modeling atmospheric transport and deposition of ammonia...
TRANSCRIPT
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Modelling atmospheric transport and deposition of ammonia and ammonium
Willem A.H. Asman
Danish Institute of Agricultural Sciences
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Contents• Processes• Model results• Conclusions
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DefinitionsNH3 (ammonia) : gasNH4
+ (ammonium): found in particles
NHx = NH3 (ammonia) + NH4
+ (ammonium)
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Modelling = book keeping
During transport:
dc/dt = emission – deposition +/- reaction
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Emission
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EMISSION-1• No NH4
+ emitted: all NH4+ has once
been NH3.• Many scattered sources with low
emission height. • Partly influenced by meteorological
conditions (that also influence deposition and atmospheric diffusion).
• Many different agricultural systems. Often no information on the distribution of different housing types, manure handling systems etc.->The emission per animal is NOT the same everywhere!
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EMISSION-2For models emission rate needed: • On a regular grid.
• With a temporal (diurnal/seasonal) resolution.
• Preferably: indication of uncertainty.
For administrators:The emission calculations should be set
up in such a way that scenarios for abatement and associated costs can be studied.
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Seasonal variation Netherlands 1990From ratio measured value/ modelled value
with constant emission rate
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EMISSION-3Europe: try to get funding for a project
that will make it possible to generate the NH3 emission rate for use in atmospheric transport models.
It will include :• Spatial distribution of agricultural
systems and soil properties.• Parameterizations for different
agricultural systems.• Dependence on the same meteorology
as used in atmospheric transport model.
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EMISSION-4
Co-dependence of emission, transport and dry deposition on meteorology:
At high wind speed:• Higher NH3 emission rate• NHx deposited further away
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Modelling emission after slurry application(Génermont and Cellier, INRA, France)
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Reaction
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Important types of reactionOne-way reaction:NH3 + H2SO4 in particle -> NH4
+ in particle. No NH3 bound in this way can volatilise.
Two way reaction:NH3 + HNO3 (gas) <-> NH4NO3 containing
particleNH3 + HCl (gas) <-> NH4Cl containing particleNH3 can volatilise again (depending on temp.,
humidity, concentrations).
Remarks: • Reaction with OH radical not so important.• Europe: 10-30% hour-1decrease in NH3 conc.
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Dry deposition NH3
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Dry deposition velocity ammonia• Relatively high; diurnal variation (meteo).• Vegetation: most ammonia not taken up
by stomata, but deposited on wet leaves.• A concentration is present in the surface
(compensation point): flux depends not only on concentration in air, but also on concentration in surface:F = -ve(cair – csurface) csurface important for vegetation (crops), sea (can lead to emission).
• Depends on wind speed/atmospheric stability and wetness surface.
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Models for dry deposition/exchange
ra = aerodynamic resistance
rb = laminar boundary layer resistance
rc = surface resistance
rcut = cuticular resistance
rst = stomatal resistance
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Dry deposition of NH3 is high close to sources, why?
• Concentrations are high, because low source height and plume is not yet diluted.
• Dry deposition velocity of NH3 is relatively high.
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Measured average NH3 conc. vs. downwinddistance east of a poultry farm
(Fowler et al., 1998)
background
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Fraction of emission dry deposited vs. distance
Source height: 3 m ; neutral atmosphere; u(60) = 4.8 m s-1
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Dry deposition ammonia• Once it is vertically diluted (no large
vertical gradient): removal rate is of the order of 1% h-1
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Dry deposition NH4+
(particles)
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Dry deposition velocity ammonium containing particles
• Dry deposition velocity depends on particle size, humidity, wind speed and atmospheric stability
• Mostly not re-emitted after deposition• If no vertical conc. gradient: removal
rate of the order of 0.1% h-1
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Comparison:Dry deposition NH3 vs. NH4
+
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Dry deposition velocity NH3 vs. NH4+
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Dry deposition velocity NH3 vs. NH4+
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Dry deposition velocity NH3 vs. NH4+
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Dry deposition velocity NH3 vs. NH4+
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Effect of limited vertical resolution in model:Fraction emission dry deposited vs. distance
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Dry deposition: additional conclusions• A high vertical resolution is needed to
model dry deposition NH3 close to sources ;or a correction factor.
• The dry deposition velocity of NH4
+ << NH3. • Once NH3 is converted to NH4
+ it can travel over long distances (only removal by precipitation is an efficient mechanism).
• Local NH3 sources can dominate local NHx deposition, but most emitted NH3travels as NH4
+ over long distances!!!
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Vertical concentration profilesNH3 and NH4
+
in area with high emission density
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Area with high
emission density
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Wet deposition of NH3 and NH4
+
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Wet deposition
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Wet deposition (continued)Process Efficiency Importance
(efficiency*conc.)Ammonia• in-cloud sc. +++ +• below-cloud sc. ++ +Ammonium• in-cloud sc. +++ +++• below-cloud sc. + +Notes: • Importance for concentration in precipitation depends on
airborne concentration.• Ammonia conc. is low at cloud-level
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Wet deposition: Conclusions• Cloud and raindrops are acidic.
