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Arnold, T, Manning AJ, Kim J, Li SL, Webster H, Thomson D, Muhle J, Weiss RF, Park S, O'Doherty S.  2018.  Inverse modelling of CF4 and NF3 emissions in East Asia. Atmospheric Chemistry and Physics. 18:13305-13320.   10.5194/acp-18-13305-2018   AbstractWebsite

Decadal trends in the atmospheric abundances of carbon tetrafluoride (CF4) and nitrogen trifluoride (NF3) have been well characterised and have provided a time series of global total emissions. Information on locations of emissions contributing to the global total, however, is currently poor. We use a unique set of measurements between 2008 and 2015 from the Gosan station, Jeju Island, South Korea (part of the Advanced Global Atmospheric Gases Experiment network), together with an atmospheric transport model, to make spatially disaggregated emission estimates of these gases in East Asia. Due to the poor availability of good prior information for this study, our emission estimates are largely influenced by the atmospheric measurements. Notably, we are able to highlight emission hotspots of NF3 and CF4 in South Korea due to the measurement location. We calculate emissions of CF4 to be quite constant between the years 2008 and 2015 for both China and South Korea, with 2015 emissions calculated at 4.3 +/- 2.7 and 0.36 +/- 0.11 Gg yr(-1), respectively. Emission estimates of NF3 from South Korea could be made with relatively small uncertainty at 0.6 +/- 0.07 Gg yr(-1) in 2015, which equates to similar to 1.6% of the country's CO2 emissions. We also apply our method to calculate emissions of CHF3 (HFC-23) between 2008 and 2012, for which our results find good agreement with other studies and which helps support our choice in methodology for CF4 and NF3.

Simmonds, PG, Rigby M, McCulloch A, Vollmer MK, Henne S, Muhle J, O'Doherty S, Manning AJ, Krummel PB, Fraser PJ, Young D, Weiss RF, Salameh PK, Harth CM, Reimann S, Trudinger CM, Steele LP, Wang RHJ, Ivy DJ, Prinn RG, Mitrevski B, Etheridge DM.  2018.  Recent increases in the atmospheric growth rate and emissions of HFC-23 (CHF3) and the link to HCFC-22 (CHClF2) production. Atmospheric Chemistry and Physics. 18:4153-4169.   10.5194/acp-18-4153-2018   AbstractWebsite

High frequency measurements of trifluoromethane (HFC-23, CHF3), a potent hydrofluorocarbon greenhouse gas, largely emitted to the atmosphere as a by-product of the production of the hydrochlorofluorocarbon HCFC-22 (CHClF2), at five core stations of the Advanced Global Atmospheric Gases Experiment (AGAGE) network, combined with measurements on firn air, old Northern Hemisphere air samples and Cape Grim Air Archive (CGAA) air samples, are used to explore the current and historic changes in the atmospheric abundance of HFC-23. These measurements are used in combination with the AGAGE 2-D atmospheric 12-box model and a Bayesian inversion methodology to determine model atmospheric mole fractions and the history of global HFC-23 emissions. The global modelled annual mole fraction of HFC-23 in the background atmosphere was 28.9 +/- 0.6 pmol mol(-1) at the end of 2016, representing a 28% increase from 22.6 +/- 0.4 pmol mol(-1) in 2009. Over the same time frame, the modelled mole fraction of HCFC-22 increased by 19% from 199 +/- 2 to 237 +/- 2 pmol mol(-1). However, unlike HFC-23, the annual average HCFC-22 growth rate slowed from 2009 to 2016 at an annual average rate of -0.5 pmol mol(-1) yr(-2). This slowing atmospheric growth is consistent with HCFC-22 moving from dispersive (high fractional emissions) to feedstock (low fractional emissions) uses, with HFC-23 emissions remaining as a consequence of incomplete mitigation from all HCFC-22 production. Our results demonstrate that, following a minimum in HFC-23 global emissions in 2009 of 9.6 +/- 0.6, emissions increased to a maximum in 2014 of 14.5 +/- 0.6 Gg yr(-1) and then declined to 12.7 +/- 0.6 Gg yr(-1) (157 MtCO(2) eq.yr(-1)) in 2016. The 2009 emissions minimum is consistent with estimates based on national reports and is likely a response to the implementation of the Clean Development Mechanism (CDM) to mitigate HFC-23 emissions by incineration in developing (non-Annex 1) countries under the Kyoto Protocol. Our derived cumulative emissions of HFC-23 during 20102016 were 89 +/- 2 Gg (1.1 +/- 0.2 GtCO(2) eq.), which led to an increase in radiative forcing of 1.0 +/- 0.1mWm(-2) over the same period. Although the CDM had reduced global HFC-23 emissions, it cannot now offset the higher emissions from increasing HCFC-22 production in non-Annex 1 countries, as the CDM was closed to new entrants in 2009. We also find that the cumulative European HFC-23 emissions from 2010 to 2016 were similar to 1.3 Gg, corresponding to just 1.5% of cumulative global HFC-23 emissions over this same period. The majority of the increase in global HFC-23 emissions since 2010 is attributed to a delay in the adoption of mitigation technologies, predominantly in China and East Asia. However, a reduction in emissions is anticipated, when the Kigali 2016 amendment to the Montreal Protocol, requiring HCFC and HFC production facilities to introduce destruction of HFC-23, is fully implemented.

