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NILU and Hydro Aluminium performed a test campaign for measurements of CF4 and C2F6 for stack emissions at Husnes Aluminium Smelter. Time-integrated samples were taken with evacuated canisters combined with low-flow restrictors for continuous sampling periods as long as 6 weeks. The samples were analyzed at NILU with a Medusa preconcentration method combined with GC-MS SIM. As a main conclusion, time integrated sampling together with Medusa GC-MS methodology is a very precise alternative to the traditional attempts to quantify PFC-emission. NILU og Hydro Aluminium utførte en testkampanje for målinger av CF4 og C2F6 fra skorsteinsemisjoner ved Husnes Aluminium. Tidsintegrerte prøver ble tatt ved hjelp av evakuerte stålbeholdere kombinert med gass-fløde restriksjoner over tidsperioder på opptil 6 uker. Prøvene ble analysert på NILU med en Medusa oppkonsentreringsenhet som er koblet til en GC-MS i SIM modus. Metoden viser seg til å være et godt alternativ til de tradisjonelle emisjonsberegninger.

This annual report for 2021 summarizes the activities and results of the greenhouse gas monitoring at the Zeppelin Observatory, situated on Svalbard, during the period 2001-2021, and the greenhouse gas monitoring and aerosol observations from Birkenes for 2009-2021. Denne årsrapporten for 2021 presenterer aktiviteter og måleresultater fra klimagassovervåkingen ved Zeppelinobservatoriet på Svalbard for årene 2001-2021 og klimagassmålinger og klimarelevante partikkelmålinger fra Birkenes for 2009-2021.

Seasonal to interannual variations in the concentrations of sulfur aerosols (< 2.5 µm in diameter; non sea-salt sulfate: NSS-SO42-; anthropogenic sulfate: Anth-SO42-; biogenic sulfate: Bio-SO42-; methanesulfonic acid: MSA) in the Arctic atmosphere were investigated using measurements of the chemical composition of aerosols collected at Ny-Ålesund, Svalbard (78.9∘ N, 11.9∘ E) from 2015 to 2019. In all measurement years the concentration of NSS-SO42- was highest during the pre-bloom period and rapidly decreased towards summer. During the pre-bloom period we found a strong correlation between NSS-SO42- (sum of Anth-SO42- and Bio-SO42-) and Anth-SO42-. This was because more than 50 % of the NSS-SO42- measured during this period was Anth-SO42-, which originated in northern Europe and was subsequently transported to the Arctic in Arctic haze. Unexpected increases in the concentration of Bio-SO42- aerosols (an oxidation product of dimethylsulfide: DMS) were occasionally found during the pre-bloom period. These probably originated in regions to the south (the North Atlantic Ocean and the Norwegian Sea) rather than in ocean areas in the proximity of Ny-Ålesund. Another oxidation product of DMS is MSA, and the ratio of MSA to Bio-SO42- is extensively used to estimate the total amount of DMS-derived aerosol particles in remote marine environments. The concentration of MSA during the pre-bloom period remained low, primarily because of the greater loss of MSA relative to Bio-SO42- and the suppression of condensation of gaseous MSA onto particles already present in air masses being transported northwards from distant ocean source regions (existing particles). In addition, the low light intensity during the pre-bloom period resulted in a low concentration of photochemically activated oxidant species including OH radicals and BrO; these conditions favored the oxidation pathway of DMS to Bio-SO42- rather than to MSA, which acted to lower the MSA concentration at Ny-Ålesund. The concentration of MSA peaked in May or June and was positively correlated with phytoplankton biomass in the Greenland and Barents seas around Svalbard. As a result, the mean ratio of MSA to the DMS-derived aerosols was low (0.09 ± 0.07) in the pre-bloom period but high (0.32 ± 0.15) in the bloom and post-bloom periods. There was large interannual variability in the ratio of MSA to Bio-SO42- (i.e., 0.24 ± 0.11 in 2017, 0.40 ± 0.14 in 2018, and 0.36 ± 0.14 in 2019) during the bloom and post-bloom periods. This was probably associated with changes in the chemical properties of existing particles, biological activities surrounding the observation site, and air mass transport patterns. Our results indicate that MSA is not a conservative tracer for predicting DMS-derived particles, and the contribution of MSA to the growth of newly formed particles may be much larger during the bloom and post-bloom periods than during the pre-bloom period.

