1.
Emissions
1.1 Anthropogenic Emissions
The
major driver of the LOTOS-EUROS system is the anthropogenic emission data of
VOC, SOx, NOx, NH3, CO, CH4 and PM.
In the framework of UBA-project FKZ 202 43270, a European-wide emission data
base for the year 2000 has been made on grids of 0.25 x 0.125 latlong, about 15
x 15 km2. The emission sectoral totals have been scaled to conform to the
latest country submissions to EMEP for the year 2000, whenever available ( Visschedijk
and Denier van der Gon, 2005). The database contains a separation between area
and point source information. This database for point sources has been set up
already in the 80s and has been updated since, using various sources of
information such as national authorities, contacts with (local) experts,
industrial interest organisations, various proprietary data bases etc. PM
emissions for 2000 are assumed to be the same as those in the CEPMEIP project
(derived for 1995). The reasoning is that the uncertainty in the emission
estimate is much larger than the trend in the PM emissions. The CEPMEIP
database does not specify the composition of the emitted particles. Therefore,
black carbon emissions were derived from the primary PM2.5 emissions. The BC
emissions are calculated in the model from the estimated BC-fractions per
country and source category (Schaap et al., 2004b). We assume 2% of the SO2
emissions to be emitted as particulate sulphate.
1.1.1 Time- and temperature factors
The basic information, which
is also the input data for the chemistry-transport-model (LOTOS-EUROS), is the
gridded yearly averaged anthropogenic emission database. However in reality
emissions of specific source categories, as for example road transport,
fluctuate in time and/or with temperature. The time and temperature factors
that are in use LOTOS-EUROS are the result of a critical review of these
factors within the TROTREP project (Builtjes et al., 2003). The factors used
are specified in the tables below.
Table 8.1 Monthly emissions factors for the SNAP level 1 categories.
|
category |
jan |
feb |
mar |
apr |
may |
jun |
jul |
aug |
sep |
oct |
nov |
dec |
|
|
1 |
Power generation |
1.20 |
1.15 |
1.05 |
1.00 |
0.90 |
0.85 |
0.80 |
0.87 |
0.95 |
1.00 |
1.08 |
1.15 |
|
2 |
Residential,
commercial and other combustion |
1.70 |
1.50 |
1.30 |
1.00 |
0.70 |
0.40 |
0.20 |
0.40 |
0.70 |
1.05 |
1.40 |
1.65 |
|
3 |
Industrial
combustion |
1.10 |
1.08 |
1.05 |
1.00 |
0.95 |
0.90 |
0.93 |
0.95 |
0.97 |
1.00 |
1.02 |
1.05 |
|
4 |
Industrial processes |
1.02 |
1.02 |
1.02 |
1.02 |
1.02 |
1.02 |
1.00 |
0.84 |
1.02 |
1.02 |
1.02 |
0.90 |
|
5 |
Extraction
distribution of fossil fuels |
1.20 |
1.20 |
1.20 |
0.80 |
0.80 |
0.80 |
0.80 |
0.80 |
0.80 |
1.20 |
1.20 |
1.20 |
|
6 |
Solvent use |
0.95 |
0.96 |
1.02 |
1.00 |
1.01 |
1.03 |
1.03 |
1.01 |
1.04 |
1.03 |
1.01 |
0.91 |
|
7a |
Road transport
gasoline |
0.88 |
0.92 |
0.98 |
1.03 |
1.05 |
1.06 |
1.01 |
1.02 |
1.06 |
1.05 |
1.01 |
0.93 |
|
7b |
Road transport
diesel |
0.88 |
0.92 |
0.98 |
1.03 |
1.05 |
1.06 |
1.01 |
1.02 |
1.06 |
1.05 |
1.01 |
0.93 |
|
7c |
Road transport
evaporation |
0.88 |
0.92 |
0.98 |
1.03 |
1.05 |
1.06 |
1.01 |
1.02 |
1.06 |
1.05 |
1.01 |
0.93 |
|
8 |
Other mobile sources
and machinery |
0.88 |
0.92 |
0.98 |
1.03 |
1.05 |
1.06 |
1.01 |
1.02 |
1.06 |
1.05 |
1.01 |
0.93 |
|
9 |
Waste treatment and
disposal |
1.00 |
1.00 |
1.00 |
1.00 |
1.00 |
1.00 |
1.00 |
1.00 |
1.00 |
1.00 |
1.00 |
1.00 |
|
10 |
Agriculture |
0.45 |
1.30 |
2.35 |
1.70 |
0.85 |
0.85 |
0.85 |
1.00 |
1.10 |
0.65 |
0.45 |
0.45 |
Table 8.2 Emission
factors for the day of the week for the SNAP level 1 categories.
