding area generally flows southeasterly towards the Erie Canal; locally, groundwater is not used as a drinking water resource. The risk to human health was evaluated outside the Guterl Site boundary from the possibility of impacted groundwater discharging to and mixing with the Erie Canal waters. This condition was evaluated because canal water is infrequently used as an emergency water supply for the City of Lockport via an intake located approximately 122 meters (m) (400 feet [ft]) southeast of the Guterl Site. Modeling was performed to assess whether mixing of groundwater with surface water in the Erie Canal could result in levels of uranium exceeding the U.S. Environmental Protection Agency (USEPA) established drinking water standard for total uranium; the Maximum Concentration Limit (MCL). Geotechnical test data indicate that the major portion of uranium in the soil will adsorb or remain bound to soil, yet leaching to groundwater appears as an on-site source. Soil leaching was modeled using low adsorption factors to replicate worst-case conditions where the uranium leaches to the groundwater. Results indicate that even after several decades, which is the period of time since uranium was processed at the Guterl Site, leaching from soil does not fully account for the currently observed levels of groundwater contamination. Modeling results suggest that there were historic releases of uranium from processing operations directly to the shallow fractured rock and possibly other geochemical conditions that have produced the current groundwater contamination. Groundwater data collected at the site between 1997 and 2011 do not indicate an increasing level of uranium in the main plume, thus the uranium adsorbed to the soil is in equilibrium with the groundwater geochemistry and transport conditions. Consequently, increases in the overall plume concentration or size are not expected. Groundwater flowing through fractures under the Guterl Site transports dissolved uranium from the site to the Erie Canal, where the groundwater has been observed to seep from the northern canal wall at some locations. The seeps discharge uranium at concentrations near or below the MCL to the Erie Canal. Conservative mixing calculations were performed using two worst-case assumptions: 1) the seeps were calculated as contiguous discharges from the Erie Canal wall and 2) the uranium concentration of the seepage is 274 micrograms per liter (μg/L) of uranium, which is the highest on-site uranium concentration in groundwater and nearly ten-fold the actual seep concentrations. The results indicate that uranium concentrations in the seep water would have to be more than 200 times greater than the highest observed on-site groundwater concentrations (or nearly 55,000 μg/L) to potentially exceed the drinking water standard (the MCL) for total uranium in the Erie Canal. (authors)

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

The Development of Vocational Vehicle Drive Cycles and Segmentation

Under a collaborative interagency agreement between the U.S. Environmental Protection Agency and the U.S Department of Energy (DOE), the National Renewable Energy Laboratory (NREL) performed a series of in-depth analyses to characterize the on-road driving behavior including distributions of vehicle speed, idle time, accelerations and decelerations, and other driving metrics of medium- and heavy-duty vocational vehicles operating within the United States. As part of this effort, NREL researchers segmented U.S. medium- and heavy-duty vocational vehicle driving characteristics into three distinct operating groups or clusters using real world drive cycle data collected at 1 Hz and stored in NREL's Fleet DNA database. The Fleet DNA database contains millions of miles of historical real-world drive cycle data captured from medium- and heavy vehicles operating across the United States. The data encompass data from existing DOE activities as well as contributions from valued industry stakeholder participants. For this project, data captured from 913 unique vehicles comprising 16,250 days of operation were drawn from the Fleet DNA database and examined. The Fleet DNA data used as a source for this analysis has been collected from a total of 30 unique fleets/data providers operating across 22 unique geographic locations spread across the United States. This includes locations with topology ranging from the foothills of Denver, Colorado, to the flats of Miami, Florida. The range of fleets, geographic locations, and total number of vehicles analyzed ensures results that include the influence of these factors. While no analysis will be perfect without unlimited resources and data, it is the researchers understanding that the Fleet DNA database is the largest and most thorough publicly accessible vocational vehicle usage database currently in operation. This report includes an introduction to the Fleet DNA database and the data contained within, a presentation of the results of the statistical analysis performed by NREL, review of the logistic model developed to predict cluster membership, and a discussion and detailed summary of the development of the vocational drive cycle weights and representative transient drive cycles for testing and simulation. Additional discussion of known limitations and potential future work are also included in the report content.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2023

Quantification of oil and gas methane emissions in the Delaware and Marcellus basins using a network of continuous tower-based measurements