Simmonds, PG, Rigby M, Manning AJ, Lunt MF, O'Doherty S, McCulloch A, Fraser PJ, Henne S, Vollmer MK, Muhle J, Weiss RF, Salameh PK, Young D, Reimann S, Wenger A, Arnold T, Harth CM, Krummel PB, Steele LP, Dunse BL, Miller BR, Lunder CR, Hermansen O, Schmidbauer N, Saito T, Yokouchi Y, Park S, Li S, Yao B, Zhou LX, Arduini J, Maione M, Wang RHJ, Ivy D, Prinn RG.  2016.  Global and regional emissions estimates of 1,1-difluoroethane (HFC-152a, CH3CHF2) from in situ and air archive observations. Atmospheric Chemistry and Physics. 16:365-382.   10.5194/acp-16-365-2016   AbstractWebsite

High frequency, in situ observations from 11 globally distributed sites for the period 1994-2014 and archived air measurements dating from 1978 onward have been used to determine the global growth rate of 1,1-difluoroethane (HFC-152a, CH3CHF2). These observations have been combined with a range of atmospheric transport models to derive global emission estimates in a top-down approach. HFC-152a is a greenhouse gas with a short atmospheric lifetime of about 1.5 years. Since it does not contain chlorine or bromine, HFC-152a makes no direct contribution to the destruction of stratospheric ozone and is therefore used as a substitute for the ozone de- pleting chlorofluorocarbons (CFCs) and hydrochlorofluorocarbons (HCFCs). The concentration of HFC-152a has grown substantially since the first direct measurements in 1994, reaching a maximum annual global growth rate of 0.84 +/- 0.05 ppt yr(-1) in 2006, implying a substantial increase in emissions up to 2006. However, since 2007, the annual rate of growth has slowed to 0.38 +/- 0.04 ppt yr(-1) in 2010 with a further decline to an annual average rate of growth in 2013-2014 of -0.06 +/- 0.05 ppt yr(-1). The annual average Northern Hemisphere (NH) mole fraction in 1994 was 1.2 ppt rising to an annual average mole fraction of 10.1 ppt in 2014. Average annual mole fractions in the Southern Hemisphere (SH) in 1998 and 2014 were 0.84 and 4.5 ppt, respectively. We estimate global emissions of HFC-152a have risen from 7.3 +/- 5.6 Gg yr(-1) in 1994 to a maximum of 54.4 +/- 17.1 Gg yr(-1) in 2011, declining to 52.5 +/- 20.1 Gg yr(-1) in 2014 or 7.2 +/- 2.8 Tg-CO2 eq yr(-1). Analysis of mole fraction enhancements above regional background atmospheric levels suggests substantial emissions from North America, Asia, and Europe. Global HFC emissions (so called "bottom up" emissions) reported by the United Nations Framework Convention on Climate Change (UNFCCC) are based on cumulative national emission data reported to the UNFCCC, which in turn are based on national consumption data. There appears to be a significant underestimate (> 20 Gg) of "bottom-up" reported emissions of HFC-152a, possibly arising from largely underestimated USA emissions and undeclared Asian emissions.