|
category |
Mon |
Tue |
Wed |
Thu |
Fri |
Sat |
Sun |
|
|
1 |
Power generation |
1.06 |
1.06 |
1.06 |
1.06 |
1.06 |
0.85 |
0.85 |
|
2 |
Residential, commercial and other combustion |
1.08 |
1.08 |
1.08 |
1.08 |
1.08 |
0.8 |
0.8 |
|
3 |
Industrial combustion |
1.08 |
1.08 |
1.08 |
1.08 |
1.08 |
0.8 |
0.8 |
|
4 |
Industrial processes |
1.02 |
1.02 |
1.02 |
1.02 |
1.02 |
1.02 |
1 |
|
5 |
Extraction distribution of fossil fuels |
1 |
1 |
1 |
1 |
1 |
1 |
1 |
|
6 |
Solvent use |
1.2 |
1.2 |
1.2 |
1.2 |
1.2 |
0.5 |
0.5 |
|
7a |
Road transport gasoline |
1.02 |
1.06 |
1.08 |
1.1 |
1.14 |
0.81 |
0.79 |
|
7b |
Road transport diesel |
1.02 |
1.06 |
1.08 |
1.1 |
1.14 |
0.81 |
0.79 |
|
7c |
Road transport evaporation |
1.02 |
1.06 |
1.08 |
1.1 |
1.14 |
0.81 |
0.79 |
|
8 |
Other mobile sources and machinery |
1 |
1 |
1 |
1 |
1 |
1 |
1 |
|
9 |
Waste treatment and disposal |
1 |
1 |
1 |
1 |
1 |
1 |
1 |
|
10 |
Agriculture |
1 |
1 |
1 |
1 |
1 |
1 |
1 |
Table 8.3 Emission
factors for the hour of day (
|
|
Hour of day |
||||||||||||
|
category |
1 |
2 |
3 |
4 |
5 |
6 |
7 |
8 |
9 |
10 |
11 |
12 |
|
|
1 |
Power generation |
0.79 |
0.72 |
0.72 |
0.71 |
0.74 |
0.80 |
0.92 |
1.08 |
1.19 |
1.22 |
1.21 |
1.21 |
|
2 |
Residential,
commercial and other combustion |
0.38 |
0.36 |
0.36 |
0.36 |
0.37 |
0.50 |
1.19 |
1.53 |
1.57 |
1.56 |
1.35 |
1.16 |
|
3 |
Industrial
combustion |
0.75 |
0.75 |
0.78 |
0.82 |
0.88 |
0.95 |
1.02 |
1.09 |
1.16 |
1.22 |
1.28 |
1.30 |
|
4 |
Industrial processes |
1.00 |
1.00 |
1.00 |
1.00 |
1.00 |
1.00 |
1.00 |
1.00 |
1.00 |
1.00 |
1.00 |
1.00 |
|
5 |
Extraction
distribution of fossil fuels |
1.00 |
1.00 |
1.00 |
1.00 |
1.00 |
1.00 |
1.00 |
1.00 |
1.00 |
1.00 |
1.00 |
1.00 |
|
6 |
Solvent use |
0.50 |
0.35 |
0.20 |
0.10 |
0.10 |
0.20 |
0.75 |
1.25 |
1.40 |
1.50 |
1.50 |
1.50 |
|
7a |
Road transport
gasoline |
0.19 |
0.09 |
0.06 |
0.05 |
0.09 |
0.22 |
0.86 |
1.84 |
1.86 |
1.41 |
1.24 |
1.20 |
|
7b |
Road transport
diesel |
0.19 |
0.09 |
0.06 |
0.05 |
0.09 |
0.22 |
0.86 |
1.84 |
1.86 |
1.41 |
1.24 |
1.20 |
|
7c |
Road transport
evaporation |
0.19 |
0.09 |
0.06 |
0.05 |
0.09 |
0.22 |
0.86 |
1.84 |
1.86 |
1.41 |
1.24 |
1.20 |
|
8 |
Other mobile sources
and machinery |
0.19 |
0.09 |
0.06 |
0.05 |
0.09 |
0.22 |
0.86 |
