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Title: U.S. emissions of HFC-134a derived for 2008-2012 from an extensive flask-air sampling network: US emissions of HFC-134a

Abstract

Abstract U.S. national and regional emissions of HFC‐134a are derived for 2008–2012 based on atmospheric observations from ground and aircraft sites across the U.S. and a newly developed regional inverse model. Synthetic data experiments were first conducted to optimize the model assimilation design and to assess model‐data mismatch errors and prior flux error covariances computed using a maximum likelihood estimation technique. The synthetic data experiments also tested the sensitivity of derived national and regional emissions to a range of assumed prior emissions, with the goal of designing a system that was minimally reliant on the prior. We then explored the influence of additional sources of error in inversions with actual observations, such as those associated with background mole fractions and transport uncertainties. Estimated emissions of HFC‐134a range from 52 to 61 Gg yr −1 for the contiguous U.S. during 2008–2012 for inversions using air transport from Hybrid Single‐Particle Lagrangian Integrated Trajectory (HYSPLIT) model driven by the 12 km resolution meteorogical data from North American Mesoscale Forecast System (NAM12) and all tested combinations of prior emissions and background mole fractions. Estimated emissions for 2008–2010 were 20% lower when specifying alternative transport from Stochastic Time‐Inverted Lagrangian Transport (STILT) model driven by the Weathermore » Research and Forecasting (WRF) meteorology. Our estimates (for HYSPLIT‐NAM12) are consistent with annual emissions reported by U.S. Environmental Protection Agency for the full study interval. The results suggest a 10–20% drop in U.S. national HFC‐134a emission in 2009 coincident with a reduction in transportation‐related fossil fuel CO 2 emissions, perhaps related to the economic recession. All inversions show seasonal variation in national HFC‐134a emissions in all years, with summer emissions greater than winter emissions by 20–50%.« less

Authors:
 [1];  [2];  [1];  [2];  [3];  [1];  [2];  [1];  [4];  [5];  [2];  [2];  [6];  [6];  [6];  [7];  [7];  [7];  [8];  [9] more »;  [9];  [2];  [2];  [2] « less
  1. Univ. of Colorado, Boulder, CO (United States); National Oceanic and Atmospheric Administration (NOAA), Boulder, CO (United States)
  2. National Oceanic and Atmospheric Administration (NOAA), Boulder, CO (United States)
  3. Univ. of Colorado, Boulder, CO (United States)
  4. Univ. of Groningen, (Netherlands). Centre for Isotope Research
  5. US Environmental Protection Agency (EPA), Washington DC (United States)
  6. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  7. Atmospheric and Environmental Research, Lexington MA (United States)
  8. Harvard Univ., Cambridge, MA (United States)
  9. National Oceanic and Atmospheric Administration (NOAA), College Park, MD (United States)
Publication Date:
Research Org.:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Biological and Environmental Research (BER)
OSTI Identifier:
1512160
Alternate Identifier(s):
OSTI ID: 1402295
Grant/Contract Number:  
AC02-05CH11231
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Geophysical Research: Atmospheres
Additional Journal Information:
Journal Volume: 120; Journal Issue: 2; Journal ID: ISSN 2169-897X
Publisher:
American Geophysical Union
Country of Publication:
United States
Language:
English
Subject:
54 ENVIRONMENTAL SCIENCES

