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Simone Meinardi, Barbara Barletta, Paul Nissenson, Donald Dubdub and Donald Blake
University of California, Irvine
ARCTAS Goal :
better understand the factors driving current changes in Arctic atmospheric composition and climate,
(1) transport of midlatitude pollution
(2) boreal forest fires
(3) chemical processes
Observation of CFC replacements during the 2008 Arctic Research of the Composition of the
Troposphere from Aircraft and Satellites (ARCTAS) field campaign.
ARCTASA : April 2008
ARCTASB : JuneJuly 2008
ARCTASCARB :
4 flights – 617 cans
Aircrafts : DC8 / P3 / B200
Deployments:
Analytical System
CH3Br Ethylbenzene
3Methyl2BuONO2 CH3Cl oXylene
2PeONO2 CCl4 pXylene
3PeONO2 C2Cl4 mXylene
Limonene 2BuONO2 C2HCl3 Toluene
betaPinene nPrONO2 CH2Cl2 Benzene
alphaPinene iPrONO2 CH3CCl3 nHexane
Isoprene EtONO2 CHCl3 nPentane
MeONO2 HCFC141b iPentane
Methanol CO HCFC142b iButene
Ethanol CH4 HCFC22 1Butene
MAC DMS HFC152a trans2Butene
MVK CS2 HFC134a cis2Butene
2Butanone OCS H1301 nButane
Acetone CHBr3 H2402 iButane
Acetaldehyde CHBr2Cl H1211 Propene
CHBrCl2 CFC114 Propane
HFC365mfc CH2Br2 CFC113 Ethyne
HCFC123 CH2ClCH2Cl CFC11 Ethene
HCFC124 CH3I CFC12 Ethane
126 124 122 120 118 116
32
34
36
38
40
42
44
Longitude
Latitude
2
4
6
8
10
12
Altitude, km
ARCTASCARB sampling
Flights 1215 + 16 + 24
San Joaquin Valley – SJV (red circles)
San Diego (red +) Mexico border (blue +)
128 126 124 122 120 118 116 30
32
34
36
38
40
Longitude
Latitud
e
2
4
6
8
10
12
123 122 121 120 119 118 31.5
32.0
32.5
33.0
33.5
34.0
31.5
32.0
118 117.5 117 116.5 116 115.5 115 31.5
32.0
32.5
33.0
33.5
34.0
San Diego
South Coast Air Basin –SCAB (within gray line)
+ Los Angeles – LA area
(red circles)
128 126 124 122 120 118 116 114 112 30
32
34
36
38
40
42
44
46
Longitude
Latitude
1
2
3
4
5
6
7
8
9 Altitude, km
Inflow – 60 samples – Flight 14
Designed to capture air moving toward California, with minimal North American influence.
They do not represent the regional background as they could be affected by polluted air masses intercepted over the Pacific area,
0
20
40
60
80
100
1988 1992 1996 2000 2004 2008 2012 2016 2020 2024 2028 2032 2036 2040
NonA5 A5
NonA5 baseline: 1989* A5 baseline: 2015
* Baseline calculated as 1989 HCFC consumption + 2.8% of 1989 CFC consumption
(%)
Applicable to consumption HCFCs
0
50
100
150
200
250
10 90 190 290 390 490 590
LA SCAB San Diego SJV Mexico Border clean air
HCFC142b (GWP 100yr : 2310) 407, 598, 780, 856
0
20
40
60
80
100
120
140
10 90 190 290 390 490 590
LA SCAB San Diego SJV Mexico Border clean air
HCFC141b (GWP 100yr : 725) 237
59 ± 137 pptv over LA area 20.1 ± 1.1 pptv inflow
30 ± 16 pptv over LA area 19.7 ± 1.0 pptv inflow
HFC134a (GWP 100yr : 1430)
INTEXB 2006
20 25 30 35 40 45 50 55 60 65
0 50 100 150 200
HFC
134a, pptv
Stratospheric intrusion Chinese Plumes Asian Plumes Background US Plumes
0
50
100
150
200
250
300
350
400
10 90 190 290 390 490 590
LA SCAB San Diego SJV Mexico Border clean air
HFC
134a, pptv
89 ± 77 pptv over LA area 46 ± 2 pptv inflow
ARCTAS 2008
HFC152a – 1,1Difluoroethane
GWP 100yr : 124
42 ± 40 pptv over LA area 8.9 ± 5.0 pptv inflow
0
50
100
150
200
250
300
350
400
450
10 90 190 290 390 490 590
LA SCAB San Diego SJV Mexico Border clean air
HFC152a – 1,1Difluoroethane 1a – HFC152a Mixing Ratios, pptv 1a – HFC152a Mixing Ratios, pptv
HFC152a – 1,1Difluoroethane 1b HFC152a Mixing Ratios, pptv 1b HFC152a Mixing Ratios, pptv
0.005 – 0.01 [1] Australia 2004
37 [2] Global 2006
0.46 [1] Europe 199598
0.8 [1] Europe 200001
2 [1] Europe 2003
16 [2] North
America 2006
2004
200203
Late ‘90s
Year
Global
Global
Global
Location
28 [1]
20 22 [1] 4 [1]
Emissions (Gg/yr)
HFC152a global emissions for the 19942004 period increased at a rate of about 14% per year.