1.84 |
1.86 |
1.41 |
1.24 |
1.20 |
|
9 |
Waste treatment and
disposal |
1.00 |
1.00 |
1.00 |
1.00 |
1.00 |
1.00 |
1.00 |
1.00 |
1.00 |
1.00 |
1.00 |
1.00 |
|
10 |
Agriculture |
1.00 |
1.00 |
1.00 |
1.00 |
1.00 |
1.00 |
1.00 |
1.00 |
1.00 |
1.00 |
1.00 |
1.00 |
Table 8.4 Emission
factors for the hour of day (
|
|
Hour of day |
||||||||||||
|
category |
13 |
14 |
15 |
16 |
17 |
18 |
19 |
20 |
21 |
22 |
23 |
24 |
|
|
1 |
Power generation |
1.17 |
1.15 |
1.14 |
1.13 |
1.10 |
1.07 |
1.04 |
1.02 |
1.02 |
1.01 |
0.96 |
0.88 |
|
2 |
Residential,
commercial and other combustion |
1.07 |
1.06 |
1.00 |
0.98 |
0.99 |
1.12 |
1.41 |
1.52 |
1.39 |
1.35 |
1.00 |
0.42 |
|
3 |
Industrial
combustion |
1.22 |
1.24 |
1.25 |
1.16 |
1.08 |
1.01 |
0.95 |
0.90 |
0.85 |
0.81 |
0.78 |
0.75 |
|
4 |
Industrial processes |
1.00 |
1.00 |
1.00 |
1.00 |
1.00 |
1.00 |
1.00 |
1.00 |
1.00 |
1.00 |
1.00 |
1.00 |
|
5 |
Extraction
distribution of fossil fuels |
1.00 |
1.00 |
1.00 |
1.00 |
1.00 |
1.00 |
1.00 |
1.00 |
1.00 |
1.00 |
1.00 |
1.00 |
|
6 |
Solvent use |
1.50 |
1.50 |
1.50 |
1.50 |
1.50 |
1.40 |
1.25 |
1.10 |
1.00 |
0.90 |
0.80 |
0.70 |
|
7a |
Road transport
gasoline |
1.32 |
1.44 |
1.45 |
1.59 |
2.03 |
2.08 |
1.51 |
1.06 |
0.74 |
0.62 |
0.61 |
0.44 |
|
7b |
Road transport
diesel |
1.32 |
1.44 |
1.45 |
1.59 |
2.03 |
2.08 |
1.51 |
1.06 |
0.74 |
0.62 |
0.61 |
0.44 |
|
7c |
Road transport
evaporation |
1.32 |
1.44 |
1.45 |
1.59 |
2.03 |
2.08 |
1.51 |
1.06 |
0.74 |
0.62 |
0.61 |
0.44 |
|
8 |
Other mobile sources
and machinery |
1.32 |
1.44 |
1.45 |
1.59 |
2.03 |
2.08 |
1.51 |
1.06 |
0.74 |
0.62 |
0.61 |
0.44 |
|
9 |
Waste treatment and
disposal |
1.00 |
1.00 |
1.00 |
1.00 |
1.00 |
1.00 |
1.00 |
1.00 |
1.00 |
1.00 |
1.00 |
1.00 |
|
10 |
Agriculture |
1.00 |
1.00 |
1.00 |
1.00 |
1.00 |
1.00 |
1.00 |
1.00 |
1.00 |
1.00 |
1.00 |
1.00 |
The hour of day is local
time, hence information over the deviation from GMT is needed for each country.
The following time-zones are incorporated:
GMT+0
GMT+1 all
other European countries except those listed with GMT+2:
GMT+2 for
GMT+3 Azerbaidjan,
Currently it is assumed that
all countries have the shift from summer to wintertime and vice versa at the
same days, i.e. the last Sunday of October and March, respectively.
