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Measurement-based verification of regional emissions of halogenated greenhouse gases

English title Measurement-based verification of regional emissions of halogenated greenhouse gases
Applicant Reimann Stefan
Number 137638
Funding scheme Project funding (Div. I-III)
Research institution Luftfremdstoffe / Umwelttechnik 500 - Mobility, Energy and Environment EMPA
Institution of higher education Swiss Federal Laboratories for Materials Science and Technology - EMPA
Main discipline Climatology. Atmospherical Chemistry, Aeronomy
Start/End 01.04.2012 - 30.04.2016
Approved amount 218'739.00
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Keywords (5)

greenhouse gas; halocarbons; emission verification; Kyoto Protocol; Jungfraujoch

Lay Summary (English)

Lead
Lay summary

For the fluorinated substances explicitly listed as greenhouse gases in the Kyoto-Protocol industrialized countries annually report their emissions, based on information about usage and specific source factors (bottom-up estimates). However, a real-world verification of emissions with atmospheric measurements is yet missing (top-down estimates). In addition, the industry is continuously marketing new halocarbons as replacements of forbidden compounds (e.g. CFCs) or is using them as feedstock in production processes. For these so far unregulated halocarbons it is important to initiate measurement capabilities to provide an early-warning tool.

At the high-Alpine site of Jungfraujoch halogenated greenhouse gases are continuously measured since 2000 uisng gas chromatography-mass spectrometry (GCMS). These measurements are exploited for detecting atmospheric background trends and for localizing and quantifying regional European emissions.

With this PhD work this approach will be extended and new developments will be incorporated to advance both analytical and instrumental techniques for atmospheric halocarbons and to employ new tools for emission estimation. Furthermore, existing methods to quantify regional sources will be applied in campaigns in currently still under-sampled European regions (Spain, Greece).

The PhD work will be composed of three tasks:

1) Use the new abilities of the highly sensitive Medusa-GCMS measurement technology to detect new halocarbons in the atmosphere. This will be achieved by both screening for unknown substances and selectively searching for newly marketed substances and halocarbons used as feedstock.

2) Use the newly developed high-resolution transport model COSMO-FLEXPART for improved independent estimations of Swiss and regional European emissions of halogenated greenhouse gases by measurements at the high-Alpine site Jungfraujoch.

3) Perform measurement campaigns in Greece and Spain (under-sampled regions of Europe) and independently verify regional emission of halocarbons.

The main expected impact will be an improved understanding of the spatial distribution of European halocarbon emissions. This will be an important step for the verification of inventories used within international treaties by real-world atmospheric measurements.

Direct link to Lay Summary Last update: 21.02.2013

Responsible applicant and co-applicants

Employees

Publications

Publication
Abundance and sources of atmospheric halocarbons in the Eastern Mediterranean
Schoenenberger Fabian, Henne Stephan, Hill Matthias, Vollmer Martin K., Kouvarakis Giorgos, Mihalopoulos Nikolaos, O&, apos, Doherty Simon, Maione Michela, Emmenegger Lukas, Peter Thomas, Reimann Stefan (2018), Abundance and sources of atmospheric halocarbons in the Eastern Mediterranean, in Atmospheric Chemistry and Physics, 18(6), 4069-4092.
Abrupt reversal in emissions and atmospheric abundance of HCFC‐133a (CF3CH2Cl)
Vollmer Martin, Rigby Matt, Laube Johannes C., Henne Stephan, Rhee Tae Siek, J. Gooch Lauren, Wenger Angelina, Young Dickon, Steele L. Paul, Langenfelds Ray L., Brenninkmeijer Carl A. M., Wang Jia‐Lin, Ou‐Yang Chang‐Feng, Wyss Simon A., Hill Matthias, Oram David E., Krummel Paul B., Schoenenberger Fabian, Zellweger Christoph, Fraser Paul J., Sturges William T., O'Doherty Simon, Reimann Stefan (2015), Abrupt reversal in emissions and atmospheric abundance of HCFC‐133a (CF3CH2Cl), in Geophysical Research Letters, 42(20), 8702-8710.
First observations, trends and emissions of HCFC-31 (CH2ClF) in the global atmosphere
Schoenenberger Fabian, Vollmer Martin, Rigby Matt, Hill Matthias, Fraser Paul, Krummel Paul, Langenfelds Ray, Rhee Tae Siek, Peter Thomas, Reimann Stefan (2015), First observations, trends and emissions of HCFC-31 (CH2ClF) in the global atmosphere, in Geophysical Research Letters, 42(18), 7817-7824.
Modern inhalation anesthetics: Potent greenhouse gases in the global atmosphere
Vollmer Martin, Rhee Tae Siek, Rigby Matt, Hofstetter Doris, Hill Matthias, Schoenenberger Fabian, Reimann Stefan (2015), Modern inhalation anesthetics: Potent greenhouse gases in the global atmosphere, in Geophysical Research Letters, 42(5), 1606-1611.

