An analytical inversion method for determining regional and global emissions of greenhouse gases: Sensitivity studies and application to halocarbons

Abstract. A new analytical inversion method has been developed to determine the regional and global emissions of long-lived atmospheric trace gases. It exploits in situ measurement data from three global networks and builds on backward simulations with a Lagrangian particle dispersion model. The emission information is extracted from the observed concentration increases over a baseline that is itself objectively determined by the inversion algorithm. The method was applied to two hydrofluorocarbons (HFC-134a, HFC-152a) and a hydrochlorofluorocarbon (HCFC-22) for the period January 2005 until March 2007. Detailed sensitivity studies with synthetic as well as with real measurement data were done to quantify the influence on the results of the a priori emissions and their uncertainties as well as of the observation and model errors. It was found that the global a posteriori emissions of HFC-134a, HFC-152a and HCFC-22 all increased from 2005 to 2006. Large increases (21%, 16%, 18%, respectively) from 2005 to 2006 were found for China, whereas the emission changes in North America (−9%, 23%, 17%, respectively) and Europe (11%, 11%, −4%, respectively) were mostly smaller and less systematic. For Europe, the a posteriori emissions of HFC-134a and HFC-152a were slightly higher than the a priori emissions reported to the United Nations Framework Convention on Climate Change (UNFCCC). For HCFC-22, the a posteriori emissions for Europe were substantially (by almost a factor 2) higher than the a priori emissions used, which were based on HCFC consumption data reported to the United Nations Environment Programme (UNEP). Combined with the reported strongly decreasing HCFC consumption in Europe, this suggests a substantial time lag between the reported time of the HCFC-22 consumption and the actual time of the HCFC-22 emission. Conversely, in China where HCFC consumption is increasing rapidly according to the UNEP data, the a posteriori emissions are only about 40% of the a priori emissions. This reveals a substantial storage of HCFC-22 and potential for future emissions in China. Deficiencies in the geographical distribution of stations measuring halocarbons in relation to estimating regional emissions are also discussed in the paper. Applications of the inversion algorithm to other greenhouse gases such as methane, nitrous oxide or carbon dioxide are foreseen for the future.

[1]  A. Stohl,et al.  On the pathways and timescales of intercontinental air pollution transport , 2002 .

[2]  Petra Seibert,et al.  Iverse Modelling with a Lagrangian Particle Disperion Model: Application to Point Releases Over Limited Time Intervals , 2004 .

[3]  W. Menke Geophysical data analysis , 1984 .

[4]  Petra Seibert,et al.  Parameterization of Convective Transport in a Lagrangian Particle Dispersion Model and Its Evaluation , 2007 .

[5]  P. Fraser,et al.  Trace gas emissions from Melbourne, Australia, based on AGAGE observations at Cape Grim, Tasmania, 1995-2000 , 2005 .

[6]  R. Weiss,et al.  A history of chemically and radiatively important gases in air deduced from ALE/GAGE/AGAGE , 2000 .

[7]  Derek M. Cunnold,et al.  Observations of 1,1‐difluoroethane (HFC‐152a) at AGAGE and SOGE monitoring stations in 1994–2004 and derived global and regional emission estimates , 2007 .

[8]  Remo Guidieri Res , 1995, RES: Anthropology and Aesthetics.

[9]  A. Stohl,et al.  Arctic smoke – record high air pollution levels in the European Arctic due to agricultural fires in Eastern Europe in spring 2006 , 2006 .

[10]  William Menke,et al.  10 – FACTOR ANALYSIS , 1984 .

[11]  P. Midgley,et al.  Recent changes in the production and global atmospheric emissions of chlorodifluoromethane (HCFC-22) , 2006 .

[12]  Kerstin Stebel,et al.  Estimation of the vertical profile of sulfur dioxide injection into the atmosphere by a volcanic eruption using satellite column measurements and inverse transport modeling , 2008 .

[13]  S. Reimann,et al.  Localization of source regions of selected hydrofluorocarbons combining data collected at two European mountain stations. , 2008, The Science of the total environment.

[14]  S. Reimann,et al.  Halogenated greenhouse gases at the Swiss High Alpine site of Jungfraujoch (3580 m asl): Continuous measurements and their use for regional European source allocation , 2004 .

[15]  R. Prinn,et al.  Estimation of atmospheric methane emissions between 1996 and 2001 using a three-dimensional global chemical transport model , 2006 .

[16]  M. Maione,et al.  Evaluation of an automatic sampling gas chromatographic–mass spectrometric instrument for continuous monitoring of trace anthropogenic gases , 2004 .

[17]  L. Kuijpers,et al.  Emission profiles from the foam and refrigeration sectors comparison with atmospheric concentrations. Part 2: results and discussion , 2004 .