Abstract. According to the United States Environmental Protection Agency (US EPA), emissions from oil and gas infrastructure contribute 30 % of all anthropogenic methane (CH4) emissions in the US. Studies in the last decade have shown emissions from this sector to be substantially larger than bottom-up assessments, including the EPA inventory, highlighting both the increased importance of methane emissions from the oil and gas sector in terms of their overall climatological impact and the need for independent monitoring of these emissions. In this study we present continuous monitoring of regional methane emissions from two oil and gas basins using tower-based observing networks. Continuous methane measurements were taken at four tower sites in the northeastern Marcellus basin from May 2015 through December 2016 and five tower sites in the Delaware basin in the western Permian from March 2020 through April 2022. These measurements, an atmospheric transport model, and prior emission fields are combined using an atmospheric inversion to estimate monthly methane emissions in the two regions. This study finds the mean overall emission rate from the Delaware basin during the measurement period to be 146–210 Mg CH4 h−1 (energy-normalized loss rate of 1.1 %–1.5 %, gas-normalized rate of 2.5 %–3.5 %). Strong temporal variability in the emissions was present, with the lowest emission rates occurring during the onset of the COVID-19 pandemic. Additionally, a synthetic model–data experiment performed using the Delaware tower network shows that the presence of intermittent sources is not a significant source of uncertainty in monthly quantification of the mean emission rate. In the Marcellus, this study finds the overall mean emission rate to be 19–28 Mg CH4 h−1 (gas-normalized loss rate of 0.30 %–0.45 %), with relative consistency in the emission rate over time. These totals align with aircraft top-down estimates from the same time periods. In both basins, the tower network was able to constrain monthly flux estimates within ±20 % uncertainty in the Delaware and ±24 % uncertainty in the Marcellus. The results from this study demonstrate the ability to monitor emissions continuously and detect changes in the emissions field, even in a basin with relatively low emissions and complex background conditions.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2020

Success Using A Granular-Activated Carbon Filtration Swab to Rehabilitate Westbay{sup R} Multi-level Groundwater Monitoring Wells at the INL - 20544

In November 2015, tetrachloroethylene (PCE) was discovered in groundwater samples collected from a Westbay{sup R} multi-level groundwater monitoring well at the Idaho National Laboratory (INL).a Subsequent investigation determined that PCE was not present in the groundwater. The detected PCE was instead due to inadvertent contamination of the internal tubing fluid in the Westbay well-monitoring system, which is isolated from the surrounding groundwater. Further investigation showed that three of the 11 Westbay wells at the INL contained PCE-contaminated tubing fluid at concentrations above the U.S. Environmental Protection Agency's maximum contaminant level for drinking water (5 μg/L). Loose sediment at the bottom of some Westbay wells was also found to contain PCE; the three wells were then identified for rehabilitation as part of the INL well maintenance program. The unique construction of the Westbay wells - i.e., the small diameter (5.72 cm [2.25 in.]) and the depths of the tubing fluid ranging from 144.8 to 419 m (475 to 1,376 ft) below ground surface - posed unique challenges to the rehabilitation. Because the tubing fluid provides structural integrity, the fluid cannot be removed and then replaced without damaging the integrity of the Westbay well. Additionally, the small diameter of the systems and the associated depths limit the availability of equipment that can be used for the rehabilitation. After an evaluation of potential methods, it was determined that the use of an in-well, custom-fabricated, granular-activated-carbon filtration swab deployed via a wire line would provide the safest and most cost-effective method for rehabilitation. Westbay well rehabilitation started at well MIDDLE-2051 in late June 2018 and paused in December 2018 for the season. The PCE concentration in the tubing fluid at MIDDLE-2051 was initially reduced to a maximum concentration of 3.81 μg/L from a maximum of 642 μg/L, while the concentration of PCE in the sediment had been reduced from 5,360 to 2,270 μg/kg. Sampling was performed at MIDDLE-2051 again in August 2019, and the tubing fluid increased to a maximum concentration of 45.4 μg/L, while the concentration in the sediment decreased further to 1,890 μg/kg due to desorption of PCE from the sediment to the tubing fluid. Rehabilitation resumed at well MIDDLE-2050A in late August 2019, and the PCE concentration in the tubing fluid had been reduced to a maximum concentration of 19.0 μg/L. Although the method has been shown to be time-consuming, it has proven to be effective and safe for personnel performing the work and to the integrity of the well. Future sample data results at all wells will help determine an estimated completion of the rehabilitation. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2012