Global and regional atmospheric measurements and modeling can play key roles in discovering and quantifying unexpected nascent emissions of environmentally important substances. We focus here on three hydrochlorofluorocarbons (HCFCs) that are restricted by the Montreal Protocol because of their roles in stratospheric ozone depletion. Based on measurements of archived air samples and on in situ measurements at stations of the Advanced Global Atmospheric Gases Experiment (AGAGE) network, we report global abundances, trends, and regional enhancements for HCFC-132b ( C H 2 C l C C l F 2 ), which is newly discovered in the atmosphere, and updated results for HCFC-133a ( C H 2 C l C F 3 ) and HCFC-31 ( C H 2 ClF). No purposeful end-use is known for any of these compounds. We find that HCFC-132b appeared in the atmosphere 20 y ago and that its global emissions increased to 1.1 Gg⋅y −1 by 2019. Regional top-down emission estimates for East Asia, based on high-frequency measurements for 2016–2019, account for ∼95% of the global HCFC-132b emissions and for ∼80% of the global HCFC-133a emissions of 2.3 Gg⋅y −1 during this period. Global emissions of HCFC-31 for the same period are 0.71 Gg⋅y −1 . Small European emissions of HCFC-132b and HCFC-133a, found in southeastern France, ceased in early 2017 when a fluorocarbon production facility in that area closed. Although unreported emissive end-uses cannot be ruled out, all three compounds are most likely emitted as intermediate by-products in chemical production pathways. Identification of harmful emissions to the atmosphere at an early stage can guide the effective development of global and regional environmental policy.

This is chapter 4 of the State of Environmental Science in Svalbard (SESS) report 2020 (https://sios-svalbard.org/SESS_Issue3). The phenomenon of Arctic haze was studied in Ny-Ålesund at two observatories close to each other but at different altitudes (Gruvebadet and Mt Zeppelin, 50 m and 700 m a.s.l.). The sites are influenced by a different mix of sources and transport processes: mainly long-range sources and free troposphere at Mt Zeppelin and short-range inputs at Gruvebadet. These two complementary sites offer a way to better understand advection of polluted air masses to Svalbard at continental and local-to-regional scale. The data series from Mt Zeppelin covers the last 27 years while the Gruvebadet data series begins in 2010. Here we present the first comparison of the available data on chemical tracers for this potentially harmful phenomenon (sulphate and ammonium), to be developed further by taking into account other tracers. Sulphate concentrations in the atmosphere have been decreasing in the Arctic since the 1990s (in line with falling SO2 emissions). Our data show continued decreases at roughly the same rate also in the first decade of the 21st century. Moreover, we find that this decrease is particularly intense during Arctic haze months (winter and early spring), whereas in autumn the concentrations are constant or slightly rising. Decreases in sulphate may have opposing fallouts on climate, environment and human health in Svalbard, since the atmosphere is becoming poorer in sulphuric acid, favouring an additional warming of the atmosphere (lower scattering effect on incoming solar radiation) and modifying the chemistry of the atmosphere (towards a more alkaline character, richer in ammonia).