Therefore all NH3 taken up by them is converted to NH4
+
• Only models can calculate contributions of different processes to the NH4
+ conc. in precipitation• Most NH4
+ in precipitation originatesfrom in-cloud scavenging of NH4
+
containing particles• Removal due to incloud-scavenging is
fast (order: 75% h-1), but it rains only 5-10% of the time in NW Europe
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Model results
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Fate of ammonia emissions (whole lifetime)Width of the arrows is measure of importance
NW Europe 1990; Calculated with TREND model
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Cumulative deposition as a function of downwind distance (NW Europe, 1990)
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Ammonia emission Denmark (kg N ha-1 yr -1)
Sea
Sea
Sea
Germany
Sweden
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NH3 conc.
ground-level
Resolution
5x5 km2
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NH4+ conc.
ground-level
Resolution
5x5 km2
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NHx wet
deposition
Resolution
5x5 km2
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NHx total
deposition
(dry+wet)
Resolution
5x5 km2
In this area
dry dep. ofNH3dominates
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Ammonia emission Denmark (kg N ha-1 yr -1)
Sea
Sea
Sea
Horizontal gradient
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Concentrations and depositions across Denmark
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Modelled vs measured NH3 conc.
Resolution
5x5 km2
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Modelled vs measured NH4+ conc.
Resolution
5x5 km2
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Modelled vs measured NHx wet deposition
Resolution
5x5 km2
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NH3 conc. vs. NH3 emission density (5x5 km2)
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Ratio
dry/ total
deposition
0 .2 .4 .6 .8 1
Close to areas with high emission density:
dry deposition
dominates
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NH3: meas. vs. modelled conc. Netherlands
with different model resolution
5x5 km2 75x75 km2
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NH3: meas. vs. modelled conc. Netherlands
with different model resolution
5x5 km2 150x150 km2
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Ammonia emission (all sources)
-180 -150 -120 -90 -60 -30 0 30 60 90 120 150 180-90
-60
-30
0
30
60
90
-90
-60
-30
0
30
60
90
NH3 emission (g N m-2 yr-1)
0 - 0.050.05 - 0.10.1 - 0.50.5 - 1
1 - 22 - 3
> 3
NH3 emission from all sources
Europe
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Ammonia emission Europe (kg N ha-1 yr -1)
Denmark
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Ammonia emission Denmark (kg N ha-1 yr -1)
Part of Vejle County
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Ammonia emission part of Vejle County
Map made by Bernd Münier
Resolution:
100x100 m2
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Total N deposition part of Vejle county(from all European NH3 and NOx sources)
Map drawn by
Bernd Münier
Transport model runs within GIS
system
Resolution: 100x100 m2
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Purpose atmospheric transport models
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Models can have different purposes• Size of the area to be modelled (local
effect of one farm or distribution of particles over the whole U.S.)
• Time scale: episodes or annual averages.
• Compound to be modelled (e.g. NHxdeposition or fine particle concentration).
All these factors have influence on the spatial and temporal resolution of themodel results and input data needed.
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Is there one model that can describe allsituations?
No. Computers have limited resources(speed, memory).
What to do then?Optimize the model design for the
required purpose:• Adapt to spatial/temporal resolution.• Describe some processes in detail, and
others more generally.
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Conclusions NHx modellingNW Europe
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Conclusions-1NHx mainly deposited as:• Dry deposition of NH3 close to the source.• Wet deposition due to in-cloud
scavenging of NH4+ further away from the
source.
The NH4+ particle conc.
• Originates mainly from distant sources, but not in coastal areas with dominant wind from the sea.
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Conclusions-2Model resolution:Deposition modelling in areas with high
NH3 emission densities:• high spatial resolution (>1x1 km2) is
needed to adequately model the large horizontal gradients.
Deposition modelling in other areas and particle formation modelling:
• High resolution not necessary, but correct modelling of dry dep. of ammonia near source still needed.
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Conclusions-3: Examples of model typesLocal modelling:• High vertical resolution (plume
dilution).• High horizontal resolution.• Limited chemistry.
Regional modelling:• Limited horizontal and vertical
resolution.• Correction factor local NH3 deposition.• More complicated (photo)chemistry.