Datasets

Atmospheric Halocarbon Observations at Finokalia, Crete, Greece

Author Reimann, Stefan
Publication date 01.03.2018
Persistent Identifier (PID) https://zenodo.org/record/1186221#.XA6Go4oxlOQ
Repository Zenodo
Abstract
Atmospheric halocarbon (HFC, HCFC) observations (mole fractions) from the site Finokalia (FKL, 35.34 °N, 25.67 °E, 250 m a.s.l.) on the island of Crete, Greece, covering the period December 2012 to August 2013). The measurements were conducted using a gas chromatograph(Agilent 6890) and:mass spectrometer (Agilent 5973) (GC-MS), coupled to an adsorption desorption system (ADS) for preconcentration of samples from the air (Simmonds et al., 1995).The measurements are described in detail in: Schoenenberger, F., S. Henne, M. Hill, M. K. Vollmer, G. Kouvarakis, N. Mihalopoulos, S. O'Doherty, M. Maione, L. Emmenegger, T. Peter, and S. Reimann (2017), Abundance and Sources of Atmospheric Halocarbons in the Eastern Mediterranean, Atmos. Chem. Phys. Discuss., 2017, 1-46, doi: 10.5194/acp-2017-451.The data format is plain text character-separated and follows that used in the AGAGE community. Further details are given at the AGAGE data archive: http://agage.eas.gatech.edu/data_archive/agage/

FLEPXART backward dispersion simulations

Author Henne, Stephan
Publication date 08.03.2018
Persistent Identifier (PID) https://zenodo.org/record/1194037#.XA6IRIoxlOQ
Repository Zenodo
Abstract
The dataset contains results of the Lagrangian Particle Dispersion Model FLEXPART as used in Schoenenberger et al. (201).FLEXPART was run in backward, receptor-oriented mode for 4 sites: Jungfraujoch, Monte Cimone, Mace Head, Finokalia.FLEXPART was driven by ECMWF IFS windfields with a global resolution of 1° x 1° and 0.2° x 0.2° for the Alpine area. 50,000 particles are released every 3 hours and followed backward in time for 10 days.

R packages for atmospheric emission inversion

Author Henne, Stephan
Publication date 09.03.2018
Persistent Identifier (PID) https://zenodo.org/record/1194642#.XA6JJooxlOQ
Repository Zenodo
Abstract
R packages that were developed for the inverse modelling of regional halocarbon emissions. The main package Rinversion (revision 7833), contains the code for the inverse modelling, whereas the other packages contain required dependencies: Rflexpart (r8303), deals with output from the atmospheric dispersion model FLEXPART myRplots (r8130), contains basic utilities to plot different types of spatial distributions myRtools (r8135), provides additional helper functions (interpolation, grid operators, etc.) meteoconv (r8122), provides basic, frequently-used conversion functions for atmospheric quantitiesThe packages were developed using R version 3.1.0. Using a newer version of R may result in compatibility issues and is not recommended. The revision numbers reflect the versions as used in Schönenberger et al., Atmospheric Chemistry and Physics, 2018.

Atmospheric inversion results: sources of atmospheric halocarbons in the Eastern Mediterranean

Author Henne, Stephan
Publication date 09.03.2018
Persistent Identifier (PID) https://zenodo.org/record/1194645#.XA6JkIoxlOQ
Repository Zenodo
Abstract
Settings, run script, observations and results from all inverse modelling runs used in Schönenberger et al., APC, 2018, for European sources of halocarbons for the year 2013.Settings and run script can be found in inversion_run_scripts.tar.gz. In order to reprocess the results the R package 'Rinversion' for atmospheric inversion (https://doi.org/10.5281/zenodo.1194641) has to be installed and the simulated source sensitivities (https://doi.org/10.5281/zenodo.1194037) have to be downloaded. Observations (halocarbon_observations.tar.gz) are post-processed observations of the AGAGE network (http://agage.mit.edu/) plus those gathered at the Finokalia site (https://doi.org/10.5281/zenodo.1186221).Inversion results (inversion_results.tar) are contained as separate packages for each individual sensitivity experiment described in the publication. The sensitivity experiments are listed in inversion_results/InversionRuns.xlsx and agree with those listed in Table 1 of the publication. Subfolders are organised by halocarbon species: HCFC_142b, HCFC_22, HFC_125, HFC_152a, HFC_134, HFC_143a. For each halocarbon results are stored in form of plots, ASCII spread sheets (csv, dat) or R data objects (.rda). Time series and distribution plots are available in separate subfolders. Intermediate data used by the inversion code are stored in 'intermediates', whereas the final results of each inversion run are stored as a single R object (inversion_results_XXX.rda).