The Integrated Carbon Observation System (ICOS) is a pan-European research infrastructure which provides harmonized and high-precision scientific data on the carbon cycle and the greenhouse gas budget. All stations have to undergo a rigorous assessment before being labeled, i.e., receiving approval to join the network. In this paper, we present the labeling process for the ICOS atmosphere network through the 23 stations that were labeled between November 2017 and November 2019. We describe the labeling steps, as well as the quality controls, used to verify that the ICOS data (CO2, CH4, CO and meteorological measurements) attain the expected quality level defined within ICOS. To ensure the quality of the greenhouse gas data, three to four calibration gases and two target gases are measured: one target two to three times a day, the other gases twice a month. The data are verified on a weekly basis, and tests on the station sampling lines are performed twice a year. From these high-quality data, we conclude that regular calibrations of the CO2, CH4 and CO analyzers used here (twice a month) are important in particular for carbon monoxide (CO) due to the analyzer's variability and that reducing the number of calibration injections (from four to three) in a calibration sequence is possible, saving gas and extending the calibration gas lifespan. We also show that currently, the on-site water vapor correction test does not deliver quantitative results possibly due to environmental factors. Thus the use of a drying system is strongly recommended. Finally, the mandatory regular intake line tests are shown to be useful in detecting artifacts and leaks, as shown here via three different examples at the stations. .

The report summarizes the activities and results of the greenhouse gas monitoring at the Zeppelin Observatory, situated on Svalbard in Arctic Norway, during the period 2001-2020, and the greenhouse gas monitoring and aerosol observations from Birkenes for 2009-2020. Rapporten presenterer aktiviteter og måleresultater fra klimagassovervåkingen ved Zeppelinobservatoriet på Svalbard for årene 2001-2020 og klimagassmålinger og klimarelevante partikkelmålinger fra Birkenes for 2009-2020.

The concentrations of the measured components are generally low and below national limit values for the protection of human health and critical levels for the protection of vegetation. Wind from northern sectors gave the highest average concentrations of nitrogen oxides and sulfur dioxide, which indicates the power station and the harbour as possible sources. We also see single episodes of long-range transport of sulfur dioxide. De målte konsentrasjonene var generelt lave for alle komponenter og under nasjonale grenseverdier for beskyttelse av menneskets helse og økosystemet. Vind fra nordlige sektorer ga de høyeste gjennomsnittskonsentrasjonene av nitrogenoksider og svoveldioksid, noe som peker på kraftstasjonen og havnen som mulige kilder. Vi ser også enkelte episoder med langtransport av svoveldioksid.

The report summarizes the results from additional snow sampling and regular monitoring activities in connection to the rocket launch in Ny-Ålesund 7 Dec 2018, 26 Nov 2019 and 10 Dec 2019 to document possible impacts on environment and on the monitoring activities in Ny-Ålesund. An enhanced deposition of aluminium (Al) and iron (Fe) on the local environment due to the rocket launch is observed. Rapporten oppsummerer resultatene fra ekstra analyser av snøprøver samt pågående overvåkingsaktiviteter i forbindelse med rakettoppskytingen i Ny-Ålesund 7. desember 2018, 26. november 2019 og 10. desember 2019 for å dokumentere mulige påvirkninger av rakettoppskyting på miljøet og overvåkingsaktivitetene i Ny-Ålesund. Det observeres en økt avsetning av Al og Fe i Ny-Ålesund-området som skyldes utslipp fra rakettoppskytingen.

The report summarizes the activities and results of the greenhouse gas monitoring at the Zeppelin Observatory, situated on Svalbard in Arctic Norway, during the period 2001-2019, and the greenhouse gas monitoring and aerosol observations from Birkenes for 2009-2019. Rapporten presenterer aktiviteter og måleresultater fra klimagassovervåkingen ved Zeppelin observatoriet på Svalbard for årene 2001-2019 og klimagassmålinger og klimarelevante partikkelmålinger fra Birkenes for 2009-2019.