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End
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Diurnal variation Netherlands
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Dry deposition velocity ammonium containing particles: Sea (continued)
ra = aerodynamic resistance
rb = laminar boundary layer resistance
rvgd = resistance gravitational settling dry particles
rvgw = resistance gravitational settling wet particles
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Link emission <-> conc./depositionNetherlands 1994-1997:• Abatement: estimated 35% emission
reduction• No detectable trend measured ammonia
conc.• 10% reduction in measured ammonium
wet deposition (model estimate:• 29% reduction in measured ammonium
aerosol concentrationWhy?• Maybe influence from parallel trends in
sulphur dioxide and nitrogen oxidesemission
• Maybe abatement not so effective as estimated
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Link between ammonia emission changesand measured conc./depositions
Rothamsted, UK; line = modelled with hist. emission
0
2
4
6
8
10
12
1870 1890 1910 1930 1950 1970 1990
NH
4+ wet
dep
ositi
on (k
g N
ha-1
yr-1
)
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Generation of emission as a function oftime and space:
Use geographical distribution of:• Number of animals, fodder, housing,
storage, application techniques, grazing, use of fertilisers, soil properties, regultations
But:Generate then the emission with a
preprocessor or in the transport model, using process descriptions that are functions of the meteorological conditions
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Why?Because the emission, diffusion and dry
deposition depend on the same meteorological conditions
Result: Higher wind speed-> then more emission which is deposited further away
Disadvantage for policymakers:Emission shows interannual variations already
due to variations in the meteorological conditions (if all other factors are the same)
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Annually average dry NHx deposition vs. distance:as a function of the wind direction
up to a factor of 5 difference!
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Variation of dry deposition with wind speedRatio dry dep. at 2 m s-1/4 m s-1 (rc = 60 s m-1)
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Variation dry deposition with dry deposition velocity vd
ratio dry dep. at vd=0.0254/0.0127 m s-1
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Vertical concentration profilesat two different dry deposition velocities
Distance from source: 200 m
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Variation of dry deposition withsurface resistance rc
ratio dry dep. at various rc vs. at rc = 60 s m-1
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Variation dry deposition with source heightratio dry dep. at 1 m/6 m (rc = 60 s m-1)
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Fraction of emission dry deposited vs. distance
Source height: 3 m ; neutral atmosphere; u(60) = 4.8 m s-1
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Vertical NH3 flux as function of thedistance to a farm with 500 pigs and influence of compensation point
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NH3 flux North Sea found from measuredconcentrations
Emission
Deposition
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Moorland-experiment
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Measured horizontal NH3 gradient
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Modelled horizontal NH3 gradient(with different model options)
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Measured vs. Modelled NH3 conc.
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Vertical NH3 profiles in emission area (--)and nature area (- - -)
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NH3 vs. NOxHow large is the global emission ofammonia compared to that of nitrogenoxides (NO + NO2)?
Compound tonnes N yr-1
Ammonia 53.7×106
Nitrogen oxides 41.8×106
Conclusion:Same order, but a larger fraction of ammonia comes from anthropogenic sources
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Geographical distribution global emission
The scale is the same in all figures!
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Ammonia emission from animal manure
-180 -150 -120 -90 -60 -30 0 30 60 90 120 150 180-90
-60
-30
0
30
60
90
-90
-60
-30
0
30
60
90
NH3 emission (g N m-2 yr-1)
0 - 0.050.05 - 0.10.1 - 0.50.5 - 1
1 - 22 - 3
> 3
NH3 emission from animal waste
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Ammonia emission from fertiliser
-180 -150 -120 -90 -60 -30 0 30 60 90 120 150 180-90
-60
-30
0
30
60
90
-90
-60
-30
0
30
60
90
NH3 emission (g N m-2 yr-1)
0 - 0.050.05 - 0.10.1 - 0.50.5 - 1
1 - 22 - 3
> 3
NH3 emission from synthetic fertilizer use
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Ammonia emission from biomass burning
(deforestation, savanna burning, agr. waste burning)
-180 -150 -120 -90 -60 -30 0 30 60 90 120 150 180-90
-60
-30
0
30
60
90
-90
-60
-30
0
30
60
90
NH3 emission (g N m-2 yr-1)
0 - 0.050.05 - 0.10.1 - 0.50.5 - 1
1 - 22 - 3
> 3
NH3 emission from biomass burning (deforestation, savanna bruning, agr. waste burning)
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Ammonia emission (all sources)
-180 -150 -120 -90 -60 -30 0 30 60 90 120 150 180-90
-60
-30
0
30
60
90
-90
-60
-30
0
30
60
90
NH3 emission (g N m-2 yr-1)
0 - 0.050.05 - 0.10.1 - 0.50.5 - 1
1 - 22 - 3
> 3
NH3 emission from all sources
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C• P
NH3 conc.
(µg NH3 m-3)
0 .2 .5 1 2 5 10 20
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NH4 conc.
(µg NH4 m-3)
0 1 2 3 4 5 6 10
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NHx dry
deposition
(mol ha-1 yr-1)
0 1 2 4 8 16 32 x100
100 mol = 1.4 kg N
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NHx wet
deposition
(mol ha-1 yr-1)
0 1 2 4 8 16 32 x100
100 mol = 1.4 kg N
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NHx total
Deposition
(wet + dry)
(mol ha-1 yr-1)
100 mol = 1.4 kg N
0 1 2 4 8 16 32 x100
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Ratio
dry/ total
deposition
0 .2 .4 .6 .8 1
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NHx deposition
Kattegat sea area
(kg N km-2 yr-1)
DK
S
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NOy deposition
Kattegat sea area
(kg N km-2 yr-1)
DK
S
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C• P
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C• P