Articles | Volume 18, issue 16
https://doi.org/10.5194/acp-18-11729-2018
© Author(s) 2018. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-18-11729-2018
© Author(s) 2018. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
17 Aug 2018
Research article |
| 17 Aug 2018
| 17 Aug 2018
Toward resolving the budget discrepancy of ozone-depleting carbon tetrachloride (CCl4): an analysis of top-down emissions from China
Department of Oceanography Kyungpook National University, Daegu 41566, Republic of Korea
Kyungpook Institute of Oceanography Kyungpook National University, Daegu 41566, Republic of Korea
Shanlan Li
Kyungpook Institute of Oceanography Kyungpook National University, Daegu 41566, Republic of Korea
Climate Research Division, National Institute of Meteorological Sciences, Seogwipo, Korea
Jens Mühle
Scripps Institution of Oceanography, University of California, San Diego, La Jolla, CA 92093, USA
Simon O'Doherty
School of Chemistry, University of Bristol, Bristol, UK
Ray F. Weiss
Scripps Institution of Oceanography, University of California, San Diego, La Jolla, CA 92093, USA
Xuekun Fang
Center for Global Change Science, Massachusetts Institute of Technology, Cambridge, MA 02139, USA
Stefan Reimann
Empa, Laboratory for Air Pollution and Environmental Technology, Swiss Federal Laboratories for Materials Science and Technology, Überlandstrasse 129, 8600 Dübendorf, Switzerland
Ronald G. Prinn
Center for Global Change Science, Massachusetts Institute of Technology, Cambridge, MA 02139, USA
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Martin Vojta, Andreas Plach, Saurabh Annadate, Sunyoung Park, Gawon Lee, Pallav Purohit, Florian Lindl, Xin Lan, Jens Mühle, Rona L. Thompson, and Andreas Stohl
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Haklim Choi, Alison L. Redington, Hyeri Park, Jooil Kim, Rona L. Thompson, Jens Mühle, Peter K. Salameh, Christina M. Harth, Ray F. Weiss, Alistair J. Manning, and Sunyoung Park
Atmos. Chem. Phys., 24, 7309–7330, https://doi.org/10.5194/acp-24-7309-2024, https://doi.org/10.5194/acp-24-7309-2024, 2024
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Hanqin Tian, Naiqing Pan, Rona L. Thompson, Josep G. Canadell, Parvadha Suntharalingam, Pierre Regnier, Eric A. Davidson, Michael Prather, Philippe Ciais, Marilena Muntean, Shufen Pan, Wilfried Winiwarter, Sönke Zaehle, Feng Zhou, Robert B. Jackson, Hermann W. Bange, Sarah Berthet, Zihao Bian, Daniele Bianchi, Alexander F. Bouwman, Erik T. Buitenhuis, Geoffrey Dutton, Minpeng Hu, Akihiko Ito, Atul K. Jain, Aurich Jeltsch-Thömmes, Fortunat Joos, Sian Kou-Giesbrecht, Paul B. Krummel, Xin Lan, Angela Landolfi, Ronny Lauerwald, Ya Li, Chaoqun Lu, Taylor Maavara, Manfredi Manizza, Dylan B. Millet, Jens Mühle, Prabir K. Patra, Glen P. Peters, Xiaoyu Qin, Peter Raymond, Laure Resplandy, Judith A. Rosentreter, Hao Shi, Qing Sun, Daniele Tonina, Francesco N. Tubiello, Guido R. van der Werf, Nicolas Vuichard, Junjie Wang, Kelley C. Wells, Luke M. Western, Chris Wilson, Jia Yang, Yuanzhi Yao, Yongfa You, and Qing Zhu
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Piers M. Forster, Chris Smith, Tristram Walsh, William F. Lamb, Robin Lamboll, Bradley Hall, Mathias Hauser, Aurélien Ribes, Debbie Rosen, Nathan P. Gillett, Matthew D. Palmer, Joeri Rogelj, Karina von Schuckmann, Blair Trewin, Myles Allen, Robbie Andrew, Richard A. Betts, Alex Borger, Tim Boyer, Jiddu A. Broersma, Carlo Buontempo, Samantha Burgess, Chiara Cagnazzo, Lijing Cheng, Pierre Friedlingstein, Andrew Gettelman, Johannes Gütschow, Masayoshi Ishii, Stuart Jenkins, Xin Lan, Colin Morice, Jens Mühle, Christopher Kadow, John Kennedy, Rachel E. Killick, Paul B. Krummel, Jan C. Minx, Gunnar Myhre, Vaishali Naik, Glen P. Peters, Anna Pirani, Julia Pongratz, Carl-Friedrich Schleussner, Sonia I. Seneviratne, Sophie Szopa, Peter Thorne, Mahesh V. M. Kovilakam, Elisa Majamäki, Jukka-Pekka Jalkanen, Margreet van Marle, Rachel M. Hoesly, Robert Rohde, Dominik Schumacher, Guido van der Werf, Russell Vose, Kirsten Zickfeld, Xuebin Zhang, Valérie Masson-Delmotte, and Panmao Zhai
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This paper tracks some key indicators of global warming through time, from 1850 through to the end of 2023. It is designed to give an authoritative estimate of global warming to date and its causes. We find that in 2023, global warming reached 1.3 °C and is increasing at over 0.2 °C per decade. This is caused by all-time-high greenhouse gas emissions.