Citation Formats

Hu, Lei, Montzka, Stephen A., Miller, John B., Andrews, Aryln E., Lehman, Scott J., Miller, Benjamin R., Thoning, Kirk, Sweeney, Colm, Chen, Huilin, Godwin, David S., Masarie, Kenneth, Bruhwiler, Lori, Fischer, Marc L., Biraud, Sebastien C., Torn, Margaret S., Mountain, Marikate, Nehrkorn, Thomas, Eluszkiewicz, Janusz, Miller, Scot, Draxler, Roland R., Stein, Ariel F., Hall, Bradley D., Elkins, James W., and Tans, Pieter P. U.S. emissions of HFC-134a derived for 2008-2012 from an extensive flask-air sampling network: US emissions of HFC-134a. United States: N. p., 2014. Web. doi:10.1002/2014JD022617.
Hu, Lei, Montzka, Stephen A., Miller, John B., Andrews, Aryln E., Lehman, Scott J., Miller, Benjamin R., Thoning, Kirk, Sweeney, Colm, Chen, Huilin, Godwin, David S., Masarie, Kenneth, Bruhwiler, Lori, Fischer, Marc L., Biraud, Sebastien C., Torn, Margaret S., Mountain, Marikate, Nehrkorn, Thomas, Eluszkiewicz, Janusz, Miller, Scot, Draxler, Roland R., Stein, Ariel F., Hall, Bradley D., Elkins, James W., & Tans, Pieter P. U.S. emissions of HFC-134a derived for 2008-2012 from an extensive flask-air sampling network: US emissions of HFC-134a. United States. https://doi.org/10.1002/2014JD022617
Hu, Lei, Montzka, Stephen A., Miller, John B., Andrews, Aryln E., Lehman, Scott J., Miller, Benjamin R., Thoning, Kirk, Sweeney, Colm, Chen, Huilin, Godwin, David S., Masarie, Kenneth, Bruhwiler, Lori, Fischer, Marc L., Biraud, Sebastien C., Torn, Margaret S., Mountain, Marikate, Nehrkorn, Thomas, Eluszkiewicz, Janusz, Miller, Scot, Draxler, Roland R., Stein, Ariel F., Hall, Bradley D., Elkins, James W., and Tans, Pieter P. Wed . "U.S. emissions of HFC-134a derived for 2008-2012 from an extensive flask-air sampling network: US emissions of HFC-134a". United States. https://doi.org/10.1002/2014JD022617. https://www.osti.gov/servlets/purl/1512160.
@article{osti_1512160,
title = {U.S. emissions of HFC-134a derived for 2008-2012 from an extensive flask-air sampling network: US emissions of HFC-134a},
author = {Hu, Lei and Montzka, Stephen A. and Miller, John B. and Andrews, Aryln E. and Lehman, Scott J. and Miller, Benjamin R. and Thoning, Kirk and Sweeney, Colm and Chen, Huilin and Godwin, David S. and Masarie, Kenneth and Bruhwiler, Lori and Fischer, Marc L. and Biraud, Sebastien C. and Torn, Margaret S. and Mountain, Marikate and Nehrkorn, Thomas and Eluszkiewicz, Janusz and Miller, Scot and Draxler, Roland R. and Stein, Ariel F. and Hall, Bradley D. and Elkins, James W. and Tans, Pieter P.},
abstractNote = {Abstract U.S. national and regional emissions of HFC‐134a are derived for 2008–2012 based on atmospheric observations from ground and aircraft sites across the U.S. and a newly developed regional inverse model. Synthetic data experiments were first conducted to optimize the model assimilation design and to assess model‐data mismatch errors and prior flux error covariances computed using a maximum likelihood estimation technique. The synthetic data experiments also tested the sensitivity of derived national and regional emissions to a range of assumed prior emissions, with the goal of designing a system that was minimally reliant on the prior. We then explored the influence of additional sources of error in inversions with actual observations, such as those associated with background mole fractions and transport uncertainties. Estimated emissions of HFC‐134a range from 52 to 61 Gg yr −1 for the contiguous U.S. during 2008–2012 for inversions using air transport from Hybrid Single‐Particle Lagrangian Integrated Trajectory (HYSPLIT) model driven by the 12 km resolution meteorogical data from North American Mesoscale Forecast System (NAM12) and all tested combinations of prior emissions and background mole fractions. Estimated emissions for 2008–2010 were 20% lower when specifying alternative transport from Stochastic Time‐Inverted Lagrangian Transport (STILT) model driven by the Weather Research and Forecasting (WRF) meteorology. Our estimates (for HYSPLIT‐NAM12) are consistent with annual emissions reported by U.S. Environmental Protection Agency for the full study interval. The results suggest a 10–20% drop in U.S. national HFC‐134a emission in 2009 coincident with a reduction in transportation‐related fossil fuel CO 2 emissions, perhaps related to the economic recession. All inversions show seasonal variation in national HFC‐134a emissions in all years, with summer emissions greater than winter emissions by 20–50%.},
doi = {10.1002/2014JD022617},
journal = {Journal of Geophysical Research: Atmospheres},
number = 2,
volume = 120,
place = {United States},
year = {Wed Dec 17 00:00:00 EST 2014},
month = {Wed Dec 17 00:00:00 EST 2014}
}