DECOMMISSIONING AND ENVRIONMENTAL CLEANUP OF SMALL ARMS TRAINING FACILITY

USDOE performed a (CERCLA) non-time critical removal (NTCR) action at the Small Arms Training Area (SATA) Site Evaluation Area (SEA) located at the Savannah River Site (SRS), in Aiken, South Carolina. From 1951 to May 2010, the SATA was used as a small weapons practice and qualifying firing range. The SATA consisted of 870.1 ha (2,150 ac) of woodlands and open field, of which approximately 2.9 ha (7.3 ac) were used as a firing range. The SATA facility was comprised of three small arms ranges (one static and two interactive), storage buildings for supplies, a weapons cleaning building, and a control building. Additionally, a 113- m (370-ft) long earthen berm was used as a target backstop during live-fire exercises. The berm soils accumulated a large amount of spent lead bullets in the berm face during the facilities 59- years of operation. The accumulation of lead was such that soil concentrations exceeded the U.S. Environmental Protection Agency (USEPA) residential and industrial worker regional screening levels (RSLs). The RSL threshold values are based on standardized exposure scenarios that estimate contaminant concentrations in soil that the USEPA considers protective of humans over a lifetime. For the SATA facility, lead was present in soil at concentrations that exceed both the current residential (400 mg/kg) and industrial (800 mg/kg) RSLs. In addition, the concentration of lead in the soil exceeded the Toxicity Characteristic Leaching Procedure (TCLP) (40 Code of Federal Regulations [CFR] 261.24) regulatory limit. The TCLP analysis simulates landfill conditions and is designed to determine the mobility of contaminants in waste. In addition, a principal threat source material (PTSM) evaluation, human health risk assessment (HHRA), and contaminant migration (CM) analysis were conducted to evaluate soil contamination at the SATA SEA. This evaluation determined that there were no contaminants present that constitute PTSM and the CM analysis revealed that no constituents posed a migration risk to groundwater. The NTCR action involved removal of approximately 12,092 m3 (15,816 yd3) of spent bullets and lead-impacted soil and off-site disposal. The removal action included soils from the berm area, a fill area that received scraped soils from the berm, and soil from a drainage ditch located on the edge of the berm area. Also included in the removal action was a mixture of soil, concrete, and asphalt from the other three range areas. Under this action, 11,796 m3 (15,429 yd3) of hazardous waste and impacted soil were removed from the SATA and transported to a permitted hazardous waste disposal facility (Lone Mountain Facility in Oklahoma) and 296 m3 (387 yd3) of nonhazardous waste (primarily concrete debris) were removed and transported to a local solid waste landfill for disposal. During the excavation process, the extent was continuously assessed through the use of a hand-held, field-portable X-ray fluorescence unit with results verified using confirmation sampling with certified laboratory analysis. Following the completion of the excavation and confirmation sampling, final contouring, grading, and establishment of vegetative cover was performed to stabilize the affected areas. The NTCR action began on August 17, 2010, and mechanical completion was achieved on April 27, 2011. The selected removal action met the removal action objectives (RAOs), is protective of human health and the environment both in the short- and long-term, was successful in removing potential ecological risks, and is protective of surface water and groundwater. Furthermore, the selected NTCR action met residential cleanup goals and resulted in the release of the SEA from restricted use contributing to the overall footprint reduction at SRS.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2012

Enhanced High Temperature Performance of NOx Reduction Catalyst Materials

Two primary NOx after-treatment technologies have been recognized as the most promising approaches for meeting stringent NOx emission standards for diesel vehicles within the Environmental Protection Agency’s (EPA’s) 2007/2010 mandated limits, NOx Storage Reduction (NSR) and NH3 selective catalytic reduction (SCR); both are, in fact being commercialized for this application. However, in looking forward to 2015 and beyond with expected more stringent regulations, the continued viability of the NSR technology for controlling NOx emissions from lean-burn engines such as diesels will require at least two specific, significant and inter-related improvements. First, it is important to reduce system costs by, for example, minimizing the precious metal content while maintaining, even improving, performance and long-term stability. A second critical need for future NSR systems, as well as for NH3 SCR, will be significantly improved higher and lower temperature performance and stability. Furthermore, these critically needed improvements will contribute significantly to minimizing the impacts to fuel economy of incorporating these after-treatment technologies on lean-burn vehicles. To meet these objectives will require, at a minimum an improved scientific understanding of the following things: i) the various roles for the precious and coinage metals used in these catalysts; ii) the mechanisms for these various roles; iii) the effects of high temperatures on the active metal performance in their various roles; iv) mechanisms for higher temperature NOx storage performance for modified and/or alternative storage materials; v) the interactions between the precious metals and the storage materials in both optimum NOx storage performance and long term stability; vi) the sulfur adsorption and regeneration mechanisms for NOx reduction materials; vii) materials degradation mechanisms in CHA-based NH3 SCR catalysts. The objective of this CRADA project between PNNL and Cummins, Inc. is to develop a fundamental understanding of the above-listed issues. Model catalysts that are based on literature formulations are the focus of the work being carried out at PNNL. In addition, the performance and stability of more realistic high temperature NSR catalysts, supplied by JM, are being studied in order to provide baseline data for the model catalysts that are, again, based on formulations described in the open literature. For this short summary, we will primarily highlight representative results from our recent studies of the stability of candidate high temperature NSR materials.

