Atmospheric ammonia (NH3) has increased dramatically as a consequence of the production of synthetic nitrogen (N) fertilizer and proliferation of intensive livestock systems. It is a chemical of environmental concern as it readily reacts with atmospheric acids to produce fine particulate matter and indirectly contributes to nitrous oxide (N2O) emissions. Here, we present the first tall tower observations of NH3within the U.S. Corn Belt for the period April 2017 through December 2018. Hourly average NH3mixing ratios were measured at 100 and 56 m above the ground surface and fluxes were estimated using a modified gradient approach. The highest NH3mixing ratios (>30 nmol mol−1) occurred during early spring and late fall, coinciding with the timing of fertilizer application within the region and the occurrence of warm air temperatures. Net ecosystem NH3exchange was greatest in spring and fall with peak emissions of about +50 nmol m−2 s−l. Annual NH3emissions estimated using state‐of‐the‐art inventories ranged from 0.6 to 1.4 × the mean annual gross tall tower fluxes (+2.1 nmol m−2 s−1). If the tall tower observations are representative of the Upper Midwest and broader U.S. Corn Belt regions, the annual gross emissions were +720 Gg NH3‐N y−1and +1,340 Gg NH3‐N y−1, respectively. Finally, considering the N2O budget over the same region, we estimated total reactive N emissions (i.e., N2O + NH3) of approximately 1,790 Gg N y−1from the U.S. Corn Belt, representing ~23% of the current annual new N input.
Modeling the sources and transport processes during extreme ammonia episodes in the US Corn Belt
Atmospheric ammonia (NH3) is the primary form of reactive nitrogen (Nr) and a precursor ofammonium (NH4+) aerosols. Ammonia has been linked to adverse impacts on human health, the loss ofecosystem biodiversity, and plays a key role in aerosol radiative forcing. The midwestern United States is themajor NH3source in North America because of dense livestock operations and the high use of syntheticnitrogen fertilizers. Here, we combine tall‐tower (100 m) observations in Minnesota and Weather Researchand Forecasting model coupled with Chemistry (WRF‐Chem) modeling to investigate high and low NH3emission episodes within the U.S. Corn Belt to improve our understanding of the distribution of emissionsources and transport processes. We examined observations and performed model simulations for cases inFebruary through November of 2017 and 2018. The results showed the following: (1) Peak emissions inNovember 2017 were enhanced by above‐normal air temperatures, implying aQ10(i.e., the change in NH3emissions for a temperature increase of 10°C) of 2.5 for emissions. (2) The intensive livestock emissionsrom northern Iowa, approximately 400 km away from the tall tower, accounted for 17.6% of theabundance in tall‐tower NH3mixing ratios. (3) Ammonia mixing ratios in the innermost domain 3frequently (i.e., 336 hr, 48% of November 2017) exceeded 5.3 ppb, an important air quality health standard.(4) In November 2017, simulated NH3net ecosystem exchange (the difference between NH3emissionsand dry deposition) accounted for 60–65% of gross NH3emissions for agricultural areas and was2.8–3.1 times the emissions of forested areas. (5) We estimated a mean annual NH3net ecosystem exchangeof 1.60 ± 0.06 nmol · m−2·s−1for agricultural lands and−0.07 ± 0.02 nmol · m−2·s−1for forested lands.These results imply that future warmer fall temperatures will enhance agricultural NH3emissions, increasethe frequency of dangerous NH3episodes, and enhance dry NH3deposition in adjacent forested lands.
