Ammonia Dry Deposition in an Alpine Ecosystem Traced to Agricultural Emission Hotpots.

Elevated reactive nitrogen (Nr) deposition is a concern for alpine ecosystems, and dry NH3 deposition is a key contributor. Understanding how emission hotspots impact downwind ecosystems through dry NH3 deposition provides opportunities for effective mitigation. However, direct NH3 flux measurements with sufficient temporal resolution to quantify such events are rare. Here, we measured NH3 fluxes at Rocky Mountain National Park (RMNP) during two summers and analyzed transport events from upwind agricultural and urban sources in northeastern Colorado. We deployed open-path NH3 sensors on a mobile laboratory and an eddy covariance tower to measure NH3 concentrations and fluxes. Our spatial sampling illustrated an upslope event that transported NH3 emissions from the hotspot to RMNP. Observed NH3 deposition was significantly higher when backtrajectories passed through only the agricultural region (7.9 ng m-2 s-1) versus only the urban area (1.0 ng m-2 s-1) and both urban and agricultural areas (2.7 ng m-2 s-1). Cumulative NH3 fluxes were calculated using observed, bidirectional modeled, and gap-filled fluxes. More than 40% of the total dry NH3 deposition occurred when air masses were traced back to agricultural source regions. More generally, we identified that 10 (25) more national parks in the U.S. are within 100 (200) km of an NH3 hotspot, and more observations are needed to quantify the impacts of these hotspots on dry NH3 deposition in these regions.

Methane emissions from natural gas vehicles in China.

Natural gas vehicles (NGVs) have been promoted in China to mitigate air pollution, yet our measurements and analyses show that NGV growth in China may have significant negative impacts on climate change. We conducted real-world vehicle emission measurements in China and found high methane emissions from heavy-duty NGVs (90% higher than current emission limits). These emissions have been ignored in previous emission estimates, leading to biased results. Applying our observations to life-cycle analyses, we found that switching to NGVs from conventional vehicles in China has led to a net increase in greenhouse gas (GHG) emissions since 2000. With scenario analyses, we also show that the next decade will be critical for China to reverse the trend with the upcoming China VI standard for heavy-duty vehicles. Implementing and enforcing the China VI standard is challenging, and the method demonstrated here can provide critical information regarding the fleet-level CH4 emissions from NGVs.

Variability of Ammonia and Methane Emissions from Animal Feeding Operations in Northeastern Colorado.

Concentrated animal feeding operations (CAFOs) are major emitters of both ammonia (NH3) and methane (CH4). However, current emission inventories have limited temporal resolution and use data derived from a small subset of farms. To this end, we deployed three mobile laboratories during the DISCOVER-AQ campaign in summer 2014 with a focus on northeastern Colorado. Observations of NH3 and CH4 plumes downwind of 43 CAFOs were used to investigate the diurnal and site-to-site variability of emissions with an inverse area source plume modeling approach. Ammonia emissions scaled to all permitted animals in Weld, Morgan, and Larimer counties were estimated at 1.9 Gg month-1, 50% greater than the U.S. NEI 2014 and 360% greater than EDGAR for the month of August. Methane emissions were likewise estimated at 10.6 Gg month-1, consistent with the U.S. GHGI but 99% greater than EDGAR. Significant differences between individual CAFOs with repeat observations were also observed for both CH4 and NH3 emissions. The large subfarm, site-to-site, and diurnal variabilities observed show the importance of measurements taken across these scales in order to derive representative emission factors.

Importance of Superemitter Natural Gas Well Pads in the Marcellus Shale.

A large-scale study of methane emissions from well pads was conducted in the Marcellus shale (Pennsylvania), the largest producing natural gas shale play in the United States, to better identify the prevalence and characteristics of superemitters. Roughly 2100 measurements were taken from 673 unique unconventional well pads corresponding to ∼18% of the total population of active sites and ∼32% of the total statewide unconventional natural gas production. A log-normal distribution with a geometric mean of 2.0 kg h-1 and arithmetic mean of 5.5 kg h-1 was observed, which agrees with other independent observations in this region. The geometric standard deviation (4.4 kg h-1) compared well to other studies in the region, but the top 10% of emitters observed in this study contributed 77% of the total emissions, indicating an extremely skewed distribution. The integrated proportional loss of this representative sample was equal to 0.53% with a 95% confidence interval of 0.45-0.64% of the total production of the sites, which is greater than the U.S. Environmental Protection Agency inventory estimate (0.29%), but in the lower range of other mobile observations (0.09-3.3%). These results emphasize the need for a sufficiently large sample size when characterizing emissions distributions that contain superemitters.