In addition to the time
factors specified above in Table
8.1 to 8.4, a t
Figure 8.1 Temperature factors to be applied for VOC and CO from road transport category (71 and 72: gasoline and diesel).
The higher emissions for VOC and CO at lower temperatures are due to the so-called “cold start”.
1.1.2 NMVOC-speciation
CBM-IV uses nine primary organic species (i.e., species emitted directly to the atmosphere as opposed to secondary organic species formed by chemical reaction in the atmosphere). Most of the organic species in the mechanism represent carbon-carbon bond types, but ethene (ETH), isoprene (ISOP) and formaldehyde (FORM) are represented explicitly. CB99 includes two additional primary organic species, methanol (MEOH) and ethanol (ETOH). The carbon-bond types include carbon atoms that contain only single bonds (PAR), double-bonded carbon atoms (OLE), 7-carbon ring structures represented by toluene (TOL), 8-carbon ring structures represented by xylene (XYL), the carbonyl group with adjacent carbon atom and higher molecular weight aldehydes represented by acetaldehyde (ALD2), and non-reactive carbon atoms (NR).
Many organic compounds are apportioned to the carbon-bond species based simply on the basis of molecular structure. For example, propane is represented by three PARs since all three carbon atoms have only single bonds, and propene is represented as one OLE (for the one carbon-carbon double bond) and one PAR (for the carbon atom with all single bonds). Some apportionments are based on reactivity considerations, however. For example, olefins with internal double bonds are represented as ALD2s and PARs rather than OLEs and PARs. Further, the reactivity of some compounds may be lowered by apportioning some of the carbon atoms to the non-reactive class NR. For example, the less reactive ethane (C2H6) is represented as 0.4 PAR and 1.6 NR)(EPA, 1999). Apportioning rules have been established for many organic compounds and can be found in e.g. Gery (1989), US EPA (1989) and Carter (1994).
The NMVOC
emissions are split into the model species as presented in Table 8.5 and 8.6
for CBM-IV and CB99, respectively. Presently, we use the VOC-splits as used in
LOTOS for CBM4 and EUROS for CB99. Hence,
the splits are not internally consistent. The split for CB99 is derived from Barrett and
Berge (1996) (see also Brouwer, 2005). The split for CBM4 is based on the
emission inventory of VOC’s, which are specified in 125 different species or
classes. These species are translated to Carbon bond species. The total and
lumbed VOC emissions within a SNAP 1 sector are summed to arrive at the total
VOC mass and the total moles of the lumbed Carbon Bond species, which were used
to determine the average VOC-split for a SNAP 1 category.
A newer version of
the split for the CBM4 gas phase chemistry scheme is available from the TROTREP
project. The major differences between the current used CBM-IV and TROTREP
split are the amount of PAR and UNR species. The TROTREP split yields more PAR
which is included as UNR (=Unreactive) in the present split. For a detailed
comparison of the available VOC-splits we refer to Brouwer (2005). For 2006 an
update of the VOC-splits to arrive at harmonisation between the schemes is
foreseen.