The Arctic is one of the most rapidly warming regions of the Earth, with predicted temperature increases of 5–7 ∘C and the accompanying extensive retreat of Arctic glacial systems by 2100. Retreating glaciers will reveal new land surfaces for microbial colonisation, ultimately succeeding to tundra over decades to centuries. An unexplored dimension to these changes is the impact upon the emission and consumption of halogenated organic compounds (halocarbons). Halocarbons are involved in several important atmospheric processes, including ozone destruction, and despite considerable research, uncertainties remain in the natural cycles of some of these compounds. Using flux chambers, we measured halocarbon fluxes across the glacier forefield (the area between the present-day position of a glacier's ice-front and that at the last glacial maximum) of a high-Arctic glacier in Svalbard, spanning recently exposed sediments (

The concentrations of the measured components are generally low and below national limit values for the protection of human health and critical levels for the protection of vegetation. Wind from northern sectors gave the highest average concentrations of nitrogen oxides and sulphur dioxide, which indicates the power station and the harbour as possible sources. The measurement results for CO2 show an annual variation with higher concentrations in the winter and lower in summer. Measured concentrations of CO were most likely caused by local snowmobile traffic. De målte konsentrasjonene var generelt lave for alle komponenter og under nasjonale grenseverdier for beskyttelse av menneskets helse og økosystemet. Vind fra nordlige sektorer ga de høyeste gjennomsnittskonsentrasjonene av nitrogenoksider og svoveldioksid, noe som peker på kraftstasjonen og havnen som mulige kilder. Måleresultatene for CO2 viser en årlig variasjon, med høyere konsentrasjoner om vinteren og lavere om sommeren. Kilder for de målte konsentrasjonene av CO var mest sannsynlig lokal snøskutertrafikk.

The report summaries the activities and results of the greenhouse gas monitoring at the Zeppelin Observatory situated on Svalbard in Arctic Norway during the period 2001-2018, and the greenhouse gas monitoring and aerosol observations from Birkenes for 2009-2018. Rapporten presenterer aktiviteter og måleresultater fra klimagassovervåkingen ved Zeppelin-observatoriet på Svalbard for årene 2001-2018 og klimagassmålinger og klimarelevante partikkelmålinger fra Birkenes for 2009-2018.

We present inverse modelling (top down) estimates of European methane (CH4) emissions for 2006-2012 based on a new quality-controlled and harmonised in situ data set from 18 European atmospheric monitoring stations. We applied an ensemble of seven inverse models and performed four inversion experiments, investigating the impact of different sets of stations and the use of a priori information on emissions. The inverse models infer total CH4 emissions of 26.8 (20.2-29.7) TgCH(4) yr(-1) (mean, 10th and 90th percentiles from all inversions) for the EU-28 for 2006-2012 from the four inversion experiments. For comparison, total anthropogenic CH4 emissions reported to UNFCCC (bottom up, based on statistical data and emissions factors) amount to only 21.3 TgCH(4) yr(-1) (2006) to 18.8 TgCH(4) yr(-1) (2012). A potential explanation for the higher range of top-down estimates compared to bottom-up inventories could be the contribution from natural sources, such as peatlands, wetlands, and wet soils. Based on seven different wetland inventories from the Wetland and Wetland CH4 Inter-comparison of Models Project (WETCHIMP), total wetland emissions of 4.3 (2.3-8.2) TgCH(4) yr(-1) from the EU-28 are estimated. The hypothesis of significant natural emissions is supported by the finding that several inverse models yield significant seasonal cycles of derived CH4 emissions with maxima in summer, while anthropogenic CH4 emissions are assumed to have much lower seasonal variability. Taking into account the wetland emissions from the WETCHIMP ensemble, the top-down estimates are broadly consistent with the sum of anthropogenic and natural bottom-up inventories. However, the contribution of natural sources and their regional distribution remain rather uncertain. Furthermore, we investigate potential biases in the inverse models by comparison with regular aircraft profiles at four European sites and with vertical profiles obtained during the Infrastructure for Measurement of the European Carbon Cycle (IMECC) aircraft campaign. We present a novel approach to estimate the biases in the derived emissions, based on the comparison of simulated and measured enhancements of CH4 compared to the background, integrated over the entire boundary layer and over the lower troposphere. The estimated average regional biases range between -40 and 20% at the aircraft profile sites in France, Hungary and Poland.

