air pollution & climate reactive gases and greenhouse gases · emission hcfc-141b. hcfc-141b ....

Air pollution & ClimateReactive Gases and Greenhouse Gases

Laboratory for Air Pollution and Environmental TechnologyBrigitte Buchmann, Stefan Reimann

Materials Sci ence & Technolog y

© R

. Lor

enzo

Air Pollution/Environmental Technology LaboratoryMaterials Sci ence & Technolog y

Overview

Measurement Programme @ Jungfraujoch

Laboratory Air Pollution / Environmental Technology

Examples of results- Detection of Trends / success of reduction measures- Emission Estimations- Analysis of Global Change impacts / Early warning

Future Activities

Measurements & Models


- Trace gas detection(low concentrations:ppq = 10-15)

- Satellite data(OMI column;

24 x 13 km2)

- Flux measurements(spectra @ kHz)

Lab’s Approach - Goals

MEDUSA

- Interspecies correlation(known emission inventory)

- Inverse modelling(Lagrangian ParticleDispersion model)

=EU-Emission CO

CO over background

Emission HCFC-141b

HCFC-141b over background=

EU-Emission CO

CO over background

EU-Emission CO

CO over background

Emission HCFC-141b

HCFC-141b over background

Emission HCFC-141b

HCFC-141b over background

Quantum Cascade Laser

- Statisticlal Approaches(receptor moels)

ijqp'

ip'pjp

ipij efgfgx ++= ∑∑ ~~~

ijqp'

ip'pjp

ipij efgfgx ++= ∑∑ ~~~

Emission EstimationLong-range Transport

Trend Analysis

Jungfraujoch – NETWORKS: CH, EU, world

40

0

South Pole

Point Barrow

Mauna Loa

Alert

Pallas-Sodankylä

MinamitorishimaKenya

Assekrem -Tamanrasset

Arembepe

Ushuaia

Izana

Amsterdam IslandCape Grim

Cape Point

Samoa

Ny Ålesund

Lauder

Mace Head

40

80

40

0

40

80

160 80 0 80 160

Zugspitze-Hohenpeissenberg

Mt Waliguan

Neumayer Station

Bukit Koto Tabang

Jungfraujoch

40

0

South Pole

Point Barrow

Mauna Loa

Alert

Pallas-Sodankylä

MinamitorishimaKenya

Assekrem -Tamanrasset

Arembepe

Ushuaia

Izana

Amsterdam IslandCape Grim

Cape Point

Samoa

Ny Ålesund

Lauder

Mace Head

40

80

40

0

40

80

160 80 0 80 160

Zugspitze-Hohenpeissenberg

Mt Waliguan

Neumayer Station

Bukit Koto Tabang

Jungfraujoch

Basel

Bern

Chaumont

Davos

DübendorfHärkingen

Jungfraujoch

Lägeren

Lausanne

Lugano

Magadino

PayerneRigi

Sion

TänikonZürich

Basel

Bern

Chaumont

Davos

DübendorfHärkingen

Lägeren

Lausanne

Lugano

Magadino

Payerne Rigi

Sion

TänikonZürich

Jungfraujoch

Global Atmosphere Watch, GAW, WMO

EMEP, EU


Swiss Air Pollution monitoringnetwork, NABEL

Advanced Global Atmospheric Gases Experiment

Laboratory for Air Pollution/Environmental Technology

Empa, ETH ZurichNABEL (FOEN, Empa)Empa

campaignscampaigns

,

PAN, HNO3OVOCs

H2

NABEL (FOEN, Empa), , , , NO, NO2, NOy

NABEL (FOEN, Empa)SO2

NABEL (FOEN, Empa)CO

NABEL (FOEN, Empa)O3Reactive gases

University of BerneCO2

NABEL (FOEN, Empa)SF6

SOGE (Empa, FOEN), , HCFCs, HFCs

SOGE (Empa, FOEN)CFCs

NABEL (FOEN, Empa)N2O

NABEL (FOEN, Empa)CH4Greenhouse gases

fundingJungfraujochRecommendedfor GAW

NABEL (FOEN, Empa)VOCs

Jungfraujoch: Greenhouse Gases & Reactive Gases

Non - CO2- Greenhouse Gases

Montreal Protocol

• CFCs: Fluorochlorocarbons:CFC-11, CFC-12CFC-113

• HCFCs: HydrofluorochlorocarbonsHCFC-141b, HCFC-124, HCFC-22, HCFC-142b,

• Halones: (containing bromo-atoms):H-1301, H-1211

• 1,1,1-Trichloroethane• Carbon tetrachloride (CCl4)