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Works referenced in this record:

Anthropogenic emissions of methane in the United States
journal, November 2013

  • Miller, S. M.; Wofsy, S. C.; Michalak, A. M.
  • Proceedings of the National Academy of Sciences, Vol. 110, Issue 50
  • DOI: 10.1073/pnas.1314392110

Global emissions of HFC-143a (CH 3 CF 3 ) and HFC-32 (CH 2 F 2 ) from in situ and air archive atmospheric observations
journal, January 2014

  • O'Doherty, S.; Rigby, M.; Mühle, J.
  • Atmospheric Chemistry and Physics, Vol. 14, Issue 17
  • DOI: 10.5194/acp-14-9249-2014

Vertical mixing in atmospheric tracer transport models: error characterization and propagation
journal, January 2008

  • Gerbig, C.; Körner, S.; Lin, J. C.
  • Atmospheric Chemistry and Physics, Vol. 8, Issue 3
  • DOI: 10.5194/acp-8-591-2008

The global recession of 2009 in a long-term development perspective
journal, July 2010

  • Gore, Charles
  • Journal of International Development, Vol. 22, Issue 6
  • DOI: 10.1002/jid.1725

An extended Kalman-filter for regional scale inverse emission estimation
journal, January 2012

  • Brunner, D.; Henne, S.; Keller, C. A.
  • Atmospheric Chemistry and Physics, Vol. 12, Issue 7
  • DOI: 10.5194/acp-12-3455-2012

Coupled weather research and forecasting–stochastic time-inverted lagrangian transport (WRF–STILT) model
journal, May 2010

  • Nehrkorn, Thomas; Eluszkiewicz, Janusz; Wofsy, Steven C.
  • Meteorology and Atmospheric Physics, Vol. 107, Issue 1-2
  • DOI: 10.1007/s00703-010-0068-x

Halocarbon Emissions from the United States and Mexico and Their Global Warming Potential
journal, February 2009

  • Millet, Dylan B.; Atlas, Elliot L.; Blake, Donald R.
  • Environmental Science & Technology, Vol. 43, Issue 4
  • DOI: 10.1021/es802146j

Assessing the uncertainty associated with national greenhouse gas emission inventories:
journal, November 2001


Robust estimation of the variogram: I
journal, April 1980

  • Cressie, Noel; Hawkins, Douglas M.
  • Journal of the International Association for Mathematical Geology, Vol. 12, Issue 2
  • DOI: 10.1007/bf01035243

Linking emissions of fossil fuel CO 2 and other anthropogenic trace gases using atmospheric 14 CO 2 : THE
journal, April 2012

  • Miller, John B.; Lehman, Scott J.; Montzka, Stephen A.
  • Journal of Geophysical Research: Atmospheres, Vol. 117, Issue D8
  • DOI: 10.1029/2011JD017048

Maximum likelihood estimation of covariance parameters for Bayesian atmospheric trace gas surface flux inversions
journal, January 2005

  • Michalak, Anna M.; Hirsch, Adam; Bruhwiler, Lori
  • Journal of Geophysical Research, Vol. 110, Issue D24
  • DOI: 10.1029/2005JD005970

A multitower measurement network estimate of California's methane emissions: CALIFORNIA'S METHANE EMISSIONS
journal, October 2013

  • Jeong, Seongeun; Hsu, Ying-Kuang; Andrews, Arlyn E.
  • Journal of Geophysical Research: Atmospheres, Vol. 118, Issue 19
  • DOI: 10.1002/jgrd.50854

North American CO 2 exchange: inter-comparison of modeled estimates with results from a fine-scale atmospheric inversion
journal, January 2012


