Characterisation of 13CH4 source signatures from methane sources in Germany using mobile measurements
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This document summarizes research characterizing methane (CH4) isotopic (δ13CH4) signatures from various CH4 sources in Germany using mobile measurements. Key points: 1) A mobile instrument setup was developed and tested to measure δ13CH4 signatures downwind of sources without direct sampling. 2) Measurements near dairy farms, landfills, wastewater treatment plants, coal mines, and natural gas facilities showed distinct δ13CH4 ranges consistent with prior studies. 3) The mobile setup allows efficient characterization of different source signatures and comparisons to direct samples and other studies.
δ13
C(Atm)(‰) 1980 1990 2000 2010
(Schaefer et al., 2016)
September 13, 2018 2 / 13](https://image.slidesharecdn.com/session14hoheiselicosprague-181002115729/85/Characterisation-of-13CH4-source-signatures-from-methane-sources-in-Germany-using-mobile-measurements-2-320.jpg)
![Motivation
δ13
CH4 Isotopes
isotope ratio R and δ-notation
13
R =
13CH4
[12CH4 ]
δ =
Rsample
Rstandard
− 1 · 1000
main formation processes of CH4
biogenic −55 to −70 e.g. wetlands, landfills, WWTPs and
ruminants
thermogenic −25 to −45 e.g. main component of natural gas
pyrogenic −13 to −25 e.g. incomplete combustion of organic
matter
September 13, 2018 3 / 13](https://image.slidesharecdn.com/session14hoheiselicosprague-181002115729/85/Characterisation-of-13CH4-source-signatures-from-methane-sources-in-Germany-using-mobile-measurements-3-320.jpg)
![Measurement Setup
AirCore Measurements
2
3
4
5
6
CH4[ppm]
monitoring mode AirCore measurement
0 2 4 6 8 10 12 14
δ13
CH4[‰]
-65
-50
-55
-45
-60
-40
time [min]
CRDS
Nafion
dryer
AirCore
air
inlet
September 13, 2018 8 / 13](https://image.slidesharecdn.com/session14hoheiselicosprague-181002115729/85/Characterisation-of-13CH4-source-signatures-from-methane-sources-in-Germany-using-mobile-measurements-8-320.jpg)
![Data Analysis
Limitation Factors
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0 1 2 3 4 5 6 7 8 9 10
CH4 range [ppm]
δ13
CH4[‰]fiterrorof
40
35
30
25
20
15
10
5
0
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10
20
30
40
0.0 0.2 0.4 0.6 0.8 1.0
CH4 range [ppm]
●
δ13
CH4[‰]fiterrorof
simulations
measured data}
number of
data points
10
20
40
70
140
210
280
25-280
Criterion:
uncertainty of δ13
CH4
lower than 5
September 13, 2018 10 / 13](https://image.slidesharecdn.com/session14hoheiselicosprague-181002115729/85/Characterisation-of-13CH4-source-signatures-from-methane-sources-in-Germany-using-mobile-measurements-11-320.jpg)
![Data Analysis
δ13
CH4 Signature of CH4 Sources
79 AirCore measurements on 21 days between July 2016 to July 2017
q
q
−70 −65 −60 −55 −50 −45 −40
δ13
CH4 [‰]
natural gas facility Sandhausen
natural gas facility Hähnlein/Gernsheim
bituminous deep coal mine Bottrop
WWTP Heidelberg
landfill Sinsheim (plume)
landfill Sinsheim (on landfill)
biogas plant Heidelberg
dairy farm Ladenburg
dairy farm Kleve
dairy farm Weinheim
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qq q
q qqq q qqq q
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single mobile result
mean mobile result
direct sample result
September 13, 2018 11 / 13](https://image.slidesharecdn.com/session14hoheiselicosprague-181002115729/85/Characterisation-of-13CH4-source-signatures-from-methane-sources-in-Germany-using-mobile-measurements-12-320.jpg)
