• Energy Research

New facility-level methane (CH4) emissions measurements obtained from 114 natural gas gathering facilities and 16 processing plants in 13 U.S. states were combined with facility counts obtained from state and national databases in a Monte Carlo simulation to estimate CH4 emissions from U.S. natural gas gathering and processing operations. Total annual CH4 emissions of 2421 (+245/-237) Gg were estimated for all U.S. gathering and processing operations, which represents a CH4 loss rate of 0.47% (±0.05%) when normalized by 2012 CH4 production. Over 90% of those emissions were attributed to normal operation of gathering facilities (1697 +189/-185 Gg) and processing plants (506 +55/-52 Gg), with the balance attributed to gathering pipelines and processing plant routine maintenance and upsets. The median CH4 emissions estimate for processing plants is a factor of 1.7 lower than the 2012 EPA Greenhouse Gas Inventory (GHGI) estimate, with the difference due largely to fewer reciprocating compressors, and a factor of 3.0 higher than that reported under the EPA Greenhouse Gas Reporting Program. Since gathering operations are currently embedded within the production segment of the EPA GHGI, direct comparison to our results is complicated. However, the study results suggest that CH4 emissions from gathering are substantially higher than the current EPA GHGI estimate and are equivalent to 30% of the total net CH4 emissions in the natural gas systems GHGI. Because CH4 emissions from most gathering facilities are not reported under the current rule and not all source categories are reported for processing plants, the total CH4 emissions from gathering and processing reported under the EPA GHGRP (180 Gg) represents only 14% of that tabulated in the EPA GHGI and 7% of that predicted from this study.

Abstract During the Ice in Clouds Experiment–Layer Clouds (ICE-L), aged biomass-burning particles were identified within two orographic wave cloud regions over Wyoming using single-particle mass spectrometry and electron microscopy. Using a suite of instrumentation, particle chemistry was characterized in tandem with cloud microphysics. The aged biomass-burning particles comprised ∼30%–40% by number of the 0.1–1.0-μm clear-air particles and were composed of potassium, organic carbon, elemental carbon, and sulfate. Aerosol mass spectrometry measurements suggested these cloud-processed particles were predominantly sulfate by mass. The first cloud region sampled was characterized by primarily homogeneously nucleated ice particles formed at temperatures near −40°C. The second cloud period was characterized by high cloud droplet concentrations (∼150–300 cm−3) and lower heterogeneously nucleated ice concentrations (7–18 L−1) at cloud temperatures of −24° to −25°C. As expected for the observed particle chemistry and dynamics of the observed wave clouds, few significant differences were observed between the clear-air particles and cloud residues. However, suggestive of a possible heterogeneous nucleation mechanism within the first cloud region, ice residues showed enrichments in the number fractions of soot and mass fractions of black carbon, measured by a single-particle mass spectrometer and a single-particle soot photometer, respectively. In addition, enrichment of biomass-burning particles internally mixed with oxalic acid in both the homogeneously nucleated ice and cloud droplets compared to clear air suggests either preferential activation as cloud condensation nuclei or aqueous phase cloud processing.

Abstract Ice concentrations in orographic wave clouds at temperatures between −24° and −29°C were shown to be related to aerosol characteristics in nearby clear air during five research flights over the Rocky Mountains. When clouds with influence from colder temperatures were excluded from the dataset, mean ice nuclei and cloud ice number concentrations were very low, on the order of 1–5 L−1. In this environment, ice number concentrations were found to be significantly correlated with the number concentration of larger particles, those larger than both 0.1- and 0.5-μm diameter. A variety of complementary techniques was used to measure aerosol size distributions and chemical composition. Strong correlations were also observed between ice concentrations and the number concentrations of soot and biomass-burning aerosols. Ice nuclei concentrations directly measured in biomass-burning plumes were the highest detected during the project. Taken together, this evidence indicates a potential role for biomass-burning aerosols in ice formation, particularly in regions with relatively low concentrations of other ice nucleating aerosols.

Chemical mass balance analysis was performed using a large dataset of molecular marker concentrations to estimate the contribution of biomass smoke to ambient organic carbon (OC) and fine particle mass in Pittsburgh, Pennsylvania. Source profiles were selected based on detailed comparisons between the ambient data and a large number of published profiles. The fall and winter data were analyzed with fireplace and woodstove source profiles, and open burning profiles were used to analyze the spring and summer data. At the upper limit, biomass smoke is estimated to contribute on average 520+/-140 ng-C m(-3) or 14.5% of the ambient OC in the fall, 210+/-85 ng-C m(-3) or 10% of the ambient OC in the winter, and 60 + 21 ng-C/m(-3) or 2% of the ambient OC in the spring and summer. In the fall and winter, there is large day-to-day variability in the amount of OC apportioned to biomass smoke. The levels of biomass smoke in Pittsburgh are much lower than in some other areas of the United States, indicating significant regional variability in the importance of biomass combustion as a source of fine particulate matter. The calculations face two major sources of uncertainty. First, the ambient ratios of levoglucosan, resin acids, and syringhaldehyde concentrations are highly variable implying that numerous sources with distinct source profiles contribute to ambient marker concentrations. Therefore, in contrast to previous CMB analyses, we find that at least three distinct biomass smoke source profiles must be included in the CMB model to explain this variability. Second, the marker-to-OC ratios of available biomass smoke profiles are highly variable. This variability introduces uncertainty of more than a factor of 2 in the amount of ambient OC apportioned to biomass smoke by different statistically acceptable CMB solutions. The marker-to-OC ratios of source profiles are critical parameters to consider when evaluating CMB solutions.

