Evaluation of interactive and prescribed agricultural ammonia emissions for simulating atmospheric composition in CAM-chem
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Published:2022-02-09
Issue:3
Volume:22
Page:1883-1904
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ISSN:1680-7324
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Container-title:Atmospheric Chemistry and Physics
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language:en
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Short-container-title:Atmos. Chem. Phys.
Author:
Vira JuliusORCID, Hess Peter, Ossohou Money, Galy-Lacaux Corinne
Abstract
Abstract. Ammonia (NH3) plays a central role in the chemistry of inorganic secondary
aerosols in the atmosphere. The largest emission sector for NH3 is agriculture,
where NH3 is volatilized from livestock wastes and fertilized soils. Although
the NH3 volatilization from soils is driven by the soil temperature and moisture,
many atmospheric chemistry models prescribe the emission using yearly emission inventories
and climatological seasonal variations. Here we evaluate an alternative approach where the
NH3 emissions from agriculture are simulated interactively using the process model
FANv2 (Flow of Agricultural Nitrogen, version 2) coupled to the Community Atmospheric
Model with Chemistry (CAM-chem). We run a set of 6-year global simulations using
the NH3 emission from FANv2 and three global emission inventories (EDGAR, CEDS and
HTAP) and evaluate the model performance using a global set of multi-component
(atmospheric NH3 and NH4+, and NH4+ wet deposition) in situ
observations. Over East Asia, Europe and North America, the simulations with different
emissions perform similarly when compared with the observed geographical patterns. The
seasonal distributions of NH3 emissions differ between the inventories, and the
comparison to observations suggests that both FANv2 and the inventories would benefit from
more realistic timing of fertilizer applications. The largest differences between the
simulations occur over data-scarce regions. In Africa, the emissions simulated by FANv2
are 200 %–300 % higher than in the inventories, and the available in situ observations
from western and central Africa, as well as NH3 retrievals from the Infrared Atmospheric Sounding Interferometer (IASI)
instrument, are consistent with the higher NH3 emissions as simulated by
FANv2. Overall, in simulating ammonia and ammonium concentrations over regions with
detailed regional emission inventories, the inventories based on these details (HTAP,
CEDS) capture the atmospheric concentrations and their seasonal variability the
best. However these inventories cannot capture the impact of meteorological variability
on the emissions, nor can these inventories couple the emissions to the biogeochemical
cycles and their changes with climate drivers. Finally, we show with sensitivity
experiments that the simulated time-averaged nitrate concentration in air is sensitive to
the temporal resolution of the NH3 emissions. Over the CASTNET monitoring network
covering the US, resolving the NH3 emissions hourly instead monthly reduced the
positive model bias from approximately 80 % to 60 % of the observed yearly mean nitrate
concentration. This suggests that some of the commonly reported overestimation of aerosol
nitrate over the US may be related to unresolved temporal variability in the NH3
emissions.
Funder
National Center for Atmospheric Research Biological and Environmental Research Strategic Research Council Academy of Finland
Publisher
Copernicus GmbH
Subject
Atmospheric Science
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