Environmental Molecular Sciences Laboratory↗
DOE OSTI2020

Big Sky Regional Carbon Sequestration Partnership (Phase III Final Scientific/Technical Report)

The Big Sky Carbon Sequestration Partnership (BSCSP) pursued a Phase III demonstration project at Kevin Dome in north central Montana. Kevin Dome covers approximately 700 square miles and is a naturally occurring CO 2 reservoir that is flanked by oil and gas fields. The carbon dioxide (CO 2 ) is in the upper Devonian Duperow (carbonate) formation and does not reach the spill point of the dome; therefore, the dome has potential as a CO 2 sequestration reservoir, a CO 2 supply, or as both if anthropogenic sources and enhanced oil recovery (EOR) operations are associated with the dome. Kevin Dome could potentially act as a buffer to continue accepting anthropogenic CO 2 when EOR flooding operations are interrupted or completed. The project objective was to produce one million tonnes of CO 2 from the gas cap of Kevin Dome, pipe it laterally, inject, and re-store it in the brine leg of the same formation to test the hub / buffer storage concept. This was to be accomplished by drilling up to five production wells, building a short pipeline and compression facilities, and drilling an injection well and several monitoring wells. BSCSP commenced outreach and site characterization activities including acquiring baseline data for near-surface insurance monitoring, acquiring 3-dimensional, 9-component surface seismic over the project area, drilling two test wells (one in the production area and one in the injection area), coring key intervals, and performing comprehensive logging. Well tests of those wells revealed two barriers to the project. The production (Danielson 33-17) well was perforated in multiple zones but failed to produce any significant CO 2 . This was despite being drilled in the near vicinity of a historic well that had produced 3700 MCF per day in a drill stem test. Modeling indicated that this was likely due to a phase change during production causing a temperature drop resulting in hydrate and/or water ice formation that clogged the formation. Tests of the injection zone (Wallewein 22-1) well indicated total dissolved solids (TDS) slightly below the EPA required 10,000 parts per million (ppm) for a Class VI underground injection control permit. While the project was initiated before Class VI rules were promulgated, and this was an experimental project (seemingly qualified for a Class V permit), the Environmental Protection Agency (EPA) indicated that injection would require a Class VI permit. The low salinity result was unexpected as contours plotted based on regional formation water quality data indicated an expected TDS above 20,000 ppm, and wells between the recharge zone and the Wallewein well tested above 10,000 ppm. Faced with the inability to obtain an injection permit, the demonstration project could not proceed. However, the project had generated valuable samples and data on a large natural analog including 32 sq. mi. of 3-D, 9-C seismic, 430 ft. of carbonate core covering seven different depositional environments taken from areas with, and without the presence of CO 2 , 30 ft. of core of two caprocks, a tight carbonate and an anhydrite, a full set of modern logs on both wells, and well tests. DOE decided to re-scope the project around completing studies utilizing this data. This report covers both the initial scope and the re-scope (Task / Section numbers preceded with an R). While the report covers a wide range of project activities, highlights of this work include: Development of a geostatic model using neural nets to match well logs to facies and using multi-waveform seismic to inform reservoir heterogeneity; Unique mechanical testing of permeability – stress relationship in two caprock materials; Development of full waveform inversion to generate a high resolution velocity model; Model development for dual permeability (fracture and matrix) systems to better account for matrix-matrix interactions; Joint seismic wave inversion (including the first quadr-joint inversion) exhibiting better imaging of a challenging reservoir zone in stiff rock; Core flow and core flood results on a reactive carbonate; and Innovative laboratory measurements of seismic response of fractured core as a function of fluid fill.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2018

Air Dispersion Modeling of Radioactive Releases During Proposed 236Z Rubble Pile Removal Activities