![Data Analysis
Samples from Natural Gas Distribution Network Heidelberg
δ13
CH4[‰]
−50
−45
−40
−35
−30
sample date
12/2016 03/2017 06/2017 09/2017 12/2017 03/2018 06/2018
winter
(Levin et al., 1999)
summer
(Levin et al., 1999)
−43.1 ± 0.8‰ 12/2016 to 02/2018
−40.3 ± 3.0‰ 1991 to 1996 (Levin et al., 1999)
(Lowry et al., 2001)
-48‰ to -54‰
(Cramer et al., 1998)
North Sea gas
Russian gas
-34 ± 3‰
September 13, 2018 12 / 13](https://image.slidesharecdn.com/session14hoheiselicosprague-181002115729/85/Characterisation-of-13CH4-source-signatures-from-methane-sources-in-Germany-using-mobile-measurements-13-320.jpg)
Characterisation of 13CH4 source signatures from methane sources in Germany using mobile measurements
- 1. antje.hoheisel@iup.uni-heidelberg.de Characterisation of δ13 CH4 source signatures from methane sources in Germany using mobile measurements A. Hoheisel, C. Yeman, F. Dinger, H. Eckhardt and M. Schmidt Institute of Environmental Physics Heidelberg University September 13, 2018 3rd ICOS Science Conference, Prague September 13, 2018 1 / 13
- 2. Motivation Global Atmospheric CH4 Mole Fraction and δ13 C HS GAW HS NOAA-ESRL 1980 1990 2000 2010 1800 1700 1600 -47.8 -47.6 -47.4 -47.2 -47.0 Year Year [CH4](p.p.b.) δ13 C(Atm)(‰) 1980 1990 2000 2010 (Schaefer et al., 2016) September 13, 2018 2 / 13
- 3. Motivation δ13 CH4 Isotopes isotope ratio R and δ-notation 13 R = 13CH4 [12CH4 ] δ = Rsample Rstandard − 1 · 1000 main formation processes of CH4 biogenic −55 to −70 e.g. wetlands, landfills, WWTPs and ruminants thermogenic −25 to −45 e.g. main component of natural gas pyrogenic −13 to −25 e.g. incomplete combustion of organic matter September 13, 2018 3 / 13
- 4. Motivation CH4 Sources Berlin Hamburg Frankfurt on the Main Cologne Stuttgart Amsterdam Brussels Munich dairy farm in Kleve deep coal mine in Bottrop opencast mine Hambach measuring sites near Heidelberg dairy farm in Weinheim dairy farm in Ladenburg natural gas storage and compressorstations Hähnlein/Gernsheim natural gas storage Sandhausen landfill in Sinsheim WWTP in Heidelberg biogas plant in Heidelberg Heidelberg Weinheim Sinsheim Mannheim 358 km 22.4 km measuring sites near Heidelberg Berlin Frankfurt on the Main Cologne Stuttgart Amsterdam Brussels Kleve Bottrop Weinheim Ladenburg Sandhausen Sinsheim Heidelberg Heidelberg Weinheim Sinsheim Mannheim 400 km 20 km Munich Hähnlein/Gernsheim Heidelberg dairy farm biogas plant wastewater treatment plant landfill natural gas storage and compressor stations deep coal mine measuring sites September 13, 2018 4 / 13
- 5. Measurement Setup Measuring Principle 7 15s mean: raw: September 13, 2018 5 / 13
- 6. Measurement Setup Mobile Measurement Setup AirCore Picarro G2201-i (Yeman,2015) September 13, 2018 6 / 13
- 7. Measurement Setup Mobile Measurement Setup filter air inlet three-way valve Nafion dryer critical orifice AirCore needle pump CRDS laptop filter valve AirCore volume: 1.77 l length: 25 m diameter: 9.5 mm flow through instrument monitoring mode: 0.16 l/min AirCore measurement: 0.10 l/min September 13, 2018 7 / 13
- 8. Measurement Setup AirCore Measurements 2 3 4 5 6 CH4[ppm] monitoring mode AirCore measurement 0 2 4 6 8 10 12 14 δ13 CH4[‰] -65 -50 -55 -45 -60 -40 time [min] CRDS Nafion dryer AirCore air inlet September 13, 2018 8 / 13