Inverse Methods for Atmospheric Sounding: Theory and Practice
book, July 2000

  • Rodgers, Clive D.
  • Series on Atmospheric, Oceanic and Planetary Physics, Vol. 2
  • DOI: 10.1142/3171

Global and regional emissions of HFC-125 (CHF 2 CF 3 ) from in situ and air archive atmospheric observations at AGAGE and SOGE observatories
journal, January 2009

  • O'Doherty, S.; Cunnold, D. M.; Miller, B. R.
  • Journal of Geophysical Research, Vol. 114, Issue D23
  • DOI: 10.1029/2009JD012184

Atmospheric inverse estimates of methane emissions from Central California
journal, January 2009

  • Zhao, Chuanfeng; Andrews, Arlyn E.; Bianco, Laura
  • Journal of Geophysical Research, Vol. 114, Issue D16
  • DOI: 10.1029/2008JD011671

Orthogonal distance regression
book, January 1990

  • Boggs, Paul T.; Rogers, Janet E.
  • Statistical Analysis of Measurement Error Models and Applications, Vol. 112
  • DOI: 10.1090/conm/112/1087109

An ensemble data assimilation system to estimate CO2 surface fluxes from atmospheric trace gas observations
journal, January 2005

  • Peters, W.; Miller, J. B.; Whitaker, J.
  • Journal of Geophysical Research, Vol. 110, Issue D24
  • DOI: 10.1029/2005JD006157

Characterization of uncertainties in atmospheric trace gas inversions using hierarchical Bayesian methods
journal, January 2014

  • Ganesan, A. L.; Rigby, M.; Zammit-Mangion, A.
  • Atmospheric Chemistry and Physics, Vol. 14, Issue 8
  • DOI: 10.5194/acp-14-3855-2014

High frequency measurements of HFCs at a remote site in east Asia and their implications for Chinese emissions
journal, January 2006

  • Yokouchi, Y.; Taguchi, S.; Saito, T.
  • Geophysical Research Letters, Vol. 33, Issue 21
  • DOI: 10.1029/2006GL026403

An atmospheric perspective on North American carbon dioxide exchange: CarbonTracker
journal, November 2007

  • Peters, W.; Jacobson, A. R.; Sweeney, C.
  • Proceedings of the National Academy of Sciences, Vol. 104, Issue 48
  • DOI: 10.1073/pnas.0708986104

Improving computational efficiency in large linear inverse problems: an example from carbon dioxide flux estimation
journal, January 2013


Emission profiles from the foam and refrigeration sectors comparison with atmospheric concentrations. Part 1: Methodology and data
journal, November 2004


Comparing atmospheric transport models for future regional inversions over Europe – Part 1: mapping the atmospheric CO<sub>2</sub> signals
journal, January 2007


Observations of HFC-134a in the remote troposphere
journal, January 1996

  • Montzka, S. A.; Myers, R. C.; Butler, J. H.
  • Geophysical Research Letters, Vol. 23, Issue 2
  • DOI: 10.1029/95GL03590

Corrigendum to "Global and regional emission estimates for HCFC-22", Atmos. Chem. Phys., 12, 10033–10050, 2012
journal, January 2014

  • Saikawa, E.; Rigby, M.; Prinn, R. G.
  • Atmospheric Chemistry and Physics, Vol. 14, Issue 10
  • DOI: 10.5194/acp-14-4857-2014

On aggregation errors in atmospheric transport inversions
journal, March 2001

  • Kaminski, Thomas; Rayner, Peter J.; Heimann, Martin
  • Journal of Geophysical Research: Atmospheres, Vol. 106, Issue D5
  • DOI: 10.1029/2000JD900581

Recent Trends in Global Emissions of Hydrochlorofluorocarbons and Hydrofluorocarbons: Reflecting on the 2007 Adjustments to the Montreal Protocol
journal, November 2014

  • Montzka, S. A.; McFarland, M.; Andersen, S. O.
  • The Journal of Physical Chemistry A, Vol. 119, Issue 19
  • DOI: 10.1021/jp5097376