Table 8.5. VOC-speciation used for CBM-IV(mol/ (Kg VOC))
|
|
S |
OLE |
PAR* |
TOL |
XYL |
FORM |
ALD |
ETH |
UNR |
|
Power generation |
1 |
0.45 |
7.08 |
0.22 |
0.09 |
1.04 |
1.70 |
5.36 |
38.00 |
|
Small combustion sources |
2 |
0.45 |
7.08 |
0.22 |
0.09 |
1.04 |
1.70 |
5.36 |
38.00 |
|
Industrial combustion |
3 |
0.45 |
7.08 |
0.22 |
0.09 |
1.04 |
1.70 |
5.36 |
38.00 |
|
Industrial processes |
4 |
2.18 |
24.55 |
0.84 |
0.42 |
2.03 |
0.28 |
7.14 |
16.06 |
|
Extraction distribution of fossil fuels |
5 |
0.45 |
7.08 |
0.22 |
0.09 |
1.04 |
1.70 |
5.36 |
38.00 |
|
Solvent use |
6 |
0.10 |
39.85 |
0.65 |
0.75 |
0.00 |
0.52 |
0.19 |
2.95 |
|
(Road transport) |
(7) |
0.25 |
29.35 |
1.35 |
1.66 |
0.87 |
0.71 |
2.18 |
10.48 |
|
Other mobile sources |
8 |
0.45 |
7.08 |
0.22 |
0.09 |
1.04 |
1.70 |
5.36 |
38.00 |
|
Waste treatment and disposal |
9 |
0.45 |
7.08 |
0.22 |
0.09 |
1.04 |
1.70 |
5.36 |
38.00 |
|
Agriculture |
10 |
0.45 |
7.08 |
0.22 |
0.09 |
1.04 |
1.70 |
5.36 |
38.00 |
|
Road transport gasoline |
71 |
0.25 |
29.35 |
1.35 |
1.66 |
0.87 |
0.71 |
2.18 |
10.48 |
|
Road transport diesel |
72 |
0.20 |
44.13 |
0.25 |
0.25 |
2.27 |
0.72 |
3.93 |
5.69 |
|
Road transport lpg |
73 |
0.20 |
44.13 |
0.25 |
0.25 |
2.27 |
0.72 |
3.93 |
5.69 |
|
Road transport evaporation |
74 |
0.81 |
63.03 |
0.16 |
0.05 |
0.27 |
1.34 |
0.00 |
0.98 |
* PAR also includes the original CBM4 species ACET and KET following PAR = PAR + 3 ACET + 4 KET
The split for CB99
does not contain toluene (TOL). The reason is that in the past all toluene was
attributed to xylene (XYL). The actual split between these compounds could not
be recovered.
Table 8.6. VOC-speciation used for CB99 (mol/ (Kg VOC))
|
|
S |
OLE |
PAR |
TOL |
XYL |
FORM |
ALD2 |
ETH |
UNR |
MEOH |
ETOH |
|
Power generation |
1 |
2.19 |
24.29 |
0.00 |
0.60 |
0.73 |
0.55 |
5.75 |
0.00 |
0.13 |
4.85 |
|
Small combustion sources |
2 |
2.19 |
24.29 |
0.00 |
0.60 |
0.73 |
0.55 |
5.75 |
0.00 |
0.13 |
4.85 |
|
Industrial combustion |
3 |
2.19 |
24.29 |
0.00 |
0.60 |
0.73 |
0.55 |
5.75 |
0.00 |
0.13 |
4.85 |
|
Industrial processes |
4 |
0.00 |
0.80 |
0.00 |
0.17 |
0.03 |
0.05 |
0.68 |
0.00 |
0.03 |
20.33 |
|
Extraction distribution of fossil fuels |
5 |
2.19 |
24.29 |
0.00 |
0.60 |
0.73 |
0.55 |
5.75 |
0.00 |
0.13 |
4.85 |
|
Solvent use |
6 |
0.00 |
26.79 |
0.00 |
5.81 |
0.00 |
0.50 |
0.00 |
0.00 |
0.00 |
4.35 |
|
Road transport gasoline |
(7) |
1.81 |
23.79 |
0.00 |
7.83 |
0.53 |
0.25 |
3.07 |
0.00 |
0.00 |
1.91 |
|
Other mobile sources |
8 |
2.19 |
24.29 |
0.00 |
0.60 |
0.73 |
0.55 |
5.75 |
0.00 |
0.13 |
4.85 |
|
Waste treatment and disposal |
9 |
2.19 |
24.29 |
0.00 |
0.60 |
0.73 |
0.55 |
5.75 |
0.00 |
0.13 |
4.85 |
|
Agriculture |
10 |
2.19 |
24.29 |
0.00 |
0.60 |
0.73 |
0.55 |
5.75 |
0.00 |
0.13 |
4.85 |
|
Road transport gasoline |
71 |
1.81 |
23.79 |
0.00 |
7.83 |
0.53 |
0.25 |
3.07 |
0.00 |
0.00 |
1.91 |
|
Road transport diesel |
72 |
1.81 |
23.79 |
0.00 |
7.83 |
0.53 |
0.25 |
3.07 |
0.00 |
0.00 |
1.91 |
|
Road transport lpg |
73 |
1.81 |
23.79 |
0.00 |
7.83 |
0.53 |
0.25 |
3.07 |
0.00 |
0.00 |
1.91 |
|
Road transport evaporation |
74 |
1.81 |
23.79 |
0.00 |
7.83 |
0.53 |
0.25 |
3.07 |
0.00 |
0.00 |
1.91 |
1.2
Biogenic emissions
1.2.1 NMVOC and NO
In
the LOTOS-EUROS the biogenic NMVOC-emissions from forests are given by a method
developed by Veldt (1991). Apart from the difference between deciduous, coniferous
and mixed forest, the only other parameter was ambient temperature. Extensive
studies by Guenther showed that next to ambient temperature also the
Photosynthetic Active Radiation (PAR) is important Guenther (1994). These
findings by Guenther (1994) have been applied to
Although
In
the UBA-project FKZ 202 43270 a new CORINE/Smiatek land use data base has been
made incorporating detailed tree-species information based on Lenz et al. (2001)
containing 115 different tree-species on grids of 1 x 1 km2 over Europe. This
land use data base will be used in the near future to determine biogenic
emissions.