Vehicle Emissions as an Important Urban Ammonia Source in the United States and China.

Ammoniated aerosols are important for urban air quality, but emissions of the key precursor NH3 are not well quantified. Mobile laboratory observations are used to characterize fleet-integrated NH3 emissions in six cities in the U.S. and China. Vehicle NH3:CO2 emission ratios in the U.S. are similar between cities (0.33-0.40 ppbv/ppmv, 15% uncertainty) despite differences in fleet composition, climate, and fuel composition. While Beijing, China has a comparable emission ratio (0.36 ppbv/ppmv) to the U.S. cities, less developed Chinese cities show higher emission ratios (0.44 and 0.55 ppbv/ppmv). If the vehicle CO2 inventories are accurate, NH3 emissions from U.S. vehicles (0.26 ± 0.07 Tg/yr) are more than twice those of the National Emission Inventory (0.12 Tg/yr), while Chinese NH3 vehicle emissions (0.09 ± 0.02 Tg/yr) are similar to a bottom-up inventory. Vehicle NH3 emissions are greater than agricultural emissions in counties containing near half of the U.S. population and require reconsideration in urban air quality models due to their colocation with other aerosol precursors and the uncertainties regarding NH3 losses from upwind agricultural sources. Ammonia emissions in developing cities are especially important because of their high emission ratios and rapid motorizations.

Characterization of Ammonia, Methane, and Nitrous Oxide Emissions from Concentrated Animal Feeding Operations in Northeastern Colorado.

Atmospheric emissions from animal husbandry are important to both air quality and climate, but are hard to characterize and quantify as they differ significantly due to management practices and livestock type, and they can vary substantially throughout diurnal and seasonal cycles. Using a new mobile laboratory, ammonia (NH3), methane (CH4), nitrous oxide (N2O), and other trace gas emissions were measured from four concentrated animal feeding operations (CAFOs) in northeastern Colorado. Two dairies, a beef cattle feedlot, and a sheep feedlot were chosen for repeated diurnal and seasonal measurements. A consistent diurnal pattern in the NH3 to CH4 enhancement ratio is clearly observed, with midday enhancement ratios approximately four times greater than nighttime values. This diurnal pattern is similar, with slight variations in magnitude, at the four CAFOs and across seasons. The average NH3 to CH4 enhancement ratio from all seasons and CAFOs studied is 0.17 (+0.13/-0.08) mol/mol, in agreement with statewide inventory averages and previous literature. Enhancement ratios for NH3 to N2O and N2O to CH4 are also reported. The enhancement ratios can be used as a source signature to distinguish feedlot emissions from other NH3 and CH4 sources, such as fertilizer application and fossil fuel development, and the large diurnal variability is important for refining inventories, models, and emission estimates.

Near-Field Characterization of Methane Emission Variability from a Compressor Station Using a Model Aircraft.

A model aircraft equipped with a custom laser-based, open-path methane sensor was deployed around a natural gas compressor station to quantify the methane leak rate and its variability at a compressor station in the Barnett Shale. The open-path, laser-based sensor provides fast (10 Hz) and precise (0.1 ppmv) measurements of methane in a compact package while the remote control aircraft provides nimble and safe operation around a local source. Emission rates were measured from 22 flights over a one-week period. Mean emission rates of 14 ± 8 g CH4 s(-1) (7.4 ± 4.2 g CH4 s(-1) median) from the station were observed or approximately 0.02% of the station throughput. Significant variability in emission rates (0.3-73 g CH4 s(-1) range) was observed on time scales of hours to days, and plumes showed high spatial variability in the horizontal and vertical dimensions. Given the high spatiotemporal variability of emissions, individual measurements taken over short durations and from ground-based platforms should be used with caution when examining compressor station emissions. More generally, our results demonstrate the unique advantages and challenges of platforms like small unmanned aerial vehicles for quantifying local emission sources to the atmosphere.