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- Award ID(s):
- 1640337
- NSF-PAR ID:
- 10199413
- Date Published:
- Journal Name:
- Journal of geophysical research
- Volume:
- 125
- ISSN:
- 0148-0227
- Page Range / eLocation ID:
- e2019JD031207
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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Abstract -
BACKGROUND The availability of nitrogen (N) to plants and microbes has a major influence on the structure and function of ecosystems. Because N is an essential component of plant proteins, low N availability constrains the growth of plants and herbivores. To increase N availability, humans apply large amounts of fertilizer to agricultural systems. Losses from these systems, combined with atmospheric deposition of fossil fuel combustion products, introduce copious quantities of reactive N into ecosystems. The negative consequences of these anthropogenic N inputs—such as ecosystem eutrophication and reductions in terrestrial and aquatic biodiversity—are well documented. Yet although N availability is increasing in many locations, reactive N inputs are not evenly distributed globally. Furthermore, experiments and theory also suggest that global change factors such as elevated atmospheric CO 2 , rising temperatures, and altered precipitation and disturbance regimes can reduce the availability of N to plants and microbes in many terrestrial ecosystems. This can occur through increases in biotic demand for N or reductions in its supply to organisms. Reductions in N availability can be observed via several metrics, including lowered nitrogen concentrations ([N]) and isotope ratios (δ 15 N) in plant tissue, reduced rates of N mineralization, and reduced terrestrial N export to aquatic systems. However, a comprehensive synthesis of N availability metrics, outside of experimental settings and capable of revealing large-scale trends, has not yet been carried out. ADVANCES A growing body of observations confirms that N availability is declining in many nonagricultural ecosystems worldwide. Studies have demonstrated declining wood δ 15 N in forests across the continental US, declining foliar [N] in European forests, declining foliar [N] and δ 15 N in North American grasslands, and declining [N] in pollen from the US and southern Canada. This evidence is consistent with observed global-scale declines in foliar δ 15 N and [N] since 1980. Long-term monitoring of soil-based N availability indicators in unmanipulated systems is rare. However, forest studies in the northeast US have demonstrated decades-long decreases in soil N cycling and N exports to air and water, even in the face of elevated atmospheric N deposition. Collectively, these studies suggest a sustained decline in N availability across a range of terrestrial ecosystems, dating at least as far back as the early 20th century. Elevated atmospheric CO 2 levels are likely a main driver of declines in N availability. Terrestrial plants are now uniformly exposed to ~50% more of this essential resource than they were just 150 years ago, and experimentally exposing plants to elevated CO 2 often reduces foliar [N] as well as plant-available soil N. In addition, globally-rising temperatures may raise soil N supply in some systems but may also increase N losses and lead to lower foliar [N]. Changes in other ecosystem drivers—such as local climate patterns, N deposition rates, and disturbance regimes—individually affect smaller areas but may have important cumulative effects on global N availability. OUTLOOK Given the importance of N to ecosystem functioning, a decline in available N is likely to have far-reaching consequences. Reduced N availability likely constrains the response of plants to elevated CO 2 and the ability of ecosystems to sequester carbon. Because herbivore growth and reproduction scale with protein intake, declining foliar [N] may be contributing to widely reported declines in insect populations and may be negatively affecting the growth of grazing livestock and herbivorous wild mammals. Spatial and temporal patterns in N availability are not yet fully understood, particularly outside of Europe and North America. Developments in remote sensing, accompanied by additional historical reconstructions of N availability from tree rings, herbarium specimens, and sediments, will show how N availability trajectories vary among ecosystems. Such assessment and monitoring efforts need to be complemented by further experimental and theoretical investigations into the causes of declining N availability, its implications for global carbon sequestration, and how its effects propagate through food webs. Responses will need to involve reducing N demand via lowering atmospheric CO 2 concentrations, and/or increasing N supply. Successfully mitigating and adapting to declining N availability will require a broader understanding that this phenomenon is occurring alongside the more widely recognized issue of anthropogenic eutrophication. Intercalibration of isotopic records from leaves, tree rings, and lake sediments suggests that N availability in many terrestrial ecosystems has steadily declined since the beginning of the industrial era. Reductions in N availability may affect many aspects of ecosystem functioning, including carbon sequestration and herbivore nutrition. Shaded areas indicate 80% prediction intervals; marker size is proportional to the number of measurements in each annual mean. Isotope data: (tree ring) K. K. McLauchlan et al. , Sci. Rep. 7 , 7856 (2017); (lake sediment) G. W. Holtgrieve et al. , Science 334 , 1545–1548 (2011); (foliar) J. M. Craine et al. , Nat. Ecol. Evol. 2 , 1735–1744 (2018)more » « less
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Abstract Soil drying and wetting cycles can produce pulses of nitric oxide (NO) and nitrous oxide (N2O) emissions with substantial effects on both regional air quality and Earth’s climate. While pulsed production of N emissions is ubiquitous across ecosystems, the processes governing pulse magnitude and timing remain unclear. We studied the processes producing pulsed NO and N2O emissions at two contrasting drylands, desert and chaparral, where despite the hot and dry conditions known to limit biological processes, some of the highest NO and N2O flux rates have been measured. We measured N2O and NO emissions every 30 min for 24 h after wetting soils with isotopically-enriched nitrate and ammonium solutions to determine production pathways and their timing. Nitrate was reduced to N2O within 15 min of wetting, with emissions exceeding 1000 ng N–N2O m−2 s−1and returning to background levels within four hours, but the pulse magnitude did not increase in proportion to the amount of ammonium or nitrate added. In contrast to N2O, NO was emitted over 24 h and increased in proportion to ammonium addition, exceeding 600 ng N–NO m−2 s−1in desert and chaparral soils. Isotope tracers suggest that both ammonia oxidation and nitrate reduction produced NO. Taken together, our measurements demonstrate that nitrate can be reduced within minutes of wetting summer-dry desert soils to produce large N2O emission pulses and that multiple processes contribute to long-lasting NO emissions. These mechanisms represent substantial pathways of ecosystem N loss that also contribute to regional air quality and global climate dynamics.
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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
- Free Publicly Accessible Full Text
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Accepted Manuscript1.0
- Journal Article:
- https://doi.org/doi.org/10.1029/2019JD031207