Yiming Xu, Qianlai Zhuang, Bailu Zhao, Michael Billmire, Christopher Cook, Jeremy Graham, Nancy French, and Ronald Prinn
EGUsphere, https://doi.org/10.5194/egusphere-2024-1324, https://doi.org/10.5194/egusphere-2024-1324, 2024
Preprint archived
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We use a process-based model to simulate the fire impacts on soil thermal and hydrological dynamics and carbon budget of forest ecosystems in Northern Eurasia based on satellite-derived burn severity data. We find that fire severity generally increases in this region during the study period. Simulations indicate that fires increase soil temperature and water runoff. Fires lead the forest ecosystems to lose 2.3 Pg C, shifting the forests from a carbon sink to a source in this period.
Emily Dowd, Alistair J. Manning, Bryn Orth-Lashley, Marianne Girard, James France, Rebecca E. Fisher, Dave Lowry, Mathias Lanoisellé, Joseph R. Pitt, Kieran M. Stanley, Simon O'Doherty, Dickon Young, Glen Thistlethwaite, Martyn P. Chipperfield, Emanuel Gloor, and Chris Wilson
Atmos. Meas. Tech., 17, 1599–1615, https://doi.org/10.5194/amt-17-1599-2024, https://doi.org/10.5194/amt-17-1599-2024, 2024
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We provide the first validation of the satellite-derived emission estimates using surface-based mobile greenhouse gas surveys of an active gas leak detected near Cheltenham, UK. GHGSat’s emission estimates broadly agree with the surface-based mobile survey and steps were taken to fix the leak, highlighting the importance of satellite data in identifying emissions and helping to reduce our human impact on climate change.
Rona L. Thompson, Stephen A. Montzka, Martin K. Vollmer, Jgor Arduini, Molly Crotwell, Paul B. Krummel, Chris Lunder, Jens Mühle, Simon O'Doherty, Ronald G. Prinn, Stefan Reimann, Isaac Vimont, Hsiang Wang, Ray F. Weiss, and Dickon Young
Atmos. Chem. Phys., 24, 1415–1427, https://doi.org/10.5194/acp-24-1415-2024, https://doi.org/10.5194/acp-24-1415-2024, 2024
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The hydroxyl radical determines the atmospheric lifetimes of numerous species including methane. Since OH is very short-lived, it is not possible to directly measure its concentration on scales relevant for understanding its effect on other species. Here, OH is inferred by looking at changes in hydrofluorocarbons (HFCs). We find that OH levels have been fairly stable over our study period (2004 to 2021), suggesting that OH is not the main driver of the recent increase in atmospheric methane.
Ioannis Katharopoulos, Dominique Rust, Martin K. Vollmer, Dominik Brunner, Stefan Reimann, Simon J. O'Doherty, Dickon Young, Kieran M. Stanley, Tanja Schuck, Jgor Arduini, Lukas Emmenegger, and Stephan Henne
Atmos. Chem. Phys., 23, 14159–14186, https://doi.org/10.5194/acp-23-14159-2023, https://doi.org/10.5194/acp-23-14159-2023, 2023
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The effectiveness of climate change mitigation needs to be scrutinized by monitoring greenhouse gas (GHG) emissions. Countries report their emissions to the UN in a bottom-up manner. By combining atmospheric observations and transport models someone can independently validate emission estimates in a top-down fashion. We report Swiss emissions of synthetic GHGs based on kilometer-scale transport and inverse modeling, highlighting the role of appropriate resolution in complex terrain.
Hyeri Park, Jooil Kim, Haklim Choi, Sohyeon Geum, Yeaseul Kim, Rona L. Thompson, Jens Mühle, Peter K. Salameh, Christina M. Harth, Kieran M. Stanley, Simon O'Doherty, Paul J. Fraser, Peter G. Simmonds, Paul B. Krummel, Ray F. Weiss, Ronald G. Prinn, and Sunyoung Park
Atmos. Chem. Phys., 23, 9401–9411, https://doi.org/10.5194/acp-23-9401-2023, https://doi.org/10.5194/acp-23-9401-2023, 2023
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Based on atmospheric HFC-23 observations, the first estimate of post-CDM HFC-23 emissions in eastern Asia for 2008–2019 shows that these emissions contribute significantly to the global emissions rise. The observation-derived emissions were much larger than the bottom-up estimates expected to approach zero after 2015 due to national abatement activities. These discrepancies could be attributed to unsuccessful factory-level HFC-23 abatement and inaccurate quantification of emission reductions.
Alison L. Redington, Alistair J. Manning, Stephan Henne, Francesco Graziosi, Luke M. Western, Jgor Arduini, Anita L. Ganesan, Christina M. Harth, Michela Maione, Jens Mühle, Simon O'Doherty, Joseph Pitt, Stefan Reimann, Matthew Rigby, Peter K. Salameh, Peter G. Simmonds, T. Gerard Spain, Kieran Stanley, Martin K. Vollmer, Ray F. Weiss, and Dickon Young
Atmos. Chem. Phys., 23, 7383–7398, https://doi.org/10.5194/acp-23-7383-2023, https://doi.org/10.5194/acp-23-7383-2023, 2023
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Chlorofluorocarbons (CFCs) were used in Europe pre-1990, damaging the stratospheric ozone layer. Legislation has controlled production and use, and global emissions have decreased sharply. The global rate of decline in CFC-11 recently slowed and was partly attributed to illegal emission in eastern China. This study concludes that emissions of CFC-11 in western Europe have not contributed to the unexplained part of the global increase in CFC-11 observed in the last decade.