In 2008 global emission will be ~ 47 Gg/yr
HFC152a – Emissions from literature
[1] Greally, B.R. et al., 2007 (and references therein). Journal of Geophysical Research, 112, D06308, doi:10.1029/2006JD007527. [2] Stohl, A. et al., 2009. Atmospheric Chemistry and Physics, 9, 1597.
HFC152a vs CO
= 0.98 ± 0.05 Gg/yr – LA county ** CO emissions from LA county (CARB, 2009)
0.57•10 3 mol HFC152a 66 (g/mol) HFC152a 2•10 9 (g/day) CO 365 days/yr
mol CO 28 (g/mol) CO × × ×
**
mol CO 28 (g/mol) CO ×
0
20
40
60
80
100
120
140
50 100 150 200 250 300 350
CO, ppbv
HFC
152a, pptv
slope = 0.57± 0.03 mmol/mol R 2 = 0.85
The population data can be used to estimate HFC152a emissions from the U.S.
0.98 ± 0.05 Gg/yr (LA county)
9.9•10 6 (population in LA county) 304•10 6 (U.S. population) ×
= 30 ± 1.5 Gg/yr (U.S.) = U.S. estimate for 2008
0.005 – 0.01 [1] Australia 2004
37 [2] Global 2006
0.8 [1] Europe 200001
2 [1] Europe 2003
16 [2] North America 2006
2004
Year
Global
Location
28 [1]
Emissions (Gg/yr)
U.S. Estimates
Conclusions 1. Several CFC replacements compounds were measured during the
summer 2008 over California’s most significant source regions.
2. Both HCFCs and HFCs were highly were highly enhanced over the investigated areas, particularly in Southern California and, specifically, over Los Angeles.
3. Annual emissions of HFC152a were estimated using the HFC 152a : CO ratio.
4. 0.98 Gg/yr of HFC152a were estimated from the LA County.
5. Using population data, the 2008 HFC152 emissions from the United States were 30 Gg/yr (about 60% of the global emissions).
2.3 3.8 5.0 6.3 7.5 8.8 10.0 11.3 12.5 13.8 15.0 16.3 17.5 19.7 4.2
10.0
15.0
20.0
25.0
30.0
34.1
1 GULFNEWRAMP #2 [modified by barbara, 2 peaks manually assigned] Int_Chan_5 2 GULFNEWRAMP #7 [modified by barbara, 2 peaks manually assigned] Int_Chan_5 mV
min
2 1 1 Propene (B) 4.605
2 Propane (B) 4.748
3 CH3Cl (B) 6.109
4 iButane (B) 6.796
5 1Butene/iButene (B) 7.637
6 nButane (B) 7.927
7 9.790
8 iPentane (B) 9.945 9 nPentane (B) 10.552
10 11.195
11 2,2Dimethylbutane (B) 11.282
12 Cyclopentane (B) 11.814
13 2,3Dimethylbutane (B) 11.862
14 2Methylpentane (B) 11.946
15 11.998 16 12.086
17 3Methylpentane (B) 12.201 18 nHexane (B) 12.502 19 Methylcyclopentane (B) 12.962
20 2,4Dimethylpentane (B) 13.013
21 Benzene (B) 13.352
22 Cyclohexane (B) 13.510 23 2Methylhexane (B) 13.606
24 2,3Dimethylpentane (B) 13.649
25 13.713
26 3Methylhexane (B) 13.744
27 13.873
28 13.915
29 2,2,4Trimethylpentane (B) 13.958
30 nHeptane (B) 14.098 31 Methylcylohexane (B) 14.473
32 2,3,4Trimethylpentane (B) 14.869
33 Toluene (B) 14.949
34 2Methylheptane (B) 15.049
35 15.073
36 3Methylheptane (B) 15.160
37 15.186
38 nOctane (B) 15.502
39 Ethylbenzene (B) 16.224
40 m/pXylene (B) 16.328
41 oXylene (B) 16.594
42 16.662
43 nNonane (B) 16.700
44 mEthyltoluene (B) 17.275
45 17.318
46 1,3,5Trimethylbenzene (B) 17.343
47 nDecane (B) 17.669
48 1,2,3Trimethylbenzene (B) 17.909
49 nUndecane (B) 18.565