Collaboration

Group / person Country
Types of collaboration
AGAGE United States of America (North America)
- in-depth/constructive exchanges on approaches, methods or results
- Publication
Climate Research Laboratory, University of Barcelona, LRC-PCB Spain (Europe)
- Research Infrastructure
Environmental Chemical Processes Laboratory Department of Chemistry - University of Crete Greece (Europe)
- Publication
- Research Infrastructure
Institute of Environmental Geosciences/University of Basel Switzerland (Europe)
- in-depth/constructive exchanges on approaches, methods or results
Atmospheric Chemistry Research Group/University of Bristol Great Britain and Northern Ireland (Europe)
- in-depth/constructive exchanges on approaches, methods or results

Scientific events

Active participation

Title Type of contribution Title of article or contribution Date Place Persons involved
AGAGE49 Talk given at a conference HCFC-31, first measurements 02.05.2014 Ascona, Switzerland Reimann Stefan; Schönenberger Fabian; Vollmer Martin K.;
international evaluation of Empa_Posterpresentation Poster Measurements in Finokalia 07.11.2012 Duebendorf, Switzerland Schönenberger Fabian; Brunner Dominik; Reimann Stefan;


Associated projects

Number Title Start Funding scheme
175921 IHALOME: Innovation in Halocarbon Measurements and Emission Validation 01.09.2018 Project funding (Div. I-III)
157689 APRECON-GC-TOFMS: Advanced PRECONcentration and GC-TOFMS analysis for atmospheric halocarbons, related to ozone depletion and climate change 01.09.2015 R'EQUIP
128725 Halogenated Greenhouse Gases by a Swiss MEDUSA 01.12.2009 R'EQUIP
159194 Biological ice nucleators at tropospheric cloud height (4th year) 01.09.2015 Project funding (Div. I-III)
117753 Assessment of European emissions of non-CO2 greenhouse gases by a combination of continuous measurements, transport models and RN-222 emission maps 01.06.2008 Project funding (Div. I-III)

Abstract

At the high-Alpine site of Jungfraujoch halogenated greenhouse gases are continuously measured by Empa since 2000. These measurements have been exploited for detecting atmospheric background trends and for localizing and quantifying regional European emissions.For the fluorinated substances explicitly listed as greenhouse gases in the Kyoto-Protocol industrialized countries annually report their emissions, based on information about usage and specific source factors (bottom-up estimates). However, a critical real-world verification of emissions with atmospheric measurements is yet missing (top-down estimates). In addition, the industry is continuously marketing new halocarbons as replacements of regulated compounds (e.g. CFCs) or is using them as feedstock in production processes. For these so far unregulated halocarbons it is important to initiate measurement capabilities to provide an early-warning tool. This newly designed PhD work will help to enable Empa to advance both analytical and instrumental techniques and to employ new tools for emission estimation. Furthermore, existing methods to quantify regional sources will be applied in campaigns in currently still under-sampled European regions (Spain, Greece). The PhD work is a follow-up of a nearly completed (2008-2011) PhD work at Empa (Assessment of European emissions of non-CO2 greenhouse gases by a combination of continuous measurements, transport models and 222Rn emission maps; SNF-Nr. 200021-117753/1). The PhD work will be carried out at Empa in co-operation with Prof. Thomas Peter (IACETH, ETHZ) and will be composed of three tasks:1) Use the new abilities of the highly sensitive Medusa-GCMS measurement technology to detect new halocarbons in the atmosphere. This will be achieved by both screening for unknown substances and selectively searching for newly marketed substances and undeclared halocarbons used as feedstock. 2) Use the newly developed high-resolution transport model FLEXPART-COSMO for improved independent estimations of Swiss and regional European emissions of halogenated greenhouse gases by measurements at the high-Alpine site Jungfraujoch.3) Perform measurement campaigns in Greece and Spain (i.e. under-sampled regions of Europe) and independently verify regional emission of halocarbons.The main expected impact will be an improved understanding of the spatial distribution of European halocarbon emissions. This will be an important step for the critical verification of inventories used within international treaties.
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