Elena Fillola, Raul Santos-Rodriguez, Alistair Manning, Simon O'Doherty, and Matt Rigby
Geosci. Model Dev., 16, 1997–2009, https://doi.org/10.5194/gmd-16-1997-2023, https://doi.org/10.5194/gmd-16-1997-2023, 2023
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Lagrangian particle dispersion models are used extensively for the estimation of greenhouse gas (GHG) fluxes using atmospheric observations. However, these models do not scale well as data volumes increase. Here, we develop a proof-of-concept machine learning emulator that can produce outputs similar to those of the dispersion model, but 50 000 times faster, using only meteorological inputs. This works demonstrates the potential of machine learning to accelerate GHG estimations across the globe.
Michael N. Dyonisius, Vasilii V. Petrenko, Andrew M. Smith, Benjamin Hmiel, Peter D. Neff, Bin Yang, Quan Hua, Jochen Schmitt, Sarah A. Shackleton, Christo Buizert, Philip F. Place, James A. Menking, Ross Beaudette, Christina Harth, Michael Kalk, Heidi A. Roop, Bernhard Bereiter, Casey Armanetti, Isaac Vimont, Sylvia Englund Michel, Edward J. Brook, Jeffrey P. Severinghaus, Ray F. Weiss, and Joseph R. McConnell
The Cryosphere, 17, 843–863, https://doi.org/10.5194/tc-17-843-2023, https://doi.org/10.5194/tc-17-843-2023, 2023
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Cosmic rays that enter the atmosphere produce secondary particles which react with surface minerals to produce radioactive nuclides. These nuclides are often used to constrain Earth's surface processes. However, the production rates from muons are not well constrained. We measured 14C in ice with a well-known exposure history to constrain the production rates from muons. 14C production in ice is analogous to quartz, but we obtain different production rates compared to commonly used estimates.
Peter Bergamaschi, Arjo Segers, Dominik Brunner, Jean-Matthieu Haussaire, Stephan Henne, Michel Ramonet, Tim Arnold, Tobias Biermann, Huilin Chen, Sebastien Conil, Marc Delmotte, Grant Forster, Arnoud Frumau, Dagmar Kubistin, Xin Lan, Markus Leuenberger, Matthias Lindauer, Morgan Lopez, Giovanni Manca, Jennifer Müller-Williams, Simon O'Doherty, Bert Scheeren, Martin Steinbacher, Pamela Trisolino, Gabriela Vítková, and Camille Yver Kwok
Atmos. Chem. Phys., 22, 13243–13268, https://doi.org/10.5194/acp-22-13243-2022, https://doi.org/10.5194/acp-22-13243-2022, 2022
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We present a novel high-resolution inverse modelling system, "FLEXVAR", and its application for the inverse modelling of European CH4 emissions in 2018. The new system combines a high spatial resolution of 7 km x 7 km with a variational data assimilation technique, which allows CH4 emissions to be optimized from individual model grid cells. The high resolution allows the observations to be better reproduced, while the derived emissions show overall good consistency with two existing models.
Angharad C. Stell, Michael Bertolacci, Andrew Zammit-Mangion, Matthew Rigby, Paul J. Fraser, Christina M. Harth, Paul B. Krummel, Xin Lan, Manfredi Manizza, Jens Mühle, Simon O'Doherty, Ronald G. Prinn, Ray F. Weiss, Dickon Young, and Anita L. Ganesan
Atmos. Chem. Phys., 22, 12945–12960, https://doi.org/10.5194/acp-22-12945-2022, https://doi.org/10.5194/acp-22-12945-2022, 2022
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Nitrous oxide is a potent greenhouse gas and ozone-depleting substance, whose atmospheric abundance has risen throughout the contemporary record. In this work, we carry out the first global hierarchical Bayesian inversion to solve for nitrous oxide emissions. We derive increasing global nitrous oxide emissions over 2011–2020, which are mainly driven by emissions between 0° and 30°N, with the highest emissions recorded in 2020.
Megan Jeramaz Lickley, John S. Daniel, Eric L. Fleming, Stefan Reimann, and Susan Solomon
Atmos. Chem. Phys., 22, 11125–11136, https://doi.org/10.5194/acp-22-11125-2022, https://doi.org/10.5194/acp-22-11125-2022, 2022
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Halocarbons contained in equipment continue to be emitted after production has ceased. These
banksmust be carefully accounted for in evaluating compliance with the Montreal Protocol. We extend a Bayesian model to the suite of regulated chemicals subject to banking. We find that banks are substantially larger than previous estimates, and we identify banks by chemical and equipment type whose future emissions will contribute to global warming and delay ozone-hole recovery if left unrecovered.
