Localization of source regions of selected hydrofluorocarbons combining data collected at two European mountain stations

Maione, Michela; Giostra, U.; Arduini, Jgor; Belfiore, Letizia; Furlani, Francesco; Geniali, Annalisa; Mangani, Giovanna; Vollmer, Martin K.; Reimann, Stefan

doi:10.1016/j.scitotenv.2007.10.023

Cited by 18 publications

(24 citation statements)

References 15 publications

(12 reference statements)

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“…For instance, Manning et al (2003) and O'Doherty et al (2004) used data from Mace Head, a Lagrangian particle dispersion model (LPDM), and a so-called simulated annealing technique to estimate halocarbon emissions over Europe. Even simple back trajectories combined with statistical methods have been used to derive halocarbon emission patterns qualitatively (Maione et al, 2008;Reimann et al, 2004Reimann et al, , 2008. Over the short time intervals (about 4-10 d) typically covered by back trajectories, halocarbons are almost perfectly conserved.…”

Section: Introductionmentioning

confidence: 99%

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

et al. 2009

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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 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 Correspondence to: A. Stohl (ast@nilu.no) 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.

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Section: Introductionmentioning

confidence: 99%

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

et al. 2009

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“…The system is currently operating for continuous measurements at a mountain remote site in Europe (MTC,Monte Cimone,Italy,44.17 N,10.68 E, 2165 m a.s.l.) (Maione et al, 2008). For the specific purpose of analysing flask samples, the GC inlet is connected to the stainless steel canister.…”

Section: Analytical Methodologymentioning

confidence: 99%

“…Some general considerations are: (i) the Montreal gases, especially the fully halogenated species, show a significant occurrence of "above the baseline" values, as a consequence of their current use in A5 countries surrounding the region; (ii) on the contrary, as a consequence of a more recent introduction and a possible less frequent use in the region, the Kyoto gases show less frequent spikes if compared with those occurring in time series recorded in other remote stations located in non-A5 countries Greally et al, 2007;Maione et al, 2008).…”

Section: Anthropogenic Speciesmentioning

confidence: 99%

“…6, shows the localisation of potential source regions in the domain considered. For major detail on the procedure and significance of maps of conditional probability see Maione et al (2008). Low spatial resolution of trajectories and the low temporal resolution of measurements suggest that the results should be treated with caution.…”

Section: Analysis Of Pollution Episodesmentioning

confidence: 99%

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Three-year observations of halocarbons at the Nepal Climate Observatory at Pyramid (NCO-P, 5079 m a.s.l.) on the Himalayan range

et al. 2011

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Abstract.A monitoring programme for halogenated climate-altering gases has been established in the frame of the SHARE EV-K 2 -CNR project at the Nepal Climate Laboratory -Pyramid in the Himalayan range at the altitude of 5079 m a.s.l. The site is very well located to provide important insights on changes in atmospheric composition in a region that is of great significance for emissions of both anthropogenic and biogenic halogenated compounds. Measurements are performed since March 2006, with grab samples collected on a weekly basis. The first three years of data have been analysed. After the identification of the atmospheric background values for fourteen halocarbons, the frequency of occurrence of pollution events have been compared with the same kind of analysis for data collected at other global background stations. The analysis showed the fully halogenated species, whose production and consumption are regulated under the Montreal Protocol, show a significant occurrence of "above the baseline" values, as a consequence of their current use in the developing countries surrounding the region, meanwhile the hydrogenated gases, more recently introduced into the market, show less frequent spikes.Atmospheric concentration trends have been calculated as well, and they showed a fast increase, ranging from 5.7 to 12.6%, of all the hydrogenated species, and a clear decrease of methyl chloroform (−17.7%). The comparison with time series from other stations has also allowed to derive Meridional gradients, which are absent for long living well mixed species, while for the more reactive species, the gradient inCorrespondence to: M. Maione (michela.maione@uniurb.it) creases inversely with respect to their atmospheric lifetime. The effect of long range transport and of local events on the atmospheric composition at the station has been analysed as well, allowing the identification of relevant source regions the Northern half of the Indian sub-continent. Also, at finer spatial scales, a smaller, local contribution of forest fires from the Khumbu valley has been detected.

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“…In the attempt to extend site measurements to emission surveillance, promising approaches have been made by combining measurement data with inverse modelling (e.g. Keller et al, 2011;Lunt et al, 2015;Maione et al, 2008;Simmonds et al, 2015;Stohl et al, 2010).…”

Section: Introductionmentioning

confidence: 99%

An automated gas chromatography time-of-flight mass spectrometry instrument for the quantitative analysis of halocarbons in air

2016

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Abstract. We present the characterization and application of a new gas chromatography time-of-flight mass spectrometry instrument (GC-TOFMS) for the quantitative analysis of halocarbons in air samples. The setup comprises three fundamental enhancements compared to our earlier work (Hoker et al., 2015): (1) full automation, (2) a mass resolving power R = m/ m of the TOFMS (Tofwerk AG, Switzerland) increased up to 4000 and (3) a fully accessible data format of the mass spectrometric data. Automation in combination with the accessible data allowed an indepth characterization of the instrument. Mass accuracy was found to be approximately 5 ppm in mean after automatic recalibration of the mass axis in each measurement. A TOFMS configuration giving R = 3500 was chosen to provide an R-to-sensitivity ratio suitable for our purpose. Calculated detection limits are as low as a few femtograms by means of the accurate mass information. The precision for substance quantification was 0.15 % at the best for an individual measurement and in general mainly determined by the signal-to-noise ratio of the chromatographic peak. Detector non-linearity was found to be insignificant up to a mixing ratio of roughly 150 ppt at 0.5 L sampled volume. At higher concentrations, non-linearities of a few percent were observed (precision level: 0.2 %) but could be attributed to a potential source within the detection system. A straightforward correction for those non-linearities was applied in data processing, again by exploiting the accurate mass information. Based on the overall characterization results, the GC-TOFMS instrument was found to be very well suited for the task of quantitative halocarbon trace gas observation and a big step forward compared to scanning, quadrupole MS with low mass resolving power and a TOFMS technique reported to be non-linear and restricted by a small dynamical range.

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Localization of source regions of selected hydrofluorocarbons combining data collected at two European mountain stations

Cited by 18 publications

References 15 publications

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

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

Three-year observations of halocarbons at the Nepal Climate Observatory at Pyramid (NCO-P, 5079 m a.s.l.) on the Himalayan range

An automated gas chromatography time-of-flight mass spectrometry instrument for the quantitative analysis of halocarbons in air

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