Stratospheric Ozone polar stratospheric clouds. Die Ozonproblematik Quelle: US EPA (
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Transcript of Stratospheric Ozone polar stratospheric clouds. Die Ozonproblematik Quelle: US EPA (
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Stratospheric Ozone
polar stratospheric clouds
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Die Ozonproblematik
Quelle: US EPA (http://www.epa.gov/oaqps001/gooduphigh/good.html)
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Stratosphärische Ozonschicht schützt vor UV Strahlung
UV-B
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Stratosphärische Ozonschicht schützt vor UV Strahlung
UV-AUV-B
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Brief history of stratospheric ozone (1)1881 Hartley identifies ozone as main cause for
cutoff of solar spectrum at 300 nm
1921 Fabry and Buisson obtain first reliable measurement of overhead column ozone
1918 Strutt measured tropospheric „column“ with „40 ppb or less“ bulk of ozone in stratosphere
1926 Dobson and Harrison measure latitudinal distribution of total ozone
1930 Chapman theory; Schumacher measured rate coefficients
1931-34 Götz identified an ozone layer and located maximum near 22 km
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Brief history of stratospheric ozone (2)1960 McGrath and Norris discover OH production and
propose catalytic ozone destruction cycle1971 Crutzen and Johnston discover NOx cycle1974 Molina and Rowland recognize impact of man-made
chlorofluoromethanes1985 Farman discovers Antarctic ozone hole1987 Montreal protocol1995 Nobel prize for Crutzen, Molina, and Rowland
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VERTEILUNG VON OZON
7
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Ozon-Vertikalprofile in der Nordhemisphäre
8Dütsch, 1974
Januar April
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Merdionalschnitt der Ozonverteilung in nb
9Dütsch, 1974
February May
August November
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Merdionalschnitt der Ozonverteilung in ppm
10Dütsch, 1974
April June
October December
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Dobson Units
11
1 DU entspricht der Menge Ozon in der Gesamtsäule, die bei Normaldruck (1015 hPa) und 0C in eine Höhe von 0.01 mm passen würde.
Typischer Wert für die Ozonsäulendichte:300 DU
1 DU = 2.691016 molec. cm-2
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Ozonsäulendichte
12
Homogenisierte Zeitreihe der Ozonsäulendichte 1979-2009 aus Satellitendaten; Einheit: Dobson Units (DU)
http://www.gmes-stratosphere.euhttp://www.temis.nl/macc/knmi_content/zonal_monthly_mean.png
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Ozonsäulendichte
13
Jan
Jul
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Der Chapman Zyklus (1)
(1) O2 + h O + O
(2) O + O2 + M O3 + M
(3) O3 + h O2 + O
(4) O3 + O O2 + O2
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Der Chapman Zyklus (2)
(1) O2 + h O + O
(2) O + O2 + M O3 + M
(3) O3 + h O2 + O
(4) O3 + O O2 + O2
OOOMOOO
343223
3 kjk
dt
dO
Bilanzgleichung für Ozonkonzentration:
Im Gleichgewicht:
0
O3 dt
d
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Der Chapman Zyklus (3)
OOOMOO0 34322 3 kjk O
Verlustterm L fast immer linear von der Konzentration (hier O3) abhängig.Daher:
bzw.:
3O LP
P L
O
MOOO
4
223
3
kj
kP
O
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Lebensdauer (1)
LFPFdt
dQoutin
Definition der Verweildauer:
Bei Annahme des Gleichgewichts ("steady state") gilt ebenfalls:
LF
Q
out
Allgemeine Masse-Bilanzgleichung in einem Teilvolumen der Atmosphäre:
PF
Q
in
Bezieht man die gesamte Atmosphäre als Reservoir ein, dann folgt:
P
Q
L
Q Dieses ist die Lebensdauer
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Lebensdauer (2)
Bei mehreren Verlustprozessen gilt:
bzw.:
Wenn der Verlust erster Ordnung ist (also proportional zu Q):
21
111
1
Q
Q
L
Q
2121
1
Q
Q
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Lebensdauer (3)
Bei inhomogener Konzentrationsverteilung bzw. nicht-konstanter Reaktionsrate (also im Regelfall), muss integriert werden:
V
V
dVq
dVq
xx
x
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Ozonverteilung aus dem Chapman-Zyklus
theory
observed
LebensdauerKonzentration
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Catalytic ozone destruction
(5) X + O3 XO + O2
(6) XO + O X + O2
net O3 + O O2 + O2
X can be H, OH, NO, Cl, or Br.
(6) is usually the rate-limiting step.
