network for the support of european policies on air pollution the assessment of european control...
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Network for the support of European Policies on Air Pollution
The assessment of European control measures and the effects of
non-linearities
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Non-linearities
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Definition• What goes up comes down, the atmospheric mass
balance for the emitted reactive pollutants is closed.• However, the distance scale for the processes of
transport, transformation and deposition are large, and differ between the different pollutants (some emitted nitrogen escapes from the European domain, and surface ozone concentrations over Europe are dominated by the advected flux into Europe from the North Atlantic).
• In this project, we have identified non-linearities in source-receptor relationships at regional scales in sulphur and nitrogen compounds in air or deposition.
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• Apparent non-linearities………where for example unknown sources contribute to the deposition
• Real non-linearities occur when the processes regulating the lifetime of pollutants change with time (oxidation, deposition)
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Three examples
1. Shipping and the sulphur budget
2. Changes in dry deposition with time due to changes in SO2 / NH3
3. Oxidized nitrogen budgets
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Trends in sulphur deposition throughout the UK 1986-2001
Group 1* : nss-SO42- = -3.25 y + 6542
Group 2* : nss-SO42- = -1.06 y + 2159
Group 3* : nss-SO42- = -0.21 y + 459
Group 4 : nss-SO42- = -0.11 y + 237
* Statistically significant, P < 0.01
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Shipping!
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Vessel traffic densities for year 2000 based on the sum of reported distributions from AMVER data (AMVER, 2001)
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• Some areas of the UK show large reductions in acid deposition while other areas (eg Wales and Western Scotland), including some very heavily affected areas have changed little.
• Work continues on the influence of shipping emissions on S and N deposition (Univ Oslo)
% reduction from 87-01 in total non-marine Sulphur
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2. Has the SO2 dry deposition velocity changed ?
• Concentrations are declining faster than expected by models
• Current LRT models treat deposition velocity as simply coupled to meteorology and vegetation
• LIFE project provides important clues• Is there evidence of regional variations in surface
resistance and deposition velocity?
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KhsKha KhhonoKhc
Kn1 Ks1Kc1Ka
NH3,aq CO2,aq HNO2,aq
NH3 CO2 HNO2 SO2
SO2,aq
CO32- SO3
2- SO42-
NH4+ HCO3
- NO2- HSO3
- HSO4-
Ks2Kc2 Ks3
KwH2O H++OH-
d
Rd
AQUEOUS
GASEOUS
Kha
s(NH3)
Rs
Rcut
Fcut
Rb
Ra{z-d}
{z-d}
{z0’}=c
{z0}
WET DRY
HNO3
HCl
Cl-
NO3- H2O2
O3
APOPLAST
Ft
Fd
FsK+Mg2+
Na+ Ca2
+
K+Mg2+
Na+ Ca2
+
KaNH3,aqNH4
+
KwH2O H++OH-
The surface reactions are regulated by
SO2/NH3 interactions in
suface water films
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EMEP 2003 : Total deposition of oxidized S, 2000
mg S m-2 yr-1
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0
20
40
60
80
100
120
140
160
180
200
Speulder Forest Melpitz Auchencorth
Rc (
sm-1)
0
0.1
0.2
0.3
0.4
0.5
0.6
0.7
0.8
0.9
NH
4/S
O4
RcSO2
RcNH3
NH4/SO4
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Dry deposition rates of SO2 are regulated by chemical processes
in water films on terrestrial surfaces.
NH3 is the most important of the pollutants which regulate canopy
resistance to SO2 deposition.
Long term rates of SO2 deposition have increased with time as
NH3/SO2 ratios have increased.
Non-linearity is introduced into source-receptor matrices by
changes in SO2 emission in the presence of significant NH3
concentrations.
Dynamic chemical models are able to reproduce the measured
fluxes and resistances of SO2 and NH3 but are not currently
applied in Long-Range Transport models.
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EMEP model predicts slower trend in ambient
SO2 than observed
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Sulphur in the UK 1987-2001
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Non-linearities in the oxidized nitrogen budgets
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NOx emissions
Most of the change in emission has already taken place (2005: 50% since late 80’s, only <10% in the next 15 years)
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UK Emission deposition and export of atmospheric N 1900-2000 Emission Deposition Export
Oxidized N Emission
Reduced N Emission
Total Emission
Oxidized N Deposition
Reduced N Deposition
Total Deposition
Oxidized N Export
Reduced N Export
Total Export
1900 3121 1683 480 665 1637 229 246 5 250
1910 3181 1283 446 675 1257 192 251 4 255
1920 3271 1523 480 695 1487 217 258 4 262
1930 3271 1513 479 695 1477 216 258 4 262
1940 3451 1623 508 735 1587 231 272 4 277
1950 4841 1743 658 1025 1697 271 382 5 387
1960 6591 1813 840 1395 1767 315 520 5 525
1970 7311 1903 920 1545 1857 339 577 5 582
1980 7871 2283 1015 1946 2227 416 593 6 599
1990 6652 2413 906 1966 2348 430 470 7 476
2000 4602 2634 723 1916 2119 402 270 52 321
Total10 50014 18026 68040 11475 17484 28959 38539 542 39081
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Cause 1
From 1990 to 2010 land-based NOx will decrease from 13.4 to 6.6 MtWhile NOx from shipping will increase from 2.8 to 4.6 Mt. So, by 2010, 70%
of NOx will originate from shipping (in EU)
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Cause 2
NO2 emissions declined ~50%More O3 at nightNO2 NO3 HNO3
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Ecosystem Type 1995-1997 2010
Acid grassland 27 19
Heathland 56 42
Coniferous woodland 88 79
Deciduous woodland 96 92
All ecosystems 40 32
Exceedances of critical loads of ecosystems for eutrophication by nitrogen
in the UK (%)
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Detecting the signal of Nitrogen deposition in semi-natural vegetation
• 400 1kmx1km survey plots throughout the UK• Species composition and cover 1978, 1980,
2000• N deposition (Reduced and Oxidized) 5km• Clear signal linking loss of biodiversity to N
deposition.
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Conclusions
• Non-linearities exist and are a cause of regional variation in response to emission changes
• Detailed examination of the excellent long term data for air and precipitation composition is a vital step
• Models are the tools to summarize our knowledge, for integration, assessment and exploration of the interactions…but they lag behind our understanding of processes