Luke M. Western, Alison L. Redington, Alistair J. Manning, Cathy M. Trudinger, Lei Hu, Stephan Henne, Xuekun Fang, Lambert J. M. Kuijpers, Christina Theodoridi, David S. Godwin, Jgor Arduini, Bronwyn Dunse, Andreas Engel, Paul J. Fraser, Christina M. Harth, Paul B. Krummel, Michela Maione, Jens Mühle, Simon O'Doherty, Hyeri Park, Sunyoung Park, Stefan Reimann, Peter K. Salameh, Daniel Say, Roland Schmidt, Tanja Schuck, Carolina Siso, Kieran M. Stanley, Isaac Vimont, Martin K. Vollmer, Dickon Young, Ronald G. Prinn, Ray F. Weiss, Stephen A. Montzka, and Matthew Rigby
Atmos. Chem. Phys., 22, 9601–9616, https://doi.org/10.5194/acp-22-9601-2022, https://doi.org/10.5194/acp-22-9601-2022, 2022
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The production of ozone-destroying gases is being phased out. Even though production of one of the main ozone-depleting gases, called HCFC-141b, has been declining for many years, the amount that is being released to the atmosphere has been increasing since 2017. We do not know for sure why this is. A possible explanation is that HCFC-141b that was used to make insulating foams many years ago is only now escaping to the atmosphere, or a large part of its production is not being reported.
Guus J. M. Velders, John S. Daniel, Stephen A. Montzka, Isaac Vimont, Matthew Rigby, Paul B. Krummel, Jens Muhle, Simon O'Doherty, Ronald G. Prinn, Ray F. Weiss, and Dickon Young
Atmos. Chem. Phys., 22, 6087–6101, https://doi.org/10.5194/acp-22-6087-2022, https://doi.org/10.5194/acp-22-6087-2022, 2022
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The emissions of hydrofluorocarbons (HFCs) have increased significantly in the past as a result of the phasing out of ozone-depleting substances. Observations indicate that HFCs are used much less in certain refrigeration applications than previously projected. Current policies are projected to reduce emissions and the surface temperature contribution of HFCs from 0.28–0.44 °C to 0.14–0.31 °C in 2100. The Kigali Amendment is projected to reduce the contributions further to 0.04 °C in 2100.
Haklim Choi, Mi-Kyung Park, Paul J. Fraser, Hyeri Park, Sohyeon Geum, Jens Mühle, Jooil Kim, Ian Porter, Peter K. Salameh, Christina M. Harth, Bronwyn L. Dunse, Paul B. Krummel, Ray F. Weiss, Simon O'Doherty, Dickon Young, and Sunyoung Park
Atmos. Chem. Phys., 22, 5157–5173, https://doi.org/10.5194/acp-22-5157-2022, https://doi.org/10.5194/acp-22-5157-2022, 2022
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We observed 12-year continuous CH3Br pollution signals at Gosan and estimated anthropogenic CH3Br emissions in eastern China. The analysis revealed a significant discrepancy between top-down estimates and the bottom-up emissions from the fumigation usage reported to the United Nations Environment Programme, likely due to unreported or inaccurately reported fumigation usage. This result provides information to monitor international compliance with the Montreal Protocol.
Alice E. Ramsden, Anita L. Ganesan, Luke M. Western, Matthew Rigby, Alistair J. Manning, Amy Foulds, James L. France, Patrick Barker, Peter Levy, Daniel Say, Adam Wisher, Tim Arnold, Chris Rennick, Kieran M. Stanley, Dickon Young, and Simon O'Doherty
Atmos. Chem. Phys., 22, 3911–3929, https://doi.org/10.5194/acp-22-3911-2022, https://doi.org/10.5194/acp-22-3911-2022, 2022
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Quantifying methane emissions from different sources is a key focus of current research. We present a method for estimating sectoral methane emissions that uses ethane as a tracer for fossil fuel methane. By incorporating variable ethane : methane emission ratios into this model, we produce emissions estimates with improved uncertainty characterisation. This method will be particularly useful for studying methane emissions in areas with complex distributions of sources.
Jens Mühle, Lambert J. M. Kuijpers, Kieran M. Stanley, Matthew Rigby, Luke M. Western, Jooil Kim, Sunyoung Park, Christina M. Harth, Paul B. Krummel, Paul J. Fraser, Simon O'Doherty, Peter K. Salameh, Roland Schmidt, Dickon Young, Ronald G. Prinn, Ray H. J. Wang, and Ray F. Weiss
Atmos. Chem. Phys., 22, 3371–3378, https://doi.org/10.5194/acp-22-3371-2022, https://doi.org/10.5194/acp-22-3371-2022, 2022
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Emissions of the strong greenhouse gas perfluorocyclobutane (c-C4F8) into the atmosphere have been increasing sharply since the early 2000s. These c-C4F8 emissions are highly correlated with the amount of hydrochlorofluorocarbon-22 produced to synthesize polytetrafluoroethylene (known for its non-stick properties) and related chemicals. From this process, c-C4F8 by-product is vented to the atmosphere. Avoiding these unnecessary c-C4F8 emissions could reduce the climate impact of this industry.
Dominique Rust, Ioannis Katharopoulos, Martin K. Vollmer, Stephan Henne, Simon O'Doherty, Daniel Say, Lukas Emmenegger, Renato Zenobi, and Stefan Reimann
Atmos. Chem. Phys., 22, 2447–2466, https://doi.org/10.5194/acp-22-2447-2022, https://doi.org/10.5194/acp-22-2447-2022, 2022
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Artificial halocarbons contribute to ozone layer depletion and to global warming. We measured the atmospheric concentrations of halocarbons at the Beromünster tower, modelled the Swiss emissions, and compared the results to the internationally reported Swiss emissions inventory. For most of the halocarbons, we found good agreement, whereas one refrigerant might be overestimated in the inventory. In addition, we present first emission estimates of the newest types of halocarbons.