30N, May
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Competing Reactions
H, OH and HO2 species formed by reaction of excited O atoms with H-containing atmospheric species like H2O and CH4
O3 + hn O(1D) + O2
O(1D) + H2O OH + OH
O(1D) + CH4 CH3 + OH
H2O + hn H + OH
HOx cycle (1)
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Competing Reactions
OH + O3 HO2 + O2
HO2 + O OH + O2
HOx cycle (2)
net: O + O3 2O2
X + O3 XO + O2
XO + O X + O2
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NOx cycle
N2O + O(1D) 2 NO
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Simulation of NOy in MOZART3 (March Avg)
Auroral Production
N2O+O1D production
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Reactions of NOx species with O3
NOx cycle (2)
NO + O3 NO2 + O2
NO2 + O NO + O2
net: O + O3 2O2
X + O3 XO + O2
XO + O X + O2
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ClOx cycle
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Competing Reactions
ClOx species (Cl, ClO) are produced from chlorofluorocarbons (CFCs) and methyl chloride (CH3Cl).
Example (Freon CF2Cl2):
CF2Cl2 + hn CF2Cl + Cl
CF2Cl2 + O CF2Cl + ClO
ClOx cycle
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Systematik der CFCs
32
CFC-01234a (oder HCFC-… oder HFC-…)0 = Anzahl der Doppelbindungen (fällt weg, falls keine vorhanden)1 = Anzahl C-Atome minus 1 (fällt weg, falls Null)2 = Anzahl H-Atome plus 13 = Anzahl F-Atome4 = Anzahl Cl-Atome, die durch Br ersetzt werden (fällt weg, falls keine vorhanden)a = Buchstabe zur Identifizierung unterschiedlicher Isomere
Die Anzahl Cl-Atome ergibt sich aus der Strukturformeldes Ausgangs-Kohlenwasserstoffs.
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Beispiele für CFCs
33
CFC-11 CCl3F trichlorofluoromethane
CFC-12 CCl2F2 dichlorodifluoromethane
CFC-113 CCl2F-CClF2 1,1,2-trichlorotrifluoroethane
HCFC-22 CHClF2 chlorodifluoromethane
HCFC-123 CHCl2-CF3 2,2-dichloro-1,1,1-trifluoroethane
HCFC-123a CHClF-CClF2 1,2-dichloro-1,1,2-trifluoroethane
HFC-23 CHF3 trifluoromethane
HFC-134 CHF2-CHF2 1,1,2,2-tetrafluoroethane
HFC-134a CH2F-CF3 1,2,2,2-tetrafluoroethane
HCFC-20 CHCl3 chloroform
Halon-1211 CBrClF2 bromochlorodifluoromethane
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Reactions of NOx species with O3
ClOx cycle (2)
Cl + O3 ClO + O2
ClO + O Cl + O2
net: O + O3 2O2
Nobelpreis Chemie 1995
X + O3 XO + O2
XO + O X + O2
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Katalytische Ozonzerstörung
37
Chapman:
O2 + h O + O
O + O2 + M O3 + M
O3 + h O2 + O
O3 + O O2 + O2
Aktivierungsenergie: 17.1 kJ mol-1
Katalytisch (ClOx):
Cl + O3 ClO + O2
ClO + O Cl + O2
Aktivierungsenergie: 2.1 kJ mol-1
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DAS OZONLOCH
38
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41
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42
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WMO Ozone Bulletin
43
http://www.wmo.int/pages/prog/arep/gaw/ozone/
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Entstehung des Ozonlochs in der Antarktis
• Der zirkumpolare Luftstrom ("polar vortex") im Winter sorgt für eine Isolierung der antarktischen Luftmassen vom Rest der Atmosphäre
• Extreme Abkühlung durch Abstrahlung (ca. -80C)
• Bildung von polaren Stratosphärenwolken (PSC)
• Anlagerung nicht reaktiver Chlorverbindungen (HCl und ClONO2)
• Heterogene Umwandlung in "aktive" Chlorverbindungen (HOCl und Cl2), die gasförmig freigesetzt werden
• Mit dem ersten Sonnenlicht im Frühjahr Photolyse der aktiven Chlorverbindungen und katalytische Ozonzerstörung
44
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Chlor-Aktivierung
45
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ZUKÜNFTIGE ENTWICKLUNG STRATOSPHÄRISCHEN OZONS 55
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60
"Super recovery"
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MODELLIERUNG VON STRATOSPHÄRISCHEM OZON
61
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MOZART-3
62
Model of Ozone and related tracersPaper by Kinnison et al., 2006 (J. Geophys. Res.)
• 108 Spezies• 218 Gasphasen-Reaktionen• 71 Photolyse-Reaktionen• 18 Heterogene Reaktionen
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MOZART-3 heterogene Reaktionen (1)
63
(liquid)
(solid, T 200 K)
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MOZART-3 heterogene Reaktionen (2)
64
(solid, T 185 K)
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EP TOMS vs MZ3/ECMWF, September 15, 2002
1.25 lon x 1.0 lat
1.9 lon x 1.9 lat
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EP TOMS vs MZ3/ECMWF, September 25, 2002
1.25 lon x 1.0 lat
1.9 lon x 1.9 lat