O'Doherty, S, Rigby M, Muhle J, Ivy DJ, Miller BR, Young D, Simmonds PG, Reimann S, Vollmer MK, Krummel PB, Fraser PJ, Steele LP, Dunse B, Salameh PK, Harth CM, Arnold T, Weiss RF, Kim J, Park S, Li S, Lunder C, Hermansen O, Schmidbauer N, Zhou LX, Yao B, Wang RHJ, Manning AJ, Prinn RG.  2014.  Global emissions of HFC-143a (CH3CF3) and HFC-32 (CH2F2) from in situ and air archive atmospheric observations. Atmospheric Chemistry and Physics. 14:9249-9258.   10.5194/acp-14-9249-2014   AbstractWebsite

High-frequency, in situ observations from the Advanced Global Atmospheric Gases Experiment (AGAGE), for the period 2003 to 2012, combined with archive flask measurements dating back to 1977, have been used to capture the rapid growth of HFC-143a (CH3CF3) and HFC-32 (CH2F2) mole fractions and emissions into the atmosphere. Here we report the first in situ global measurements of these two gases. HFC-143a and HFC-32 are the third and sixth most abundant hydrofluorocarbons (HFCs) respectively and they currently make an appreciable contribution to the HFCs in terms of atmospheric radiative forcing (1.7 +/- 0.04 and 0.7 +/- 0.02 mW m(-2) in 2012 respectively). In 2012 the global average mole fraction of HFC-143a was 13.4 +/- 0.3 ppt (1 sigma) in the lower troposphere and its growth rate was 1.4 +/- 0.04 ppt yr(-1); HFC-32 had a global mean mole fraction of 6.2 +/- 0.2 ppt and a growth rate of 1.1 +/- 0.04 ppt yr(-1) in 2012. The extensive observations presented in this work have been combined with an atmospheric transport model to simulate global atmospheric abundances and derive global emission estimates. It is estimated that 23 +/- 3 Gg yr(-1) of HFC-143a and 21 +/- 11 Gg yr(-1) of HFC-32 were emitted globally in 2012, and the emission rates are estimated to be increasing by 7 +/- 5% yr(-1) for HFC-143a and 14 +/- 11% yr(-1) for HFC-32.

Rigby, M, Prinn RG, O'Doherty S, Miller BR, Ivy D, Muhle J, Harth CM, Salameh PK, Arnold T, Weiss RF, Krummel PB, Steele LP, Fraser PJ, Young D, Simmonds PG.  2014.  Recent and future trends in synthetic greenhouse gas radiative forcing. Geophysical Research Letters. 41:2623-2630.   10.1002/2013gl059099   AbstractWebsite

Atmospheric measurements show that emissions of hydrofluorocarbons (HFCs) and hydrochlorofluorocarbons are now the primary drivers of the positive growth in synthetic greenhouse gas (SGHG) radiative forcing. We infer recent SGHG emissions and examine the impact of future emissions scenarios, with a particular focus on proposals to reduce HFC use under the Montreal Protocol. If these proposals are implemented, overall SGHG radiative forcing could peak at around 355mWm(-2) in 2020, before declining by approximately 26% by 2050, despite continued growth of fully fluorinated greenhouse gas emissions. Compared to no HFC policy projections, this amounts to a reduction in radiative forcing of between 50 and 240mWm(-2) by 2050 or a cumulative emissions saving equivalent to 0.5 to 2.8years of CO2 emissions at current levels. However, more complete reporting of global HFC emissions is required, as less than half of global emissions are currently accounted for.

Kim, J, Li S, Muhle J, Stohl A, Kim SK, Park S, Park MK, Weiss RF, Kim KR.  2012.  Overview of the findings from measurements of halogenated compounds at Gosan (Jeju Island, Korea) quantifying emissions in East Asia. Journal of Integrative Environmental Sciences. 9:71-80.   10.1080/1943815x.2012.696548   AbstractWebsite

With increased economic growth in East Asia, regional emissions of many anthropogenic halogenated compounds now constitute a substantial fraction of the global totals. Here, we summarize recently reported findings from measurements of a wide range of chlorofluorocarbons (CFCs), hydrochlorofluorocarbons (HCFCs), hydrofluorocarbons (HFCs), perfluorocarbons (PFCs), sulfur hexafluoride (SF6), and other halogenated compounds at Gosan (Jeju Island, Korea) within the advanced global atmospheric gases experiment (AGAGE). General wind patterns at Gosan bring air masses from the surrounding areas, allowing the monitoring of both clean baseline and polluted air masses. We have analyzed our measurements since November 2007 both with an interspecies correlation method and with an inversion method based on the FLEXPART Lagrangian particle dispersion model to estimate these regional emissions. The results show that emissions of halogenated compounds in East Asia account for over 20% of global emissions, both in terms of ozone depletion potential (ODP) and global warming potential (GWP), and emphasize the importance of atmospheric measurements for quantifying emissions of these compounds in this region.