This report is part of the planning process for the removal of the 236Z rubble remaining as of January 1, 2018, at the Plutonium Finishing Plant (PFP) on the Hanford Site. This report documents an analysis considering standard techniques for the removal of demolition rubble. It does not document any decisions about the removal approaches. This document is intended to guide the establishment of a boundary for the application of an air monitoring regime. Atmospheric dispersion modeling using estimated release rates has been conducted to provide information on the location and levels of radioactive contamination that may be expected as the result of rubble removal activities. Hourly meteorological data collected over a 6-year period (2004–2009) were used to examine the effects of wind speed, direction, and stability on projected concentrations of contaminants in air and deposited on nearby surfaces. The source terms modeled in this report were based on the residual transuranic contamination levels that are anticipated to remain in the 236Z rubble following building demolition. The potential airborne concentrations were established using the five-factor formula from DOE-HDBK-3010 (DOE 1994) considering material-at-risk, damage ratio, airborne release fraction, respirable fraction, and leak path factor. Radioactive contamination emissions were calculated by release mechanism and rubble pile area for on-shift and off-shift activities. The emissions from the applicable sources were combined to provide emissions estimates for each day from each cleanup area. The U.S. Environmental Protection Agency’s (EPA’s) AERMOD computer code was used to estimate atmospheric dispersion and deposition of the released radioactive materials in the immediate vicinity of the planned rubble removal activities Both airborne and surface concentrations were modeled with AERMOD. Hourly derived air concentrations (DAC) were modeled for an array of receptors covering the rubble pile site and surrounding area. Peak (95th and 99th percentile) values of time-integrated air concentrations at these receptor points are derived from these hourly values, with modeling results reported as total incremental air concentrations in DAC-hours occurring over the selected time period. Total accumulated deposition amounts were also evaluated with AERMOD using the same array of receptors, with results reported as disintegrations per minute (dpm) per 100 cm2. Each rubble pile was considered in terms of its size, location, and estimated contamination levels. The modeling was based on the assumed sequence of the rubble removal activities. The results in this report are based on cleanup schedules and methods proposed by CHPRC. As of January 1, 2018, there are broadly three large rubble piles (west, footprint, and east) remaining of the 236Z Building process cell. It is assumed that the overall cleanup will require either 1) 30 days over a 6-week period, or 2) 60 days over a 12-week period. Work was assumed to be performed during 10-hour day shifts. The analysis shows that some releases of radioactive material are to be anticipated during the cleanup of the 236Z rubble piles. The modeling results presented here are closely tied to the details of how the rubble removal is to be conducted. The results indicate that for the rubble removal, the radiological exposures from the planned activities are predicted to be well below the designated limits for air and soil exposures. The cleanup of the 236Z main process cell rubble is expected to release some alpha-emitting radionuclides. However, results based on 6 years of hourly climatological data, two representative cleanup periods, realistic mitigating actions, and a bounding source term indicate that concentrations at the fence line of the PFP facilities should remain well below 12 DAC-hours/week. The results presented in this report are a reevaluation of a subset of the results presented in PNNL-20173 Rev. 4.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2018

Assessment of the Area of Review and Leakage Impact for Site 7 using the NRAP-IAM-CCS Tool, Northern Michigan Basin-CarbonSAFE Phase 1 Pre-Feasibility Study

U.S. Environmental Protection Agency’s (EPA’s) Class VI regulations require owners or operators of carbon storage projects to determine an Area of Review (AoR) representative of project risk to underground sources of drinking water (USDWs). The AoR is an estimate of the project footprint and is used to develop monitoring plans to ensure protection of USDWs. In this syudy, the NRAP-IAM-CS software tool was applied to estimate the AoR and the leakage potential of legacy wells located within the AoR to impact groundwater quality at a carbon storage screening site for the NMB-CS, Phase 1 project. The NRAP-IAM-CS is a science-based toolset developed by the U.S. Department of Energy for quantitative risk assessment of geologic sequestration of carbon dioxide (CO 2 ) (Pawar et al., 2016). The toolset adopts a stochastic approach in which predictions include site uncertainties using storage reservoir, leakage scenario, and shallow groundwater impact reduced order models (ROMs). Risk-based analysis done using the NRAP-IAM-CS yielded an AoR that was comparable to estimates defined by the critical pressure needed move fluid from the reservoir to the overlying USDW through an open wellbore. The risk-based AoR was slightly smaller than that based on the critical pressure (234 km 2 compared to 269 km 2 ), because small fluxes did not impact groundwater quality. Leakage from two legacy wells located within the AoR should not impact groundwater quality over the 30-year injection period. Legacy Well 1 penetrates the simulated CO 2 plume and would require a permeability of 5 x 10 -12 m 2 (~5 Darcy) to impact groundwater quality after about 20 years of injection. Legacy Well 2 falls outside of the CO 2 plume footprint, where reservoir pressures are too small to generate large enough leakage flux to change groundwater quality even with well permeabilities as high as 5 x 10 -11 m 2 (~50 Darcy). This work represents one of the first applications of the NRAP toolset for the screening of potential CO 2 storage sites. The toolset provides a risk-based method of evaluating the AoR and the impact of CO 2 or brine leakage through legacy wells. The following recommendations will strengthen the use of probabilistic assessments for site selection and permitting of Class VI CO 2 injection wells.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2013

A Case Study Correlating Innovative Gamma Ray Scanning Detection Systems Data to Surface Soil Gamma Spectrometry Results - 13580