There is a need for continued assessment of methane (CH4) emissions associated with natural gas (NG) production, especially as recent advancements in horizontal drilling combined with staged hydraulic fracturing technologies have dramatically increased NG production (we refer to these wells as "unconventional" NG wells). In this study, we measured facility-level CH4 emissions rates from the NG production sector in the Marcellus region, and compared CH4 emissions between unconventional NG (UNG) well pad sites and the relatively smaller and older "conventional" NG (CvNG) sites that consist of wells drilled vertically into permeable geologic formations. A top-down tracer-flux CH4 measurement approach utilizing mobile downwind intercepts of CH4, ethane, and tracer (nitrous oxide and acetylene) plumes was performed at 18 CvNG sites (19 individual wells) and 17 UNG sites (88 individual wells). The 17 UNG sites included four sites undergoing completion flowback (FB). The mean facility-level CH4 emission rate among UNG well pad sites in routine production (18.8 kg/h (95% confidence interval (CI) on the mean of 12.0-26.8 kg/h)) was 23 times greater than the mean CH4 emissions from CvNG sites. These differences were attributed, in part, to the large size (based on number of wells and ancillary NG production equipment) and the significantly higher production rate of UNG sites. However, CvNG sites generally had much higher production-normalized CH4 emission rates (median: 11%; range: 0.35-91%) compared to UNG sites (median: 0.13%, range: 0.01-1.2%), likely resulting from a greater prevalence of avoidable process operating conditions (e.g., unresolved equipment maintenance issues). At the regional scale, we estimate that total annual CH4 emissions from 88 500 combined CvNG well pads in Pennsylvania and West Virginia (660 Gg (95% CI: 500 to 800 Gg)) exceeded that from 3390 UNG well pads by 170 Gg, reflecting the large number of CvNG wells and the comparably large fraction of CH4 lost per unit production. The new emissions data suggest that the recently instituted Pennsylvania CH4 emissions inventory substantially underestimates measured facility-level CH4 emissions by >10-40 times for five UNG sites in this study.

The recent growth in production and utilization of natural gas offers potential climate benefits, but those benefits depend on lifecycle emissions of methane, the primary component of natural gas and a potent greenhouse gas. This study estimates methane emissions from the transmission and storage (T&S) sector of the United States natural gas industry using new data collected during 2012, including 2,292 onsite measurements, additional emissions data from 677 facilities and activity data from 922 facilities. The largest emission sources were fugitive emissions from certain compressor-related equipment and "super-emitter" facilities. We estimate total methane emissions from the T&S sector at 1,503 [1,220 to 1,950] Gg/yr (95% confidence interval) compared to the 2012 Environmental Protection Agency's Greenhouse Gas Inventory (GHGI) estimate of 2,071 [1,680 to 2,690] Gg/yr. While the overlap in confidence intervals indicates that the difference is not statistically significant, this is the result of several significant, but offsetting, factors. Factors which reduce the study estimate include a lower estimated facility count, a shift away from engines toward lower-emitting turbine and electric compressor drivers, and reductions in the usage of gas-driven pneumatic devices. Factors that increase the study estimate relative to the GHGI include updated emission rates in certain emission categories and explicit treatment of skewed emissions at both component and facility levels. For T&S stations that are required to report to the EPA's Greenhouse Gas Reporting Program (GHGRP), this study estimates total emissions to be 260% [215% to 330%] of the reportable emissions for these stations, primarily due to the inclusion of emission sources that are not reported under the GHGRP rules, updated emission factors, and super-emitter emissions.

Emissions from solid-fuel cookstoves have been linked to indoor and outdoor air pollution, climate forcing, and human disease. Although task-based laboratory protocols, such as the Water Boiling Test (WBT), overestimate the ability of improved stoves to lower emissions, WBT emissions data are commonly used to benchmark cookstove performance, estimate indoor and outdoor air pollution concentrations, estimate impacts of stove intervention projects, and select stoves for large-scale control trials. Multiple-firepower testing has been proposed as an alternative to the WBT and is the basis for a new standardized protocol (ISO 19867-1:2018); however, data are needed to assess the value of this approach. In this work, we (a) developed a Firepower Sweep Test [FST], (b) compared emissions from the FST, WBT, and in-home cooking, and (c) quantified the relationship between firepower and emissions using correlation analysis and linear model selection. Twenty-three stove-fuel combinations were evaluated. The FST reproduced the range of PM2.5 and CO emissions observed in the field, including high emissions events not typically observed under the WBT. Firepower was modestly correlated with emissions, although the relationship varied between stove-fuel combinations. Our results justify incorporating multiple-firepower testing into laboratory-based protocols but demonstrate that firepower alone cannot explain the observed variability in cookstove emissions.