Arnold, T, Muhle J, Salameh PK, Harth CM, Ivy DJ, Weiss RF.  2012.  Automated measurement of nitrogen trifluoride in ambient air. Analytical Chemistry. 84:4798-4804.   10.1021/ac300373e   AbstractWebsite

We present an analytical method for the in situ measurement of atmospheric nitrogen trifluoride (NF3), an anthropogenic gas with a 100-year global warming potential of over 16 000. This potent greenhouse gas has a rising atmospheric abundance due to its emission from a growing number of manufacturing processes and an expanding end-use market. Here we present a modified version of the "Medusa" preconcentration gas chromatography/mass spectrometry (GC/MS) system of Miller, B. R.; Weiss, R. F.; Salameh, P. K.; Tanhua, T.; Greally, B. R; Male, J.; Simmonds, P. G. Anal. Chem. 2008, 80 (5), 1536-1545. By altering the techniques of gas separation and chromatography after initial preconcentration, we are now able to make atmospheric measurements of NF3 with relative precision <2% (1 sigma) for current background clean air samples. Importantly, this method augments the currently operational Medusa system, so that the quality of data for species already being measured is not compromised and NF3 is measured from the same preconcentrated sample. We present the first in situ measurements of NF3 from La Jolla, California made 11 times daily, illustrating how global deployment of this technique within the AGAGE (Advanced Global Atmospheric Gases Experiment) network could facilitate estimation of global and regional NF3 emissions over the coming years.

Ivy, DJ, Arnold T, Harth CM, Steele LP, Muhle J, Rigby M, Salameh PK, Leist M, Krummel PB, Fraser PJ, Weiss RF, Prinn RG.  2012.  Atmospheric histories and growth trends of C4F10, C5F12, C6F14, C7F16 and C8F18. Atmospheric Chemistry and Physics. 12:4313-4325.   10.5194/acp-12-4313-2012   AbstractWebsite

Atmospheric observations and trends are presented for the high molecular weight perfluorocarbons (PFCs): decafluorobutane (C4F10), dodecafluoropentane (C5F12), tetradecafluorohexane (C6F14), hexadecafluoroheptane (C7F16) and octadecafluorooctane (C8F18). Their atmospheric histories are based on measurements of 36 Northern Hemisphere and 46 Southern Hemisphere archived air samples collected between 1973 to 2011 using the Advanced Global Atmospheric Gases Experiment (AGAGE) 'Medusa' preconcentration gas chromatography-mass spectrometry systems. A new calibration scale was prepared for each PFC, with estimated accuracies of 6.8% for C4F10, 7.8% for C5F12, 4.0% for C6F14, 6.6% for C7F16 and 7.9% for C8F18. Based on our observations the 2011 globally averaged dry air mole fractions of these heavy PFCs are: 0.17 parts-per-trillion (ppt, i.e., parts per 10(12)) for C4F10, 0.12 ppt for C5F12, 0.27 ppt for C6F14, 0.12 ppt for C7F16 and 0.09 ppt for C8F18. These atmospheric mole fractions combine to contribute to a global average radiative forcing of 0.35 mW m(-2), which is 6% of the total anthropogenic PFC radiative forcing (Montzka and Reimann, 2011; Oram et al., 2012). The growth rates of the heavy perfluorocarbons were largest in the late 1990s peaking at 6.2 parts per quadrillion (ppq, i.e., parts per 10(15)) per year (yr) for C4F10, at 5.0 ppq yr(-1) for C5F12 and 16.6 ppq yr(-1) for C6F14 and in the early 1990s for C7F16 at 4.7 ppq yr(-1) and in the mid 1990s for C8F18 at 4.8 ppq yr(-1). The 2011 globally averaged mean atmospheric growth rates of these PFCs are subsequently lower at 2.2 ppq yr(-1) for C4F10, 1.4 ppq yr(-1) for C5F12, 5.0 ppq yr(-1) for C6F14, 3.4 ppq yr(-1) for C7F16 and 0.9 ppq yr(-1) for C8F18. The more recent slowdown in the growth rates suggests that emissions are declining as compared to the 1980s and 1990s.