Kyoto Protocol

• HFCs: Hydrofluorocarbons:HFC-125, HFC-134aHFC-152a, HFC-23HFC-365mfc, HFC-245faHFC-227ea

• PFCs: perfluorocarbonsCF4, C2F6

• SF6: sulfur hexafluoride:


Air Pollution/Environmental Technology Laboratory

SEARCH: Individual Station report http://gaw.empa.ch/gawsis/

Trend Detection for Protocol Verification

0

20

40

60

80

100

2000 2001 2002 2003 2004 2005 2006

ppt

HFC 134a1,1,1-Trichlorethan

+ 0.6 mW/m2/y

- 0.3 mW/m2/y

1975 1980 1985 1990 1995 2000 2005

01

23

45

6SO

2(µ

g/m

3 )

Materials Science & Technology

1975 1980 1985 1990 1995 2000 2005

01

23

45

6SO

2(µ

g/m

3 )

Materials Science & Technology

„OECD –Program” Montreal - ProtocolKyoto - Protocol

Sulfur dioxide SO2Acid Rain

CFCs Greenhouse GasesOzone Depletion Global Warming



0.0

0.5

1.0

1.5

2.0

2.5

3.0

1973 1976 1979 1982 1985 1988 1991 1994 1997 2000 2003 2006

Sulp

hate

[ g/

m3 ]

Jungfraujoch

05

1015

2025

1973 1976 1979 1982 1985 1988 1991 1994 1997 2000 2003 2006

TSP

[g/

m3 ]

Jungfraujoch

Longest records at JFJ

JFJ CO time series (one hourly data) from 1996 to 2007 -The light blue curve represents a fitted baseline and the orange line the trend(after Thoning, et al., 1989, Novelli, et al., 1998; Novelli, et al., 2003)

21.3% carbon monoxide decrease from 1996 to 2007 at JFJ

Corresponds to an annual decrease of 1.78% - or 2.66 ppb/year


Carbon Monoxide Trend at Jungfraujoch

Trend Detection for Emission Reduction Control

CO – Emissions Inventories vs. Measurements

CO decrease mainly because of reduction of emissions

Traffic influenced sites in Switzerland (BER, LAU)show strongest CO decrease

Decrease at JFJ less pronounced, most likely due to influence of long-range transport

Global scale events, e.g. enhanced biomass burning in 1998, is visible in JFJ data

Emission data from http://dataservice.eea.europa.eu/dataservice/metadetails.asp?id=1013

1990 1995 2000 2005

0.0

0.5

1.0

1.5

2.0

YearYear

ly C

O m

ixin

g ra

tios

rel.

to 1

997

(Sta

tions

) / re

l. C

O e

mis

sion

s (C

ount

ries)

BERHAELAULUGSIOZUEJFJHPB

ATCHDEFRIT

JFJ is well situated to study both large-scale changes and regional air quality

Air Pollution/Environmental Technology LaboratoryM t i l S i & T h l

Contributions of European countries

Carbonmonoxide @ Jungfraujoch (Jun 02 – Dez 04)


Advection from “Low Northern Latitudes” @ JFJ

An advection of clean maritime air masses from low northern latitudes led to low CH4, CO, and CHCl3 and elevated H2 mixing ratios on October 1st.

68

1012

14

Date [mm/dd]09/28 09/30 10/02 10/04

CH

Cl3

[ppt

]

460

500

540

Date [mm/dd]09/28 09/30 10/02 10/04

H2

[ppb

]

Spatial Representativeness17

8018

2018

60

09/28 09/30 10/02 10/04

CH

4 [p

pb]

7080

9011

0

time09/28 09/30 10/02 10/04

CO

[ppb

]


Jungfraujoch only

Measurements+

Trajectories


CH4 at JFJ - Influence of Air Mass Origin


WMO WDCGG data summary, WDCGG report #30 (2006)Jungfraujoch only


Measurements+

Trajectories

CH4 at JFJ - Influence of Air Mass Origin


CH4 and N2O at JFJ and AGAGE sites17

0017

5018

0018

50

time (yyyy/mm)

CH

4 [p

pb]

2005/01 2006/01 2007/01 2008/0

MCJFJTHRPCMCG

a)

318

319

320

321

time (yyyy/mm)

N2O

[ppb

]

2005/01 2006/01 2007/01 2008/

MCJFJTHRPCMCG

b)

MC: Mace Head (53°N); JFJ (46°N), TH: Trinidad Head (41°N); RP: Ragged Point, Barbados (13°N); CM: Cape Matatula, American Samoa (14°S);

CG: Cape Grim (40°S).