- 9. Data Analysis Determination of δ13 CH4 Signature δ13 CH4 Correction and Calibration CH4 interference → no effect CO2 interference → no effect H2O interference → drying unit C2H6 interference → corrections September 13, 2018 9 / 13
- 10. Data Analysis Determination of δ13 CH4 Signature δ13 CH4 Correction and Calibration H2O interference → drying unit C2H6 interference → corrections Fit Method Miller-Tans Approach δ13 CH4M · CH4M = CH4B δ13 CH4B − δ13 CH4S + δ13 CH4S · CH4M York fit Limitation Factors: precision of the analyser number of data points → importance of AirCore CH4 range Criterion: uncertainty of δ13 CH4 lower than 5 September 13, 2018 9 / 13
- 11. Data Analysis Limitation Factors ●●● ● ● ● ● ● ● ● ●● ● ● ● ● ● ● ● ● ● ●● ● ● ●● ● ● ● ● ●● ● ● ● ● ● ● ● ● ● ● ● ● ● ● ● ● ● ● ● ● ● ●● ● ● ● ● ● ●● ● ● ● ● ● ●● ● ● ● ● ● ● ● ● ● ● ● ● ● ● ● ● ● ● ● ●● ● ● ● ● ● ● ● ● ● ● ● ● ● ● ● ● ● ● ● ● ● ● ● ● ● ● ● ● ●● ● ● ● ● ● ●● ● ● ● ● ● ● ● ●●● ● ● ● ● ● ● ● ●● ● ● ● ● ● ● ● ● ● ●● ● ● ●● ● ● ● ● ●● ● ● ● ● ● ● ● ● ● ● ● ● ● ● ● ● ● ● ● ● ● ●● ● ● ● ● ● ●● ● ● ● ● ● ●● ● ● ● ● ● ● ● ● ● ● ● ● ● ● ● ● ● ● ● ●● ● ● ● ● ● ● ● ● ● ● ● ● ● ● ● ● ● ● ● ● ● ● ● ● ● ● ● ● ●● ● ● ● ● ● ●● ● ● ● ● ● ● ● 0 1 2 3 4 5 6 7 8 9 10 CH4 range [ppm] δ13 CH4[‰]fiterrorof 40 35 30 25 20 15 10 5 0 ● ● ● ●● ● ● ● ● ● ● ● ● ● ● ● ● ● ● ● ● ● ● ● ● ● ● ●● ● ● ● ● ● ● ● ● ● ● ● ● ● ● ● ● ● ● ● ● ● ● ● ● ●● ● ● ● ● ● ● ●● ● ● ● ● ● ● ● ● ● ● ● ● ● ● ● ● ● ● ● ● ● ● ●● ● ● ● ● ● ● ● ● ● ● ● ● ● ● ● ● ● ● ● ● ● ● ● ● ●● ● ● ● 0 10 20 30 40 0.0 0.2 0.4 0.6 0.8 1.0 CH4 range [ppm] ● δ13 CH4[‰]fiterrorof simulations measured data} number of data points 10 20 40 70 140 210 280 25-280 Criterion: uncertainty of δ13 CH4 lower than 5 September 13, 2018 10 / 13
- 12. Data Analysis δ13 CH4 Signature of CH4 Sources 79 AirCore measurements on 21 days between July 2016 to July 2017 q q −70 −65 −60 −55 −50 −45 −40 δ13 CH4 [‰] natural gas facility Sandhausen natural gas facility Hähnlein/Gernsheim bituminous deep coal mine Bottrop WWTP Heidelberg landfill Sinsheim (plume) landfill Sinsheim (on landfill) biogas plant Heidelberg dairy farm Ladenburg dairy farm Kleve dairy farm Weinheim q qq q qq qq q q qqq q qqq q q qqq q q qq qqqq qq qqq qqq qqqq qqq q qq q q qq q q qqq qqqq q q q q qq qqqqqq qq q q qq q q q qq qqqqqq qq q q qq q qqq qq qqq q qqqq q q q qq q qq qq qq qq q q q q qq q q single mobile result mean mobile result direct sample result September 13, 2018 11 / 13
- 13. Data Analysis Samples from Natural Gas Distribution Network Heidelberg δ13 CH4[‰] −50 −45 −40 −35 −30 sample date 12/2016 03/2017 06/2017 09/2017 12/2017 03/2018 06/2018 winter (Levin et al., 1999) summer (Levin et al., 1999) −43.1 ± 0.8‰ 12/2016 to 02/2018 −40.3 ± 3.0‰ 1991 to 1996 (Levin et al., 1999) (Lowry et al., 2001) -48‰ to -54‰ (Cramer et al., 1998) North Sea gas Russian gas -34 ± 3‰ September 13, 2018 12 / 13
- 14. Conclusion Conclusion development and test of a mobile instrument setup results of mobile campaigns are in good agreement with direct samples and values from other studies advantages: measurements can be done downwind of emission source consent of the owner is not necessary measurements can be done where it is not possible to take direct samples September 13, 2018 13 / 13
- 15. Thank you for your attention. September 13, 2018 13 / 13