We investigate regional sources contributing to CO during the Korea United States Air Quality (KORUS‐AQ) campaign conducted over Korea (1 May to 10 June 2016) using 17 tagged CO simulations from the ...Community Atmosphere Model with chemistry (CAM‐chem). The simulations use three spatial resolutions, three anthropogenic emission inventories, two meteorological fields, and nine emission scenarios. These simulations are evaluated against measurements from the DC‐8 aircraft and Measurements Of Pollution In The Troposphere (MOPITT). Results show that simulations using bottom‐up emissions are consistently lower (bias: −34 to −39%) and poorer performing (Taylor skill: 0.38–0.61) than simulations using alternative anthropogenic emissions (bias: −6 to −33%; Taylor skill: 0.48–0.86), particularly for enhanced Asian CO and volatile organic compound (VOC) emission scenarios, suggesting underestimation in modeled CO background and emissions in the region. The ranges of source contributions to modeled CO along DC‐8 aircraft from Korea and southern (90°E to 123°E, 20°N to 29°N), middle (90°E to 123°E, 29°N to 38.5°N), and northern (90°E to 131.5°E, 38.5°N to 45°N) East Asia (EA) are 6–13%, ~5%, 16–28%, and 9–18%, respectively. CO emissions from middle and northern EA can reach Korea via transport within the boundary layer, whereas those from southern EA are transported to Korea mainly through the free troposphere. Emission contributions from middle EA dominate during continental outflow events (29–51%), while Korean emissions play an overall more important role for ground sites (up to 25–49%) and plumes within the boundary layer (up to 25–44%) in Korea. Finally, comparisons with four other source contribution approaches (FLEXPART 9.1 back trajectory calculations driven by Weather Research and Forecasting (WRF) WRF inert tracer, China signature VOCs, and CO to CO2 enhancement ratios) show general consistency with CAM‐chem.
Key Points
Korean sources contribute 6‐13% to CO along DC‐8 flight tracks, while contributions of different East Asian subregions vary from 5% to 28%
Middle East Asian sources dominate (up to 64%) continental outflows to Korea, but Korean emissions are more important for CO near surface
Contributions using CAM‐chem tags agree with FLEXPART‐WRF back trajectories, WRF NO2 inert tracers, China signature VOCs, and CO/CO2
We report on measurements of acyl peroxy nitrates (APNs) obtained from two ground sites and the NSF/National Center for Atmospheric Research C‐130 aircraft during the 2014 Front Range Air Pollution ...and Photochemistry Éxperiment (FRAPPÉ). The relative abundance of the APNs observed at the Boulder Atmospheric Observatory (BAO) indicates that anthropogenic emissions of volatile organic compounds (VOCs) are the dominant drivers of photochemistry during days with the most elevated peroxyacetyl nitrate (PAN). Reduced major axis regression between propionyl peroxynitrate (PPN) and PAN observed at BAO and from the C‐130 produced a slope of 0.21 (R2 = 0.92). Periods of lower PPN/PAN ratios (~0.10) were associated with cleaner background air characterized by lower ammonia and formic acid abundances. The abundance of methacryloyl peroxynitrate relative to PAN only exceeded 0.05 at BAO when PAN mixing ratios were <300 parts per trillion by volume, implying low influence of isoprene oxidation during periods with substantial local PAN production. We show an example of a day (19 July) where high O3 was not accompanied by enhanced local PAN production. The contribution of biogenic VOCs to local O3 production on the other days in July with elevated O3 (22, 23, 28, and 29 July 2014) was small; evidence is provided in the high abundance of PPN to PAN (slopes between 0.18 and 0.26). The PAN chemistry observed from surface and aircraft platforms during FRAPPÉ implies that anthropogenic VOCs played a dominant role in PAN production during periods with the most O3 and that the relative importance of biogenic hydrocarbon chemistry decreased with increasing O3 production during FRAPPÉ.