Non - CO2- Greenhouse Gases

Montreal Protocol• CFCs: Fluorochlorocarbons:

CFC-11, CFC-12CFC-113

• HCFCs: HydrofluorochlorocarbonsHCFC-141b, HCFC-124, HCFC-22, HCFC-142b,

• Halones: (containing bromo-atoms):H-1301, H-1211

• 1,1,1-Trichloroethane• Carbon tetrachloride (CCl4)

Kyoto Protocol• HFCs: Hydrofluorocarbons:

HFC-125, HFC-134aHFC-152a, HFC-23HFC-365mfc, HFC-245faHFC-227ea

• PFCs: perfluorocarbonsCF4, C2F6

• SF6: sulfur hexafluoride:


MEDUSA

0

50

100

150

200

2000 2001 2002 2003 2004 2005

ppt

JungfraujochMace HeadNy-Alesund

F134a (refrigerant)


Emission Estimation

NWP modelsSource regions

0

10

20

30

40

50

95 96 97 98 99 00 01 02 03 04 05 06 07 08

ppt

Jungfraujoch (CH)Mace Head (IRE)Ny-Alesund (N)

HCFC 141b banned in Europe since 2003

Renewed European emissions of HCFC-141b?


2004 2005 2006 2007

2004 2005 2006 2007

F-152a

2003 520 t330 t

1880 t460 t

- t- t

National Communications to UNFCCC

AustriaBelgiumGermanyFranceItalySpain

2004 529 t288 t

1333 t297 t

- t- t

Foam blowing agent HFC-152a: Emissions from Europe

2006


2003 520 t330 t

1880 t460 t

- t

National Communications to UNFCCC

AustriaBelgiumGermanyFranceItalySpain

2004 529 t288 t

1333 t297 t

- t

2005 574 t204 t781 t313 t

- t170 t177 t 187 t

F-152a

2007

Foam blowing agent HFC-152a: Emissions from Europe

2004 2005 2006 2007

2006 416 t208 t669 t318 t

- t113 t


2000 2001 2002

Benefit of long-term series compared to short-term campaigns

Air-planeCampaignW-Europe Air-plane

CampaignCreta

Air Pollution/Environmental Technology

Ozone-destroying trichloroethane

0.3 -3.4 Gg/Jahr4 years continuous measurements Jungfraujoch / Mace Head

> 20 Gg/year 4 days aircraft observations above Europe

Krol et al., Nature (2003)Reimann et al., Nature (2005)

according to campaigns and long-term

measurements

Air Pollution/Environmental Technology

0

10

20

30

HFC-134a HFC-125 HFC-152a HCFC-141b

kt/J

ahr

2000200120022003200420052006

EU inventories

European H(C)FCs emissions: Jungfraujoch vs. inventories

kt/y

ear

Independent verification of Emissions


New foam blowing HFCs at Jungfraujoch

0

0.5

1

1.5

2

2003 2004 2005 2006 2007 2008

ppt

HFC-365mfc (pentafluorobutane)

HFC-245fa (pentafluoropropane)


Instrument development(fast and high-precision (QCL) laser spectroscopy )

CH4, N2O, CO2, H2O, NO213C16O16O, 12C18O16O, 14N15N16O, 15N14N16O

Simulated ν3 ro-vibrational bands of the CO2

12C16O16

O

12C16O18O

13C16O16

O


JFJ future Atmospheric ICOS site ?

CH Funding for Long-term EU infrastructure Programme (ESFRI): ?

Testphase of an 13 C

ICOS: Integrated Carbon Observation System: Ecosystem & Atmospheric Sites: ESFRIAtmospheric Site: CO2, 13CO2, 18CO2, CH4, N2O, H2, O2/N2, SF6, 222Radon,

First time continuous time series of CO2 Isotopes

12CO2

13CO2

C18O2


Current Cooperations

University of Bern

MeteoSwiss

PSI

ETHZ(Lohmann)

Greenhouse Gases& Reactive Gase


AGAGEMIT, CSIRO,SCRIPPS,

University of BristolETHZ

(Peter, Stählein)

University of Basel

GIRPAS

BIRA

222Radon


Papers Jungfraujoch 2007-2008

• Legreid, G., Folini, D., Staehelin, J., Balzani Lööv, J., Steinbacher, M. and Reimann, S. (2008). Measurements of organic trace gases including oxygenated volatile organic compounds at the high alpine site Jungfraujoch (Switzerland): Seasonal variation and source allocations. JOURNAL OF GEOPHYSICAL RESEARCH 113(D05307, doi:10.1029/2007JD008653.).