A geostatistical approach to surface flux estimation of atmospheric trace gases
journal, January 2004

  • Michalak, Anna M.; Bruhwiler, Lori; Tans, Pieter P.
  • Journal of Geophysical Research, Vol. 109, Issue D14
  • DOI: 10.1029/2003JD004422

Results from the International Halocarbons in Air Comparison Experiment (IHALACE)
journal, January 2014

  • Hall, B. D.; Engel, A.; Mühle, J.
  • Atmospheric Measurement Techniques, Vol. 7, Issue 2
  • DOI: 10.5194/amt-7-469-2014

Present and future sources and emissions of halocarbons: Toward new constraints
journal, January 2007

  • Daniel, J. S.; Velders, G. J. M.; Solomon, S.
  • Journal of Geophysical Research, Vol. 112, Issue D2
  • DOI: 10.1029/2006JD007275

Seasonal variation of CH 4 emissions from central California : SEASONAL VARIATION OF CH
journal, June 2012

  • Jeong, Seongeun; Zhao, Chuanfeng; Andrews, Arlyn E.
  • Journal of Geophysical Research: Atmospheres, Vol. 117, Issue D11
  • DOI: 10.1029/2011JD016896

Present and future trends in the atmospheric burden of ozone-depleting halogens
journal, April 1999

  • Montzka, S. A.; Butler, J. H.; Elkins, J. W.
  • Nature, Vol. 398, Issue 6729
  • DOI: 10.1038/19499

Estimates of European emissions of methyl chloroform using a Bayesian inversion method
journal, January 2014

  • Maione, M.; Graziosi, F.; Arduini, J.
  • Atmospheric Chemistry and Physics, Vol. 14, Issue 18
  • DOI: 10.5194/acp-14-9755-2014

Atmospheric histories and global emissions of the anthropogenic hydrofluorocarbons HFC-365mfc, HFC-245fa, HFC-227ea, and HFC-236fa
journal, January 2011

  • Vollmer, Martin K.; Miller, Benjamin R.; Rigby, Matthew
  • Journal of Geophysical Research, Vol. 116, Issue D8
  • DOI: 10.1029/2010JD015309

High increase of global F-gas emissions until 2050
journal, June 2011

  • Gschrey, Barbara; Schwarz, Winfried; Elsner, Cornelia
  • Greenhouse Gas Measurement and Management, Vol. 1, Issue 2
  • DOI: 10.1080/20430779.2011.579352

Regional-scale geostatistical inverse modeling of North American CO 2 fluxes: a synthetic data study
journal, January 2010

  • Gourdji, S. M.; Hirsch, A. I.; Mueller, K. L.
  • Atmospheric Chemistry and Physics, Vol. 10, Issue 13
  • DOI: 10.5194/acp-10-6151-2010

The large contribution of projected HFC emissions to future climate forcing
journal, June 2009

  • Velders, G. J. M.; Fahey, D. W.; Daniel, J. S.
  • Proceedings of the National Academy of Sciences, Vol. 106, Issue 27
  • DOI: 10.1073/pnas.0902817106

Evaluation of Lagrangian Particle Dispersion Models with Measurements from Controlled Tracer Releases
journal, December 2013

  • Hegarty, Jennifer; Draxler, Roland R.; Stein, Ariel F.
  • Journal of Applied Meteorology and Climatology, Vol. 52, Issue 12
  • DOI: 10.1175/jamc-d-13-0125.1

Emission estimates of HCFCs and HFCs in California from the 2010 CalNex study: EMISSION ESTIMATES OF HCFCS AND HFCS IN CA
journal, February 2013

  • Barletta, Barbara; Carreras-Sospedra, Marc; Cohan, Alex
  • Journal of Geophysical Research: Atmospheres, Vol. 118, Issue 4
  • DOI: 10.1002/jgrd.50209

Releases of refrigerant gases (CFC-12, HCFC-22 and HFC-134a) to the atmosphere
journal, March 2003


Extension and integration of atmospheric carbon dioxide data into a globally consistent measurement record
journal, January 1995