Mark F. Lunt, Alistair J. Manning, Grant Allen, Tim Arnold, Stéphane J.-B. Bauguitte, Hartmut Boesch, Anita L. Ganesan, Aoife Grant, Carole Helfter, Eiko Nemitz, Simon J. O'Doherty, Paul I. Palmer, Joseph R. Pitt, Chris Rennick, Daniel Say, Kieran M. Stanley, Ann R. Stavert, Dickon Young, and Matt Rigby
Atmos. Chem. Phys., 21, 16257–16276, https://doi.org/10.5194/acp-21-16257-2021, https://doi.org/10.5194/acp-21-16257-2021, 2021
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We present an evaluation of the UK's methane emissions between 2013 and 2020 using a network of tall tower measurement sites. We find emissions that are consistent in both magnitude and trend with the UK's reported emissions, with a declining trend driven by a decrease in emissions from England. The impact of various components of the modelling set-up on these findings are explored through a number of sensitivity studies.
Masanori Takeda, Hideaki Nakajima, Isao Murata, Tomoo Nagahama, Isamu Morino, Geoffrey C. Toon, Ray F. Weiss, Jens Mühle, Paul B. Krummel, Paul J. Fraser, and Hsiang-Jui Wang
Atmos. Meas. Tech., 14, 5955–5976, https://doi.org/10.5194/amt-14-5955-2021, https://doi.org/10.5194/amt-14-5955-2021, 2021
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This paper presents the first observations of atmospheric HFC-23 abundances with a ground-based remote sensing technique. The increasing trend of the HFC-23 abundances analyzed by this study agrees with that derived from other existing in situ measurements. This study indicates that ground-based FTIR observation has the capability to monitor the trend of atmospheric HFC-23 and could allow for monitoring the distribution of global atmospheric HFC-23 abundances in more detail.
Alistair J. Manning, Alison L. Redington, Daniel Say, Simon O'Doherty, Dickon Young, Peter G. Simmonds, Martin K. Vollmer, Jens Mühle, Jgor Arduini, Gerard Spain, Adam Wisher, Michela Maione, Tanja J. Schuck, Kieran Stanley, Stefan Reimann, Andreas Engel, Paul B. Krummel, Paul J. Fraser, Christina M. Harth, Peter K. Salameh, Ray F. Weiss, Ray Gluckman, Peter N. Brown, John D. Watterson, and Tim Arnold
Atmos. Chem. Phys., 21, 12739–12755, https://doi.org/10.5194/acp-21-12739-2021, https://doi.org/10.5194/acp-21-12739-2021, 2021
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This paper estimates UK emissions of important greenhouse gases (hydrofluorocarbons (HFCs)) using high-quality atmospheric observations and atmospheric modelling. We compare these estimates with those submitted by the UK to the United Nations. We conclude that global concentrations of these gases are still increasing. Our estimates for the UK are 73 % of those reported and that the UK emissions are now falling, demonstrating an impact of UK government policy.
Ruth E. Hill-Pearce, Aimee Hillier, Eric Mussell Webber, Kanokrat Charoenpornpukdee, Simon O'Doherty, Joachim Mohn, Christoph Zellweger, David R. Worton, and Paul J. Brewer
Atmos. Meas. Tech., 14, 5447–5458, https://doi.org/10.5194/amt-14-5447-2021, https://doi.org/10.5194/amt-14-5447-2021, 2021
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There is currently a need for gas reference materials with well-characterised delta values for monitoring N2O amount fractions. We present work towards the preparation of gas reference materials for calibration of in-field monitoring equipment, which target the WMO-GAW data quality objectives for comparability of amount fraction and demonstrate the stability of δ15Nα, δ15Nβ and δ18O values with pressure and effects of cylinder passivation.
Daniel Say, Alistair J. Manning, Luke M. Western, Dickon Young, Adam Wisher, Matthew Rigby, Stefan Reimann, Martin K. Vollmer, Michela Maione, Jgor Arduini, Paul B. Krummel, Jens Mühle, Christina M. Harth, Brendan Evans, Ray F. Weiss, Ronald G. Prinn, and Simon O'Doherty
Atmos. Chem. Phys., 21, 2149–2164, https://doi.org/10.5194/acp-21-2149-2021, https://doi.org/10.5194/acp-21-2149-2021, 2021
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Perfluorocarbons (PFCs) are potent greenhouse gases with exceedingly long lifetimes. We used atmospheric measurements from a global monitoring network to track the accumulation of these gases in the atmosphere. In the case of the two most abundant PFCs, recent measurements indicate that global emissions are increasing. In Europe, we used a model to estimate regional PFC emissions. Our results show that there was no significant decline in northwest European PFC emissions between 2010 and 2019.