HydroGeoLogic (HGL), Inc. completed a United States Environmental Protection Agency (USEPA) study to characterize radiological contamination at a site near Canoga Park, California. The characterized area contained 470 acres including the site of a prototype commercial nuclear reactor and other nuclear design, testing, and support operations from the 1950's until 1988 [1]. The site history included radiological releases during operation followed by D and D activities. The characterization was conducted under an accelerated schedule and the results will support the project remediation. The project has a rigorous cleanup to background agenda and does not allow for comparison to risk-based guidelines. To target soil sample locations, multiple lines of evidence were evaluated including a gamma radiation survey, geophysical surveys, historical site assessment, aerial photographs, and former worker interviews. Due to the time since production and decay, the primary gamma emitting radionuclide remaining is cesium-137 (Cs-137). The gamma ray survey covered diverse, rugged terrain using custom designed sodium iodide thallium-activated (NaI(Tl)) scintillation detection systems. The survey goals included attaining 100% ground surface coverage and detecting gamma radiation as sensitively as possible. The effectiveness of innovative gamma ray detection systems was tested by correlating field Cs-137 static count ratios to Cs-137 laboratory gamma spectrometry results. As a case study, the area encompassing the former location of the first nuclear power station in the U. S. was scanned, and second by second global positioning system (GPS)-linked gamma spectral data were evaluated by examining total count rate and nuclide-specific regions of interest. To compensate for Compton scattering from higher energy naturally occurring radionuclides (U-238, Th-232 and their progeny, and K-40), count rate ratios of anthropogenic nuclide-specific regions of interest to the total count rate were calculated. From the scanning data, locations with observed Cs-137 ratios exceeding six standard deviations above the mean ratio were mapped in high resolution [2]. Field teams returned to those locations to collect static count measurements using the same detection systems. Soil surface samples were collected at 30 locations and analyzed for Cs-137. An exponential correlation was identified between Cs-137 concentrations in surface soil and field-scanned Cs-137 ratios. The data indicate field minimum detectable concentration (MDC) of Cs-137 at 0.02 Bq/g (0.5 pCi/g) or lower depending on contaminant distribution in soil. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2013

Decommissioning and Environmental Cleanup of a Small Arms Training Facility - 13225

US DOE performed a (CERCLA) non-time critical removal (NTCR) action at the Small Arms Training Area (SATA) Site Evaluation Area (SEA) located at the Savannah River Site (SRS), in Aiken, South Carolina. From 1951 to May 2010, the SATA was used as a small weapons practice and qualifying firing range. The SATA consisted of 870.1 ha (2,150 ac) of woodlands and open field, of which approximately 2.9 ha (7.3 ac) were used as a firing range. The SATA facility was comprised of three small arms ranges (one static and two interactive), storage buildings for supplies, a weapons cleaning building, and a control building. Additionally, a 113- m (370-ft) long earthen berm was used as a target backstop during live-fire exercises. The berm soils accumulated a large amount of spent lead bullets in the berm face during the facilities 59- years of operation. The accumulation of lead was such that soil concentrations exceeded the U.S. Environmental Protection Agency (USEPA) residential and industrial worker regional screening levels (RSLs). The RSL threshold values are based on standardized exposure scenarios that estimate contaminant concentrations in soil that the USEPA considers protective of humans over a lifetime. For the SATA facility, lead was present in soil at concentrations that exceed both the current residential (400 mg/kg) and industrial (800 mg/kg) RSLs. In addition, the concentration of lead in the soil exceeded the Toxicity Characteristic Leaching Procedure (TCLP) (40 Code of Federal Regulations [CFR] 261.24) regulatory limit. The TCLP analysis simulates landfill conditions and is designed to determine the mobility of contaminants in waste. In addition, a principal threat source material (PTSM) evaluation, human health risk assessment (HHRA), and contaminant migration (CM) analysis were conducted to evaluate soil contamination at the SATA SEA. This evaluation determined that there were no contaminants present that constitute PTSM and the CM analysis revealed that no constituents posed a migration risk to groundwater. The NTCR action involved removal of approximately 12,092 m{sup 3} (15,816 yd{sup 3}) of spent bullets and lead-impacted soil and off-site disposal. The removal action included soils from the berm area, a fill area that received scraped soils from the berm, and soil from a drainage ditch located on the edge of the berm area. Also included in the removal action was a mixture of soil, concrete, and asphalt from the other three range areas. Under this action, 11,796 m{sup 3} (15,429 yd{sup 3}) of hazardous waste and impacted soil were removed from the SATA and transported to a permitted hazardous waste disposal facility (Lone Mountain Facility in Oklahoma) and 296 m{sup 3} (387 yd{sup 3}) of nonhazardous waste (primarily concrete debris) were removed and transported to a local solid waste landfill for disposal. During the excavation process, the extent was continuously assessed through the use of a hand-held, field-portable X-ray fluorescence unit with results verified using confirmation sampling with certified laboratory analysis. Following the completion of the excavation and confirmation sampling, final contouring, grading, and establishment of vegetative cover was performed to stabilize the affected areas. The NTCR action began on August 17, 2010, and mechanical completion was achieved on April 27, 2011. The selected removal action met the removal action objectives (RAOs), is protective of human health and the environment both in the short- and long-term, was successful in removing potential ecological risks, and is protective of surface water and groundwater. Furthermore, the selected NTCR action met residential cleanup goals and resulted in the release of the SEA from restricted use contributing to the overall footprint reduction at SRS. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2020