  • Masarie, Kenneth A.; Tans, Pieter P.
  • Journal of Geophysical Research, Vol. 100, Issue D6
  • DOI: 10.1029/95JD00859

Emissions of HFC-134a from Light-Duty Vehicles in California
conference, May 2004

  • Vincent, Richard; Cleary, Kevin; Ayala, Alberto
  • Government/Industry Meeting, SAE Technical Paper Series
  • DOI: 10.4271/2004-01-2256

Global and regional emission estimates for HCFC-22
journal, January 2012


An improved Kalman Smoother for atmospheric inversions
journal, January 2005

  • Bruhwiler, L. M. P.; Michalak, A. M.; Peters, W.
  • Atmospheric Chemistry and Physics, Vol. 5, Issue 10
  • DOI: 10.5194/acp-5-2691-2005

An analytical inversion method for determining regional and global emissions of greenhouse gases: Sensitivity studies and application to halocarbons
journal, January 2009

  • Stohl, A.; Seibert, P.; Arduini, J.
  • Atmospheric Chemistry and Physics, Vol. 9, Issue 5
  • DOI: 10.5194/acp-9-1597-2009

A multi-year record of airborne CO 2 observations in the US Southern Great Plains
journal, January 2013

  • Biraud, S. C.; Torn, M. S.; Smith, J. R.
  • Atmospheric Measurement Techniques, Vol. 6, Issue 3
  • DOI: 10.5194/amt-6-751-2013

Seasonal variations in N 2 O emissions from central California : N
journal, August 2012

  • Jeong, Seongeun; Zhao, Chuanfeng; Andrews, Arlyn E.
  • Geophysical Research Letters, Vol. 39, Issue 16
  • DOI: 10.1029/2012GL052307

A multi-year record of airborne CO2 observations in the US Southern Great Plains
journal, January 2013


Estimates of European emissions of methyl chloroform using a Bayesian inversion method
journal, January 2014


Works referencing / citing this record:

Non-CO2 Greenhouse Gases
book, July 2017


CTDAS-Lagrange v1.0: a high-resolution data assimilation system for regional carbon dioxide observations
journal, January 2018

  • He, Wei; van der Velde, Ivar R.; Andrews, Arlyn E.
  • Geoscientific Model Development, Vol. 11, Issue 8
  • DOI: 10.5194/gmd-11-3515-2018

Abundance and sources of atmospheric halocarbons in the Eastern Mediterranean
journal, January 2018

  • Schoenenberger, Fabian; Henne, Stephan; Hill, Matthias
  • Atmospheric Chemistry and Physics, Vol. 18, Issue 6
  • DOI: 10.5194/acp-18-4069-2018

Accounting for the vertical distribution of emissions in atmospheric CO2 simulations
journal, January 2019

  • Brunner, Dominik; Kuhlmann, Gerrit; Marshall, Julia
  • Atmospheric Chemistry and Physics, Vol. 19, Issue 7
  • DOI: 10.5194/acp-19-4541-2019

Validation of the Swiss methane emission inventory by atmospheric observations and inverse modelling
journal, January 2016

  • Henne, Stephan; Brunner, Dominik; Oney, Brian
  • Atmospheric Chemistry and Physics, Vol. 16, Issue 6
  • DOI: 10.5194/acp-16-3683-2016

Enhanced North American carbon uptake associated with El Niño
journal, June 2019


Validation of the Swiss methane emission inventory by atmospheric observations and inverse modelling
journal, December 2015


CTDAS-Lagrange v1.0: A high-resolution data assimilation system for regional carbon dioxide observations
journal, December 2017

  • He, Wei; van der Velde, Ivar R.; Andrews, Arlyn E.
  • Geoscientific Model Development Discussions
  • DOI: 10.5194/gmd-2017-222

Validation of the Swiss methane emission inventory by atmospheric observations and inverse modelling
text, January 2016

  • Oney, Brian; Leuenberger, Markus; Meinhardt, Frank
  • European Geosciences Union
  • DOI: 10.7892/boris.83960

Accounting for the vertical distribution of emissions in atmospheric CO2 simulations
text, January 2019