Rachel L. Tunnicliffe, Anita L. Ganesan, Robert J. Parker, Hartmut Boesch, Nicola Gedney, Benjamin Poulter, Zhen Zhang, Jošt V. Lavrič, David Walter, Matthew Rigby, Stephan Henne, Dickon Young, and Simon O'Doherty
Atmos. Chem. Phys., 20, 13041–13067, https://doi.org/10.5194/acp-20-13041-2020, https://doi.org/10.5194/acp-20-13041-2020, 2020
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This study quantifies Brazil’s emissions of a potent atmospheric greenhouse gas, methane. This is in the field of atmospheric modelling and uses remotely sensed data and surface measurements of methane concentrations as well as an atmospheric transport model to interpret the data. Because of Brazil’s large emissions from wetlands, agriculture and biomass burning, these emissions affect global methane concentrations and thus are of global significance.
Cited articles
An, X. Q., Henne, S., Yao, B., Vollmer, M. K., Zhou, L. X., and Li Y.: Estimating
emissions of HCFC-22 and CFC-11 in China by atmospheric observations and inverse
modeling, Sci. China Chem., 55, 10, 2233–2241, https://doi.org/10.1007/s11426-012-4624-8, 2012.
Bie P., Fang X., Li Z., and Hu J.: Emissions estimates of carbon tetrachloride
for 1992–2014 in China, Environ. Poll., 224, 670–678, https://doi.org/10.1016/j.envpol.2017.02.051, 2017.
Blake, N. J., Streets, D. G., Woo, J. H., Simpson, I. J., Green, J., Meinardi,
S., Kita, K., Atlas, E., Fuelberg, H. E., Sachse, G., Avery, M. A., Vay, S. A.,
Talbot, R. W., Dibb, J. E., Bandy, A. R., Thornton, D. C., Rowland, F. S., and
Blake, D. R.: Carbonyl sulfide and carbon disulfide: Large-scale distributions
over the western Pacific and emissions from Asia during TRACE-P, J. Geophys.
Res., 109, D15S05, https://doi.org/10.1029/2003JD004259, 2004.
Butler, J. H., Yvon-Lewis, S. A., Lobert, J. M., King, D. B., Montzka, S. A.,
Bullister, J. L., Koropalov, V., Elkins, J. W., Hall, B. D., Hu, L., and Liu,
Y.: A comprehensive estimate for loss of atmospheric carbon tetrachloride (CCl4)
to the ocean, Atmos. Chem. Phys., 16, 10899–10910, https://doi.org/10.5194/acp-16-10899-2016, 2016.
Cantrell, C. A.: Technical Note: Review of methods for linear least-squares
fitting of data and application to atmospheric chemistry problems, Atmos. Chem.
Phys., 8, 5477–5487, https://doi.org/10.5194/acp-8-5477-2008, 2008.
Carpenter, L. J., Reimann, S., Burkholder, J. B., Clerbaux, C., Hall, B. D.,
Hossaini, R., Laube, J. C., and Yvon-Lewis, S. A.: Ozone-Depleting Substances (ODSs)
and other gases of interest to the Montreal Protocol, in: Scientific Assessment
of Ozone Depletion: 2014, Global Ozone Research and monitoring Project, Report
No. 55, World Meteorological Organization, Geneva, Switzerland, 2014.
Choi, E., Heo, J. B., and Yi, S. M.: Apportioning and locating nonmethane
hydrocarbon sources to a background site in Korea, Environ. Sci. Technol.,
44, 5849–5854, https://doi.org/10.1021/es903634e, 2010.
Fang, X., Wu, J., Su, S., Han, J., Wu, Y., Shi, Y., Wan, D., Sun, X., Zhang,
J., and Hu, J.: Estimates of major anthropogenic halocarbon emissions from
China based on interspecies correlations, Atmos. Environ., 62, 26–33,
https://doi.org/10.1016/j.atmosenv.2012.08.010, 2012.
Fang, X., Thompson, R. L., Saito, T., Yokouchi, Y., Kim, J., Li, S., Kim, K. R.,
Park, S., Graziosi, F., and Stohl, A.: Sulfur hexafluoride (SF6)
emissions in East Asia determined by inverse modeling, Atmos. Chem. Phys.,
14, 4779–4791, https://doi.org/10.5194/acp-14-4779-2014, 2014.
Fang, X., Stohl, A., Yokouchi, Y., Kim, J., Li, S., Saito, T., Park, S., and Hu,
J.: Multiannual top-down estimate of HFC-23 emissions in East Asia, Environ.
Sci. Technol., 49, 4345–4353, https://doi.org/10.1021/es505669j, 2015.
Fraser, P., Dunse, B., Manning, A., Wang, R., Krummel, P., Steele, P., Porter,
L., Allison, C., O'Doherty, S., Simmonds, P., Mühle, J., and Prinn, R.:
Australian carbon tetrachloride (CCl4) emissions in a global context,
Environ. Chem., 11, 77–88, https://doi.org/10.1071/EN13171, 2014.
Graziosi, F., Arduini, J., Bonasoni, P., Furlani, F., Giostra, U.,
Hermanssen, O., Lunder, C., Manning, A. J., McCulloch, A., O'Doherty, S. J.,
Reimann, S., Vollmer, M. K., Maione, M.: Emissions of carbon tetrachloride (CCl4)
from Europe, Atmos. Chem. Phys., 16, 12849–12859, https://doi.org/10.5194/acp-16-12849-2016, 2016.
