Abstract. This study characterizes the impact of the Chesapeake Bay and associated meteorological phenomena on aerosol chemistry during the second Ozone Water-Land Environmental Transition Study (OWLETS-2) field campaign, which took place from 4 June to 5 July 2018. Measurements of inorganic PM2.5 composition, gas-phase ammonia (NH3), and an array of meteorological parameters were undertaken at Hart-Miller Island (HMI), a land–water transition site just east of downtown Baltimore on the Chesapeake Bay. The observations at HMI were characterized by abnormally high NH3 concentrations (maximum of 19.3 µg m−3, average of 3.83 µg m−3), which were more than a factor of 3 higher than NH3 levels measured at the closest atmospheric Ammonia Monitoring Network (AMoN) site (approximately 45 km away). While sulfate concentrations at HMI agreed quite well with those measured at a regulatory monitoring station 45 km away, aerosol ammonium and nitrate concentrations were significantly higher, due to the ammonia-rich conditions that resulted from the elevated NH3. The high NH3 concentrations were largely due to regional agricultural emissions, including dairy farms in southeastern Pennsylvania and poultry operations in the Delmarva Peninsula (Delaware–Maryland–Virginia). Reduced NH3 deposition during transport over the Chesapeake Bay likely contributed to enhanced concentrations at HMI compared to the more inland AMoN site. Several peak NH3 events were recorded, including the maximum NH3 observed during OWLETS-2, that appear to originate from a cluster of industrial sources near downtown Baltimore. Such events were all associated with nighttime emissions and advection to HMI under low wind speeds (< 1 m s−1) and stable atmospheric conditions. Our results demonstrate the importance of industrial sources, including several that are not represented in the emissions inventory, on urban air quality. Together with our companion paper, which examines aerosol liquid water and pH during OWLETS-2, we highlight unique processes affecting urban air quality of coastal cities that are distinct from continental locations.
more »
« less
Diverging trends in aerosol sulfate and nitrate measured in the remote North Atlantic in Barbados are attributed to clean air policies, African smoke, and anthropogenic emissions
Abstract. Sulfate and nitrate aerosols degrade air quality, modulate radiative forcing and the hydrological cycle, and affect biogeochemical cycles, yet their global cycles are poorly understood. Here, we examined trends in 21 years of aerosol measurements made at Ragged Point, Barbados, the easternmost promontory on the island located in the eastern Caribbean Basin. Though the site has historically been used to characterize African dust transport, here we focused on changes in nitrate and non-sea-salt (nss) sulfate aerosols from 1990–2011. Nitrate aerosol concentrations averaged over the entire period were stable at 0.59 µg m−3 ± 0.04 µg m−3, except for elevated nitrate concentrations in the spring of 2010 and during the summer and fall of 2008 due to the transport of biomass burning emissions from both northern and southern Africa to our site. In contrast, from 1990 to 2000, nss-sulfate decreased 30 % at a rate of 0.023 µg m−3 yr−1, a trend which we attribute to air quality policies enacted in the United States (US) and Europe. From 2000–2011, sulfate gradually increased at a rate of 0.021 µg m−3 yr−1 to pre-1990s levels of 0.90 µg m−3. We used the Community Multiscale Air Quality (CMAQ) model simulations from the EPA's Air QUAlity TimE Series (EQUATES) to better understand the changes in nss-sulfate after 2000. The model simulations estimate that increases in anthropogenic emissions from Africa explain the increase in nss-sulfate observed in Barbados. Our results highlight the need to better constrain emissions from developing countries and to assess their impact on aerosol burdens in remote source regions.
more »
« less
- Award ID(s):
- 2215875
- PAR ID:
- 10534521
- Publisher / Repository:
- Atmospheric Chemistry and Physics
- Date Published:
- Journal Name:
- Atmospheric Chemistry and Physics
- Volume:
- 24
- Issue:
- 13
- ISSN:
- 1680-7324
- Page Range / eLocation ID:
- 8049 to 8066
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
More Like this
-
-
Abstract. Limited data availability and distinct regional characteristics of sources lead to a wide range of future aerosol emission projections for Africa. Here, we quantify and explore the implications of this spread for climate and health impact assessments. Using the Evaluating the Climate and Air Quality Impacts of Short-Lived Pollutants (ECLIPSE), the Shared Socioeconomic Pathways (SSPs), and the United Nations Environment Programme (UNEP) emission projections, we find high scenario diversity and regional heterogeneity in projected air pollution emissions across Africa. Baseline emissions also vary in their sectoral split. Using 10 different emission pathways as input to the Oslo chemical transport model version 3 (OsloCTM3), we find that regionally averaged annual mean population-weighted fine particulate matter (PM2.5) concentrations exhibit divergent trends depending on scenario stringency, with the eastern Africa PM2.5 concentrations increasing by up to 6 µg m−3 (37 %, SD ± 2.7 µg m−3) by 2050 under the UNEP Baseline, SSP370, and ECLIPSE current legislation scenarios. In almost all cases, excess deaths increase substantially, with increases of up to more than 2.5 times compared to the baseline. We also find a net positive aerosol-induced radiative forcing across Africa in all scenarios by 2050, except two high-sulfur emission UNEP scenarios, with values ranging from 0.03 W m−2 in SSP119 to 0.27 W m−2 in SSP585. The wide spread in projected emissions and differences in sectoral distributions across scenarios highlight the critical need for accurate activity data and harmonization efforts in preparation for upcoming assessments such as the 7th Assessment Report of the Intergovernmental Panel on Climate Change.more » « less