• Maione, M., Giostra, U., Arduini, J., Belfiore, L., Furlani, F., Geniali, A., Mangani, G., Vollmer, M. K. and Reimann, S. (2008). Localization of source regions of selected hydrofluorocarbons combining data collected at two European mountain stations. Science of The Total Environment 391(2-3): 232-240.

• Reimann, S., Vollmer, M. K., Folini, D., Steinbacher, M., Hill, M., Buchmann, B., Zander, R. and Mahieu, E. (2008). Observations of long-lived anthropogenic halocarbons at the high-Alpine site of Jungfraujoch (Switzerland) for assessment of trends and Europeansources. Science of The Total Environment 391(2-3): 224-31.

• Steinbacher, M., Vollmer, M. K., Buchmann, B. and Reimann, S. (2008). An evaluation of the current radiative forcing benefit of the Montreal Protocol at the high-Alpine site Jungfraujoch. Science of The Total Environment 391(2-3): 217-223.

• Zander, R., Mahieu, E., Demoulin, P., Duchatelet, P., Roland, G., Servais, C., Maziere, M. D., Reimann, S. and Rinsland, C. P. (2008). Our changing atmosphere: Evidence based on long-term infrared solar observations at the Jungfraujoch since 1950. Science of The Total Environment 391(2-3): 184-195..

• Cozic, J., Verheggen, B., Weingartner, E., Crosier, J., Bower, K. N., Flynn, M., Coe, H., Henning, S., Steinbacher, M., Henne, S., Collaud Coen, M., Petzold, A. and Baltensperger, U. (2008). Chemical composition of free tropospheric aerosol for PM1 and coarse mode at the high alpine site Jungfraujoch. Atmos. Chem. Phys. 8(2): 407-423

• Stemmler, K., Folini, D., Ubl, S., Vollmer, M. K., Reimann, S., Doherty, S. O., Greally, B. R., Simmonds, P. G. and Manning, A. J. (2007). European emissions of HFC-365mfc, a chlorine-free substitute for the foam blowing agents HCFC-141b and CFC-11. Environ. Sci. Technol. 41(4): 1145-1151.

• Kaiser, A., Scheifinger, H., Spangl, W., Weiss, A., Gilge, S., Fricke, W., Ries, L., Cemas, D. and Jesenovec, B. (2007). Transport of nitrogen oxides, carbon monoxide and ozone to the Alpine Global Atmosphere Watch stations Jungfraujoch (Switzerland), Zugspitze and Hohenpeissenberg (Germany), Sonnblick (Austria) and Mt. Krvavec (Slovenia). Atmospheric Environment 41(40): 9273-9287.

• Derwent, R. G., Simmonds, P. G., Greally, B. R., O'Doherty, S., McCulloch, A., Manning, A., Reimann, S., Folini, D. and Vollmer, M. K. (2007). The phase-in and phase-out of European emissions of HCFC-141b and HCFC-142b under the Montreal Protocol: Evidence from observations at Mace Head, Ireland and Jungfraujoch, Switzerland from 1994 to 2004. Atmospheric Environment 41(4): 757-767.

• Greally, B. R., et al. (2007). Observations of 1,1-difluoroethane (HFC-152a) at AGAGE and SOGE monitoring stations in 1994-2004 and derived global and regional emission estimates. J. Geophys. Res.-Atmos. 112(D6).

• Maione, M., Giostra, U., Arduini, J., Belfiore, L., Furlani, F., Geniali, A., Mangani, G., Vollmer, M. K. and Reimann, S. (2008). Localization of source regions of selected hydrofluorocarbons combining data collected at two European mountain stations. Science of The Total Environment 391(2-3): 232-240.


Thanks to: S. Reimann, M.K. Vollmer, M. Hill D. Brunner, S. Henne C. Hüglin, M. Steinbacher, B. Schwarzenbach L. Emmenegger, B. Tuzson

and International Foundation High Altitude

Research Stations Jungfraujoch andGornergrat

MeteoSwiss, BAFU, SNF

all research partner AGAGE/NOAA team

air pollution & climate reactive gases and greenhouse gases · emission hcfc-141b. hcfc-141b ....

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