Conventional and Next Generation Treatment Technologies for PFAS - 20067

In 2016, the United States Environmental Protection Agency (USEPA) established a Health Advisory Limit (HAL) for perfluorooctanoic acid (PFOA) and perfluorooctane sulfonic acid (PFOS) (individually and the summation) of 70 nanograms per liter (ng/L) based on developing toxicological information. These two compounds are among several thousand per- and polyfluoroalkyl substances (PFAS). Due to a multitude of commercially beneficial physical and chemical properties, the availability of PFAS-relevant and practical water treatment technologies is limited. The use of conventional adsorbents, such as activated carbon (AC) and anion exchange (AIX) resins, have become a 'de facto' interim measure to immediately address drinking water above this criterion. However, these adsorbents can have marginal long-term efficiency and are relatively unproven against the diversity of polyfluorinated compounds. Additionally, geochemical and/or co-contaminant competition can significantly impede adsorption based PFAS removal. These challenges may be addressed using engineered filtration, such as reverse osmosis or nanofiltration (RO/NF); however, for larger flow systems RO/NF may have unacceptable reject ratios as high as 35% and the capital cost may preclude these technologies. Extending these technologies to natural waters, which have various degrees of geochemical and co-contaminant competition, often requires a treatment train, combining conventional adsorbents or engineered filtration with pretreatment and more innovative and emerging remediation solutions for PFAS. Conventional and Next Generation water treatment technologies for PFAS generally employ one of three mechanisms (adsorption, separation, or destruction). These mechanisms include many types of technologies for both municipal drinking water and extracted natural water applications. The previously mentioned AC, AIX, and RO/NF are commercially available technologies that are actively being deployed for PFAS treatment. Research and development around these technologies is focused on optimization, and ultimate destruction of PFAS is achieved through incineration. Next Generation water treatment technologies include PFAS-specific flocculants, foam fractionation, novel AIX resins, new engineered adsorptive media, electrochemical treatment, sonolysis, and photolysis, radiation, and plasma (forms of advanced reductive processes [ARP]). Research and development around these technologies is focused on proof of concept and assimilation to real world applications. As the PFAS-relevant destructive technologies (such as incineration, electrochemical treatment, sonolysis, and ARP) are energy intensive, the state of the practice for PFAS water treatment is to focus adsorption/separation based technologies on reducing and concentrating the volume of water requiring destructive treatment. This enables more flexibility with respect to circulation frequency, residence time, and more control over energy usage. Water treatment for PFAS presently requires multiple technologies (i.e. a treatment train) to protect human health in a cost-conscious manner. An investment in research and development to explore new technologies is part of a key initiative for efficient protection of human health. This presentation attempts to review PFAS-relevant water treatment technologies and provide perspective as to their status with respect to applicability and commercial relevance. (authors)

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2013

Risk-Based Remediation Approach for Cs-137 Contaminated Sediment/Soils at the Savannah River Site (SRS) Lower Three Runs Tail (U) - 13348 - SRNS-RP-2012-00546

Lower Three Runs is a large blackwater stream that runs through the eastern and southern portion of the Savannah River Site. The Lower Three Runs watershed includes two SRS facility areas: P Area (P Reactor) and R Area (R Reactor) that provided effluent discharges to Lower Three Runs. During reactor operations, effluent discharges were well above natural (pre-industrial) or present day stream discharges. The watershed contains a 2,500-acre mainstream impoundment (PAR Pond), several smaller pre-cooler ponds, and a canal system that connects the pre-cooler ponds and discharges surface water to PAR Pond. From the PAR Pond dam, Lower Three Runs flows approximately 36 kilometers braiding through bottom-land/flood-plain forests before it enters the Savannah River. About eight kilometers downstream from the PAR Pond dam, the SRS boundary narrows (termed the Lower Three Runs tail) providing a limited buffer of DOE property for the Lower Three Runs stream and associated flood-plain. Previous screening characterization efforts revealed Cs-137 contamination in the sediment/soils of the flood-plain. As a part of the American Recovery and Reinvestment Act stimulus package, a comprehensive characterization effort was executed on the sediment/soils of the Lower Three Runs tail flood-plain providing a comprehensive look at the contaminant signature of the area. As a follow-up to that characterization, a regulatory decision Core Team, comprised of members of the South Carolina Department of Health and Environmental Control, Environmental Protection Agency - Region IV, and DOE, conducted negotiations on a risk-based approach to address the level of contamination found in the tail flood-plain as an early action that provided a long-term solution to exposure scenarios. For evaluation purposes, the adolescent trespasser was selected as the most likely human receptor for the Lower Three Runs tail portion because of the natural attractiveness of the area for recreational activities (i.e., hunting, fishing, hiking etc.) and access from public property. Exposure of the adolescent trespasser to Cs-137 contaminated sediment/soil at concentrations greater than 23.7 pico curies per gram have been calculated to result in an unacceptable cancer risk (> 1 x 10{sup -4}). Comparing the characterization sampling results conducted in 2009 with the benchmark concentration of 23.7 pCi/g, identified elevated risk levels along three sampling areas in the Lower Three Runs tail portion. On January 5, 2012, it was agreed by the core team that a Removal Action in the Lower Three Runs tail was to be conducted for the identified soil/sediment locations in the three identified areas that exceed the 1 x 10{sup -4} risk (23.7 pCi/g) for the adolescent trespasser receptor. The addition of Land Use Controls following the Removal Action was appropriate to protect human health and the environment. A systematic screening matrix was initiated at the identified hot spots (i.e., sampling points with Cs-137 activities greater than 23.7 pCi/g) to identify the limits of the excavation area. Sediment/soil within the defined removal areas would be excavated to the depth necessary to achieve the cleanup goal and disposed of in a CERCLA Off-Site Rule approved disposal facility. It was agreed that this removal action would adequately reduce the volume of available Cs-137 in the Lower Three Runs tail and consequently residual activities of the Cs-137 would decay over time reducing the amount of Cs-137 available in the tail which would curtail risk. The Land Use Controls consist of installation of an additional seven miles of fencing at major road crossings, utility easements, and at areas that showed a higher probability of access. In addition, signs were placed along the entire SRS perimeter of the Lower Three Runs tail approximately every 200 feet. Sign posts included both a No Trespassing sign and a Contaminant Warning sign. The project initiated a subcontract for both the removal action and the installation of fencing and signs on May 1, 2012. All field activities were completed by July 26, 2012. The project excavated and disposed of over 2700 cubic yards of contaminated sediment/soil, erected approximately seven miles of fence and placed over 2,000 signs demonstrating DOE's commitment to protect human health and act as a good neighbor to residents in the area. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2015