-
null (Ed.)This study characterizes the impact of the Chesapeake Bay and associated meteorological phenomena on aerosol chemistry during the second Ozone Water-Land Environmental Transition Study (OWLETS-2) field campaign during summer 2018. Measurements of inorganic PM2.5 composition, gas-phase ammonia (NH3), and an array of meteorological parameters were undertaken at Hart-Miller Island (HMI), a land-water transition site just east of downtown Baltimore on the Chesapeake Bay. The observations at HMI were characterized by abnormally high NH3 concentrations (maximum of 19.3 μg m-3, average of 3.83 μg m-3), which were more than a factor of three higher than NH3 levels measured at the closest Atmospheric Ammonia Network (AMoN) site (approximately 45 km away). While sulfate concentrations at HMI agreed quite well with those measured at a regulatory monitoring station 45 km away, aerosol ammonium and nitrate concentrations were significantly higher, due to the ammonia-rich conditions that resulted from the elevated NH3. The high NH3 concentrations were largely due to regional agricultural emissions, including dairy farms in southeastern Pennsylvania and poultry operations in the Delmarva Peninsula (Delaware-Maryland-Virginia). Reduced NH3 deposition during transport over the Chesapeake Bay likely contributed to enhanced concentrations at HMI compared to the more inland AMoN site. Several peak NH3 events were recorded, including the maximum NH3 observed during OWLETS-2, that appear to originate from a cluster of industrial sources near downtown Baltimore. Such events were all associated with nighttime emissions and advection to HMI under low 15 wind speeds (< 1 m s-1) and stable atmospheric conditions. Our results demonstrate the importance of industrial sources, including several that are not represented in the emissions inventory, on urban air quality. Together with our companion paper, which examines aerosol liquid water and pH during OWLETS-2, we highlight unique processes affecting urban air quality of coastal cities that are distinct from continental locations.more » « less
-
Abstract. Our work explores the impact of two important dimensions of landsystem changes, land use and land cover change (LULCC) as well as directagricultural reactive nitrogen (Nr) emissions from soils, on ozone(O3) and fine particulate matter (PM2.5) in terms of air quality overcontemporary (1992 to 2014) timescales. We account for LULCC andagricultural Nr emissions changes with consistent remote sensingproducts and new global emission inventories respectively estimating theirimpacts on global surface O3 and PM2.5 concentrations as well as Nrdeposition using the GEOS-Chem global chemical transport model. Over thistime period, our model results show that agricultural Nr emissionchanges cause a reduction of annual mean PM2.5 levels over Europe andnorthern Asia (up to −2.1 µg m−3) while increasing PM2.5 levels in India, China and the eastern US (up to +3.5 µg m−3). Land cover changes induce small reductions in PM2.5 (up to −0.7 µg m−3) over Amazonia, China and India due to reduced biogenic volatile organic compound (BVOC) emissions and enhanced deposition of aerosol precursor gases (e.g., NO2, SO2). Agricultural Nr emissionchanges only lead to minor changes (up to ±0.6 ppbv) in annual meansurface O3 levels, mainly over China, India and Myanmar. Meanwhile, ourmodel result suggests a stronger impact of LULCC on surface O3 over the time period across South America; the combination of changes in drydeposition and isoprene emissions results in −0.8 to +1.2 ppbv surfaceozone changes. The enhancement of dry deposition reduces the surface ozone level (up to −1 ppbv) over southern China, the eastern US and central Africa. The enhancement of soil NO emission due to crop expansion also contributes to surface ozone changes (up to +0.6 ppbv) over sub-Saharan Africa. Incertain regions, the combined effects of LULCC and agricultural Nr emission changes on O3 and PM2.5 air quality can be comparable (>20 %) to anthropogenic emission changes over the same time period. Finally, we calculate that the increase in global agricultural Nr emissions leads to a net increase in global land area (+3.67×106km2) that potentially faces exceedance of the critical Nr load (>5 kg N ha−1 yr−1). Our result demonstrates the impacts of contemporary LULCC and agricultural Nr emission changes on PM2.5 and O3 in terms of air quality, as well as the importanceof land system changes for air quality over multidecadal timescales.more » « less
-
Anthropogenic sulfate aerosols are estimated to have offset sixty percent of greenhouse-gas-induced warming in the Arctic, a region warming four times faster than the rest of the world. However, sulfate radiative forcing estimates remain uncertain because the relative contributions from anthropogenic versus natural sources to total sulfate aerosols are unknown. Here we measure sulfur isotopes of sulfate in a Summit, Greenland ice core from 1850 to 2006 CE to quantify the contribution of anthropogenic sulfur emissions to ice core sulfate. We use a Keeling Plot to determine the anthropogenic sulfur isotopic signature (δ34Santhro = +2.9 ± 0.3 ‰), and compare this result to a compilation of sulfur isotope measurements of oil and coal. Using δ34Santhro, we quantify anthropogenic sulfate concentration separated from natural sulfate. Anthropogenic sulfate concentration increases to 68 ± 7% of non-sea-salt sulfate (65.1 ± 20.2 µg kg-1) during peak anthropogenic emissions from 1960 to 1990 and decreases to 45 ± 11% of non-sea-salt sulfate (25.4 ± 12.8 µg kg-1) from 1996 to 2006. These observations provide the first long-term record of anthropogenic sulfate distinguished from natural sources (e.g., volcanoes, dimethyl sulfide), and can be used to evaluate model characterization of anthropogenic sulfate aerosol fraction and radiative forcing over the industrial era.more » « less
An official website of the United States government