Guo, H., Ding, A. J., Wang, T., Simpson, I. J., Blake, D. R., Barletta, B.,
Meinardi, S., Rowland, F. S., Saunders, S. M., Fu, T. M., Hung, W. T., and Li,
Y. S.: Source origins, modeled profiles, and apportionments of halogenated
hydrocarbons in the greater Pearl River Delta region, southern China, J. Geophys.
Res.-Atmos., 114, D11302, https://doi.org/10.1029/2008JD011448, 2009.
Hu, L., Montzka, S. A., Miller, B. R., Andrews, A. E., Miller, J. B., Lehman,
S. J., Sweeney, C., Miller, S., Thoning, K., Siso, C., Atlas, E., Blake, D.,
de Gouw, J. A., Gilman, J. B., Dutton, G., Elkins, J. W., Hall, B. D., Chen, H.,
Fischer, M. L., Mountain, M., Nehrkorn, T., Biraud, S. C., Moore, F., and Tans,
P. P.: Continued emissions of carbon tetrachloride from the U.S. nearly two
decades after its phase-out for dispersive uses, P. Natl. Acad. Sci. USA, 113,
2880–2885, https://doi.org/10.1073/pnas.1522284113, 2016.
Kim, J., Li, S., Kim, K. R., Stohl, A., Muhle, J., Kim, S. K., Park, M. K.,
Kang, D. J., Lee, G., Harth, C. M., Salameh, P. K., and Weiss, R. F.: Regional
atmospheric emissions determined from measurements at Jeju Island, Korea:
Halogenated compounds from China, Geophys. Res. Lett., 37, L12801, https://doi.org/10.1029/2010GL043263, 2010.
Kim, J., Li, S., Mühle, J., Stohl, A., Kim, S. K., Park, S., Park, M. K.,
Weiss, R. F., Kim, K. R.: Overview of the findings from measurements of
halogenated compounds at Gosan (Jeju Island, Korea) quantifying emissions in
East Asia, J. Integrat. Environ. Sci., 9, 71–80, https://doi.org/10.1080/1943815X.2012.696548, 2012.
Lanz, V. A., Henne, S., Staehelin, J., Hueglin, C., Vollmer, M. K., Steinbacher,
M., Buchmann, B., and Reimann, S.: Statistical analysis of anthropogenic
non-methane VOC variability at a European background location (Jungfraujoch,
Switzerland), Atmos. Chem. Phys., 9, 3445–3459, https://doi.org/10.5194/acp-9-3445-2009, 2009.
Li, S., Kim, J., and Kim, K. R.: Emissions of halogenated compounds in East Asia
determined from measurements at Jeju Island, Korea, Environ. Sci. Technol.,
45, 5668–5675, https://doi.org/10.1021/es104124k, 2011.
Li, S., Kim, J., Park, S., Kim, S. K., Park, M. K., Mühle, J., Lee, G.,
Lee, M., Jo, C. O., and Kim, K. R.: Source identification and apportionment of
halogenated compounds observed at a remote site in East Asia, Environ. Sci.
Technol., 48, 491–498, https://doi.org/10.1021/es402776w, 2014.
Li, S., Park, M. K., Jo, C. O., and Park, S. J.: Emission estimates of methyl
chloride from industrial sources in China based on high frequency atmospheric
observations, J. Atmos. Chem., 74, 227–243, https://doi.org/10.1007/s10874-016-9354-4, 2017.
Li, X., Wang, S., Duan, L., and Hao, J.: Characterization of non-methane
hydrocarbons emitted from open burning of wheat straw and corn stover in China,
Environ. Res. Lett., 4, 044015, https://doi.org/10.1088/1748-9326/4/4/044015, 2009.
Liang, Q., Newman, P. A., Daniel, J. S., Reimann, S., Hall, B. D., Dutton, G.,
and Kuijpers L. J. M.: Constraining the carbon tetrachloride (CCl4)
budget using its global trend and inter-hemispheric gradient, Geophys. Res.
Lett., 41, 5307–5315, https://doi.org/10.1002/2014GL060754, 2014.
Liang, Q. Newman, P. A., and Reimann, S. (Eds.): SPARC Report on the Mystery
of Carbon Tetrachloride, SPARC Report No. 7, WCRP-13/2016, available at:
http://www.sparc-climate.org/publications/sparc-reports/sparc-report-no7
(last access: July 2018), 2016.
Miller, B. R., Weiss, R. F., Salameh, P. K., Tanhua, T., Greally, B. R.,
Mühle, J., and Simmonds, P. G.: Medusa: A sample preconcentration and GC/MS
detector system for in situ measurements of atmospheric trace halocarbons,
hydrocarbons, and sulfur compounds, Anal. Chem., 80, 1536–1545, https://doi.org/10.1021/ac702084k, 2008.
Montzka, S. A. and Reimann S.: Ozone-Depleting Substances 1.90 (ODSs) and
related chemicals, Chapter 1 in Scientific Assessment of Ozone Depletion: 2010,
Global Ozone Research and Monitoring Project, Report No. 52, World Meteorological
Organization, Geneva, Switzerland, 2011.