U.S. NO₂ trends (2005–2013): EPA air quality system (AQS) data versus improved observations from the Ozone Monitoring Instrument (OMI)

Emissions of nitrogen oxides (NO x ) and, subsequently, atmospheric levels of nitrogen dioxide (NO₂) have decreased over the U.S. due to a combination of environmental policies and technological change. Consequently, NO₂ levels have decreased by 30–40% in the last decade. We quantify NO₂ trends (2005–2013) over the U.S. using surface measurements from the U.S. Environmental Protection Agency (EPA) Air Quality System (AQS) and an improved tropospheric NO₂ vertical column density (VCD) data product from the Ozone Monitoring Instrument (OMI) on the Aura satellite.We demonstrate that the current OMI NO₂ algorithm is of sufficient maturity to allow a favorable correspondence of trends and variations in OMI and AQS data. Our trend model accounts for the non-linear dependence of NO₂ concentration on emissions associated with the seasonal variation of the chemical lifetime, including the change in the amplitude of the seasonal cycle associated with the significant change in NO x emissions that occurred over the last decade. The direct relationship between observations and emissions becomes more robust when one accounts for these non-linear dependencies. We improve the OMI NO₂ standard retrieval algorithm and, subsequently, the data product by using monthly vertical concentration profiles, a required algorithm input, from a high-resolution chemistry and transport model (CTM) simulation with varying emissions (2005-2013). The impact of neglecting the time-dependence of the profiles leads to errors in trend estimation, particularly in regions where emissions have changed substantially. For example, trends calculated from retrievals based on time-dependent profiles offer 18% more instances of significant trends and up to 15% larger total NO₂ reduction versus the results based on profiles for 2005. Using a CTM, we explore the theoretical relation of the trends estimated from NO₂ VCDs to those estimated from ground-level concentrations. The model-simulated trends in VCDs strongly correlate with those estimated from surface concentrations (r = 0.83, N = 355). We then explore the observed correspondence of trends estimated from OMI and AQS data. We find a significant, but slightly weaker, correspondence (i.e., r = 0.68, N = 208) than predicted by the model and discuss some of the important factors affecting the relationship, including known problems (e.g., NO z interferents) associated with the AQS data. This significant correspondence gives confidence in trend and surface concentration estimates from OMI VCDs for locations, such as the majority of the U.S. and globe, that are not covered by surface monitoring networks. Using our improved trend model and our enhanced OMI data product, we find that both OMI and AQS data show substantial downward trends from 2005 to 2013, with an average reduction of 38% for each over the U.S. The annual reduction rates inferred from OMI and AQS measurements are larger (–4.8 ± 1.9%/yr, –3.7 ± 1.5%/yr) from 2005 to 2008 than 2010 to 2013 (–1.2 ± 1.2%/yr, –2.1 ± 1.4%/yr). We quantify NO₂ trends for major U.S. cities and power plants; the latter suggest larger negative trend (–4.0 ± 1.5%/yr) between 2005 and 2008 and smaller or insignificant changes (–0.5 ± 1.2%/yr) during 2010-2013.

54 ENVIRONMENTAL SCIENCES↗