[18]  D. Jacob,et al.  Eastern Asian emissions of anthropogenic halocarbons deduced from aircraft concentration data , 2003 .

[19]  Corinne Le Quéré,et al.  Climate Change 2013: The Physical Science Basis , 2013 .

[20]  W. Menke Geophysical data analysis : discrete inverse theory , 1984 .

[21]  Hubert Glaab,et al.  Global backtracking of anthropogenic radionuclides by means of a receptor oriented ensemble dispersion modelling system in support of Nuclear-Test-Ban Treaty verification , 2007 .

[22]  Masataka Shiobara,et al.  Arctic smoke record high air pollution levels in the European Arctic due to agricultural fires in Eastern Europe , 2006 .

[23]  Y. Yokouchi,et al.  High frequency measurements of HFCs at a remote site in east Asia and their implications for Chinese emissions , 2006 .

[24]  R. Betts,et al.  Changes in Atmospheric Constituents and in Radiative Forcing. Chapter 2 , 2007 .

[25]  Gerhard Wotawa,et al.  Atmospheric transport modelling in support of CTBT verification—overview and basic concepts , 2003 .

[26]  N. Mahowald,et al.  Inverse methods in global biogeochemical cycles , 2000 .

[27]  Petra Seibert,et al.  Source-receptor matrix calculation with a Lagrangian particle dispersion model in backward mode , 2004 .

[28]  R. Weiss,et al.  Rapid growth of hydrofluorocarbon 134a and hydrochlorofluorocarbons 141b, 142b, and 22 from Advanced Global Atmospheric Gases Experiment (AGAGE) observations at Cape Grim, Tasmania, and Mace Head, Ireland , 2004 .

[29]  A. Manning,et al.  Estimating European emissions of ozone-depleting and greenhouse gases using observations and a modeling back-attribution technique , 2003 .

[30]  A. Stohl,et al.  Technical note: The Lagrangian particle dispersion model FLEXPART version 6.2 , 2005 .

[31]  D. Blake,et al.  Halocarbon emissions from the United States and Mexico and their global warming potential. , 2009, Environmental science & technology.

[32]  Kerry Emanuel,et al.  Development and Evaluation of a Convection Scheme for Use in Climate Models , 1999 .

[33]  Ronald G. Prinn,et al.  Feasibility of determining surface emissions of trace gases using an inverse method in a three‐dimensional chemical transport model , 1993 .

[34]  A. Stohl,et al.  Record high peaks in PCB concentrations in the Arctic atmosphere due to long-range transport of biomass burning emissions , 2007 .

[35]  A. Stohl,et al.  Validation of the lagrangian particle dispersion model FLEXPART against large-scale tracer experiment data , 1998 .

[36]  P. Midgley,et al.  Releases of refrigerant gases (CFC-12, HCFC-22 and HFC-134a) to the atmosphere , 2003 .

[37]  Sven-Erik Gryning,et al.  Air Pollution Modeling and Its Application XIV , 2001 .

[38]  D. Thomson,et al.  A Density Correction for Lagrangian Particle Dispersion Models , 1999 .

[39]  R. Smith,et al.  Automated Gas Chromatograph/Mass Spectrometer for Routine Atmospheric Field Measurements of the CFC Replacement Compounds, the Hydrofluorocarbons and Hydrochlorofluorocarbons , 1995 .

[40]  A. Stohl,et al.  Around the world in 17 days - hemispheric-scale transport of forest fire smoke from Russia in May 2003 , 2004 .

[41]  S. Reimann,et al.  Observations of long-lived anthropogenic halocarbons at the high-Alpine site of Jungfraujoch (Switzerland) for assessment of trends and European sources. , 2008, The Science of the total environment.

[42]  R. Weiss,et al.  Medusa: a sample preconcentration and GC/MS detector system for in situ measurements of atmospheric trace halocarbons, hydrocarbons, and sulfur compounds. , 2008, Analytical chemistry.

[43]  Ian G. Enting,et al.  Inverse problems in atmospheric constituent transport , 2002 .

[44]  Y. Yokouchi,et al.  Development of an Analytical Method for Atmospheric Halocarbons and Its Application to Airborne Observation , 2005 .

[45]  L. Kuijpers,et al.  Emission profiles from the foam and refrigeration sectors comparison with atmospheric concentrations. Part 1: Methodology and data , 2004 .

[46]  N. Mahowald,et al.  Deducing CCl3F emissions using an inverse method and chemical transport models with assimilated winds , 1997 .

[47]  Frank Arnold,et al.  A Backward Modeling Study of Intercontinental Pollution Transport using Aircraft Measurements , 2003 .

[48]  A. Jakeman,et al.  A new inverse method for trace gas flux estimation: 2. Application to tropospheric CFCl3 fluxes , 1998 .