O'Doherty, S., Simmonds, P. G., Cunnold, D. M., Wang, H. J., Sturrock, G. A.,
Fraser, P. J., Ryall, D., Derwent, R. G., Weiss, R. F., Salameh, P., Miller,
B. R., and Prinn, R. G.: In situ chloroform measurements at Advanced Global
Atmospheric Gases Experiment atmospheric research stations from 1994 to 1998,
J. Geophys. Res.-Atmos., 106, 20429–20444, https://doi.org/10.1029/2000JD900792, 2001.
Paatero, P. and Tapper, U.: Positive matrix factorization: A non-negative factor
model with optimal utilization of error estimates of data values, Environmetrics,
5, 111–126, https://doi.org/10.1002/env.3170050203, 1994.
Palmer P. I., Jacob, D. J., Mickley, L. J., Blake, D. R., Sachse, G. W.,
Fuelberg, H. E., and Kiley, C. M.: Eastern Asian emissions of anthropogenic
halocarbons deduced from aircraft concentration data, J. Geophys. Res., 108,
4753, https://doi.org/10.1029/2003JD003591, 2003.
Poirot, R. L. and Wishinski, P. R.: Visibility, sulfate and air-mass history
associated with the summertime aerosol in northern Vermont, Atmos. Environ.,
20, 1457–1469, https://doi.org/10.1016/0004-6981(86)90018-1, 1986.
Reff, A., Eberly, S. I., and Bhave, P. V.: Receptor modeling of ambient
particulate matter data using positive matrix factorization: review of existing
methods, J. Air Waste Manage. Assoc., 57, 146–154, https://doi.org/10.1080/10473289.2007.10465319, 2007.
Reimann S., Schaub, D., Stemmler, K., Folini, D., Hill, M., Hofer, P., Buchmann,
B., Simmonds, P. G., Greally, B. R., and O'Doherty, S.: Halogenated greenhouse
gases at the Swiss High Alpine Site of Jungfraujoch (3580 m asl): Continuous
measurements and their use for regional European source allocation, J. Geophys.
Res., 109, D05307J, https://doi.org/10.1029/2003JD003923, 2004.
Rhew, R. C. and Happell, J. D.: The atmospheric partial lifetime of carbon
tetrachloride with respect to the global soil sink, Geophys. Res. Lett., 43,
2889–2895, https://doi.org/10.1002/2016GL067839, 2016.
Seibert, P., Kromp-Kolb, H., Baltensperger, U., Jost, D. T., and Schwikowski,
M.: Trajectory analysis of aerosol measurements at high Apline sites, in:
Transport and transformation of pollutants in the troposphere, edited by:
Borrell, P. M., Cvitaš, T., and Seiler, W., Academic Publishing, Den Haag, 689–693, 1994.
Sherry, D., McCulloch, A., Liang, Q., Reimann, S., and Newman, P. A.: Current
sources of carbon tetrachloride in our atmosphere, Environ. Res. Lett., 13,
024004, https://doi.org/10.1088/1748-9326/aa9c87, 2018.
Stohl, A.: Trajectory statistics: A new method to establish source receptor
relationships of air pollutants and its application to the transport of
particulate sulfate in Europe, Atmos. Environ., 30, 4, 579–587, https://doi.org/10.1016/1352-2310(95)00314-2, 1996.
Stohl, A., Kim, J., Li, S., O'Doherty, S., Mühle, J., Salameh, P. K., Saito,
T., Vollmer, M. K., Wan, D., Weiss, R. F., Yao, B., Yokouchi, Y., and Zhou, L.
X.: Hydrochlorofluorocarbon and hydrofluorocarbon emissions in East Asia
determined by inverse modeling, Atmos. Chem. Phys., 10, 3545–3560, https://doi.org/10.5194/acp-10-3545-2010, 2010.
Wan, D., Xu, J., Zhang, J., Tong, X., and Hu, J.: Historical and projected
emissions of major halocarbons in China, Atmos. Environ., 43, 5822–5829,
https://doi.org/10.1016/j.atmosenv.2009.07.052, 2009.
Wang, C., Shao, M., Huang, D., Sihua, L., Zeng, L., Hu, M., and Zhang, Q.:
Estimating halocarbon emissions using measured ratio relative to tracers in
China, Atmos. Environ., 89, 816–826, https://doi.org/10.1016/j.atmosenv.2014.03.025, 2014.
UNEP – United Nations Environment Programme: Ozone Secretariat Data Access
Centre, http://ozone.unep.org/reporting/ (last access: 11 February 2018), 2009.
Zhang, Y. L., Guo, H., Wang, X. M., Simpson, I. J., Barletta, B., Blake, D. R.,
Meinardi, S., Rowland, F. S., Cheng, H. R., Saunders, S. M., and Lam, S. H. M.:
Emission patterns and spatiotemporal variations of halocarbons in the Pearl
River Delta region, southern China, J. Geophys. Res., 115, D15309, https://doi.org/10.1029/2009JD013726, 2010.
Short summary
Multi-year, real-time atmospheric carbon tetrachloride (CCl4) record obtained at Gosan station (33° N, 126° E) presents evidence of significant unreported emissions of this first-generation ozone-depleting substance. The missing emissions (~ 19 Gg yr−1) for China contribute to approximately 54 % of global emissions and are most likely related to CCl4 escape occurring during the production of chlorinated compounds and their usage as feedstocks and process agents in chemical manufacturing industries.
Multi-year, real-time atmospheric carbon tetrachloride (CCl4) record obtained at Gosan station...
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