Key Points
PPN/PAN ratios are high (>0.15) when PAN is elevated in the Front Range, and MPAN abundances are small compared to other U.S. regions
Anthropogenic VOC precursors dominate PAN production when ozone was most elevated in the Colorado Front Range in summer 2014
Similar maximum PAN mixing ratios were observed at Rocky Mountain National Park and in the Front Range during summer 2014
The U.S. National Aeronautics and Space Administration in partnership with Korea’s National Institute of Environmental Research embarked on the Korea-United States Air Quality (KORUS-AQ) study to ...address air quality issues over the Korean peninsula. Underestimation of volatile organic compound (VOC) emissions from various large facilities on South Korea’s northwest coast may contribute to this problem, and this study focuses on quantifying top-down emissions of formaldehyde (CH2O) and VOCs from the largest of these facilities, the Daesan petrochemical complex, and comparisons with the latest emission inventories. To accomplish this and additional goals discussed herein, this study employed a number of measurements acquired during KORUS-AQ onboard the NASA DC-8 aircraft during three Daesan overflights on June 2, 3, and 5, 2016, in conjunction with a mass balance approach. The measurements included fast airborne measurements of CH2O and ethane from an infrared spectrometer, additional fast measurements from other instruments, and a suite of 33 VOC measurements acquired by the whole air sampler. The mass balance approach resulted in consistent top-down yearly Daesan VOC emission flux estimates, which averaged (61 ± 14) × 103 MT/year for the 33 VOC compounds, a factor of 2.9 ± 0.6 (±1.0) higher than the bottom-up inventory value. The top-down Daesan emission estimate for CH2O and its four primary precursors averaged a factor of 4.3 ± 1.5 (± 1.9) times higher than the bottom-up inventory value. The uncertainty values in parentheses reflect upper limits for total uncertainty estimates. The resulting averaged top-down Daesan emission estimate for sulfur dioxide (SO2) yielded a ratio of 0.81–1.0 times the bottom-up SO2 inventory, and this provides an important cross-check on the accuracy of our mass balance analysis.
Forest and vegetation fires, used as tools for agriculture and deforestation, are a major source of air pollutants and can cause serious air quality issues in many parts of Asia. Actions to reduce ...fire may offer considerable, yet largely unrecognised, options for rapid improvements in air quality. In this study, we used a combination of regional and global air quality models and observations to examine the impact of forest and vegetation fires on air quality degradation and public health in Southeast Asia (including Mainland Southeast Asia and south-eastern China). We found that eliminating fire could substantially improve regional air quality across Southeast Asia by reducing the population exposure to fine particulate matter (PM2.5) concentrations by 7% and surface ozone concentrations by 5%. These reductions in PM2.5 exposures would yield a considerable public health benefit across the region; averting 59,000 (95% uncertainty interval (95UI): 55,200-62,900) premature deaths annually. Analysis of subnational infant mortality rate data and PM2.5 exposure suggested that PM2.5 from fires disproportionately impacts poorer populations across Southeast Asia. We identified two key regions in northern Laos and western Myanmar where particularly high levels of poverty coincide with exposure to relatively high levels of PM2.5 from fires. Our results show that reducing forest and vegetation fires should be a public health priority for the Southeast Asia region.
Atmospheric nitrous oxide (N2O) is, after carbon dioxide and methane, the third most important long-lived anthropogenic greenhouse gas in terms of radiative forcing. Since preindustrial times a ...rising trend in the global N2O concentrations is observed. Anthropogenic emissions of N2O, mainly from agricultural activity, contribute considerably to this trend. Sparse observational constraints have made it difficult to quantify these emissions. The few studies on top-down approaches in the U.S. that exist are mainly based on Lagrangian models and ground-based measurements. They all propose a significant underestimation of anthropogenic N2O emission sources in established inventories, such as the Emissions Database for Global Atmospheric Research (EDGAR). In this study we quantify anthropogenic N2O emissions in the Midwest of the U.S., an area of high agricultural activity. In the course of the Atmospheric Carbon and Transport – America (ACT-America) campaign spanning from summer 2016 to summer 2019, an extensive dataset over four seasons has been collected including in-situ N2O aircraft based measurements in the lower and middle troposphere onboard NASA’s C-130 and B-200 aircraft. During fall 2017 and summer 2019 we conducted measurements onboard the NASA-C130 with a Quantum-Cascade-Laser-Spectrometer (QCLS) and on both aircraft over the whole campaign flask measurements (NOAA) were collected. More than 300 joint flight hours were conducted and more than 500 flask samples were collected over the U.S. Midwest. The QCLS system collected continuous N2O data for approximately 60 flight hours in this region. The Eulerian Weather Research and Forecasting model with chemistry enabled (WRF-Chem) is being used to quantify regional agricultural N2O emissions using the spatial characteristics of these atmospheric N2O mole fraction observations. The numerical simulations enable potential surface emission distributions to be compared to our airborne measurements, and source estimates can be adjusted to minimize the differences, thus quantifying N2O sources. These results are then compared to emission rates in the EDGAR inventory.
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