For isoprene the following formula is currently used:
Econif/decid Isoprene emission strength (g/m3/hr)
Tk Temperature (K)
The emission only occurs during daylight. The emission strength is weighted with the area covered with deciduous and/or coniferous forest.
Monoterpene emissions are included in the calculation for biogenic secondary aerosol concentrations. Monoterpene emissions, a-pinene and d-limoneen, are assumed to occur only from coniferous forest. For both species the following emission strength is calculated:
Econif Emission strength (g/m3/hr)
Tk Temperature (K)
C Constant, C is 0.23 for d-limonene and 0.21 for a-pinene
The emission only occurs during daylight. The emission strength is weighted with the area covered with coniferous forest.
Previous studies indicated only about 4 %
of the total NO emissions to be biogenic. For this reason we neglect the
biogenic emission of NO at the moment. The formulation by Yienger and Levy
,1995 has also been implemented in test-form and will be used in the near
future.
1.2.2 Sea salt
The sea salt emission fluxes in LOTOS-EUROS are currently described using the source formulation by Monahan et al. (1986). This source formulation is an empirical relation between the the whitecap cover, average decay time of a whitecap, the number of drops produced per square meter of whitecap and the resulting droplet flux dF/dr:
dF/dr source flux of salt particles per increment of drop radius (μm-1m-2s-1)
rp wet droplet radius (μm)
U10 wind speed at ten meter (m s-1)
W(U10) surface fraction covered with whitecap
dE/dr droplet flux per increment of drop radius per unit whitecap (μm-1m-2)
The implementation required to translate the particle flux provided by Monahan (1986) into a sea salt mass flux. As sea salt is most probably a wet aerosol after emission we have to account for the fact that the dry radius determines the sea salt mass and that the wet radius determines the atmospheric lifetime. The relation between dry and wet radius varies with relative humidity but for simplicity we assume a constant particle size. At a relative humidity of 80% the particle radius rp and dry particle radius rd are related as follows:
rp = 2.0*rd
Such a particle has a salt mass content mp of:
With 
the density of salt
(2.17 10-6 μg/m3). The salt
so that the mass flux for the Monahan formulation becomes:
The mass flux is obtained by integrating equation x with respect to rp. As the modelling of sea salt is usually performed in several size bins to account for the lifetime differences between particles of different size, the mass flux for each bin n is taken into account. The constant E and function f are independent of rp and can be taken outside the integral:
where rn and rn-1 are the upper and lower limits of each bin. The numeric value of E is 1.56 10-6 and the value for f(U10) is evaluated every hour in the model using the meteorological parameters from the model.
The sea salt module consists of two parts. The first part integrates the size dependent part (I) of the emission formulation over the size bins chosen for the simulation. The lowest size bin is integrated starting from 0.14 um as the Monahan function has not been validated for particles smaller than this size. These calculations are only performed at the start of the simulation. The second part of the module contains the actual calculation of the emission strength and is called every hour. The total flux is scaled with the percentage sea in the grid cell.