Based on observations of three chlorofluorocarbons, CFC-13 (chlorotrifluoromethane), CFC-114 (dichlorotetrafluoroethane) and CFC-115 (chloropentafluoroethane) in atmospheric and firn samples, we reconstruct records of their tropospheric histories spanning nearly eight decades. These compounds were measured in polar firn air samples, in ambient air archived in canisters, and in-situ at the AGAGE (Advanced Global Atmospheric Gases Experiment) network and affiliated sites. Global emissions to the atmosphere are derived from these observations using an inversion based on a 12-box atmospheric transport model. For CFC-13, we provide the first comprehensive global analysis. This compound increased monotonically from its first appearance in the atmosphere in the late 1950s to a mean global abundance of 3.18 ppt (dry air mole fraction in parts-per-trillion, pmol mol−-1) in 2016. Its growth rate has decreased since the mid 1980s but has remained at a surprisingly high level of 0.02 ppt yr−1 since the late 2000s. CFC-114 increased from its appearance in the 1950s to a maximum of 16.6 ppt in the early 2000s, and has since slightly declined to 16.3 ppt in 2016. CFC-115 increased monotonically from its first appearance in the 1960s and reached a global mean mole fraction of 8.52 ppt in 2016. Growth rates of all three compounds over the past years are significantly larger than would be expected from zero emissions. Under the assumption of unaltered lifetimes and atmospheric transport patterns, we derive global emissions from our measurements, which have remained unexpectedly high in recent years: Mean yearly emissions for the last decade (2007–2016) of CFC-13 are at 0.48 ± 0.15 kt yr−1 (> 15 % of past peak emissions), of CFC-114 at 1.90 ± 0.84 kt yr−1 (~ 10 % of peak emissions), and of CFC-115 at 0.80 ± 0.50 kt yr−1 (> 5 % of peak emissions). Mean yearly emissions of CFC-115 for 2014–2016 are 1.08 ± 0.50 kt yr−1 and have more than doubled compared to 2009. Cumulative global emissions for CFC-114 derived from observations through 2016 exceed the global cumulative production derived from reported inventory data by > 10 % while those for CFC-115 agree well. We find CFC-13 emissions from aluminum smelters and impurities of CFC-115 in the refrigerant HFC-125 (CHF2CF3) but if extrapolated to global emissions neither of them can account for the lingering global emissions determined from the atmospheric observations. We also conduct regional inversions for the years 2012–2016 for the north-east Asian area using observations from the Korean Gosan AGAGE site and find significant emissions for CFC-114 and CFC-115, suggesting that a large fraction of their global emissions currently occur in north-eastern Asia and more specifically on the Chinese mainland.

The report summaries the activities and results of the greenhouse gas monitoring at the Zeppelin Observatory situated on Svalbard in Arctic Norway during the period 2001-2017, and the greenhouse gas monitoring and aerosol observations from Birkenes for 2009-2017.

The Zeppelin Observatory is an atmospheric monitoring station located on the northwest coast of Spitzbergen island, in the Svalbard archipelago. The station provides background air composition, meteorological and climatological data for numerous research projects. The observatory is located on a mountain ridge in a region with complex topography that affects local atmospheric circulation processes. Research question: How the seasonal data collected at the Zeppelin observatory and Ny-Ålesund station (Fig. 2b), a temporarily station in the settlement, is affected by: 1) micrometeorological conditions 2) mesoscale dynamics 3) local air pollution

The concentrations of the measured components are generally low and below national limit values for the protection of human health and critical levels for the protection of vegetation. Wind from northern sectors gave the highest average concentrations of nitrogen oxides and sulphur dioxide, which indicates the power station and the harbour as possible sources. The measurement results for CO2 show an annual variation with higher concentrations in the winter and lower in summer. Measured concentrations of CO were most likely caused by local snowmobile traffic. De målte konsentrasjonene var generelt lave for alle komponenter og under nasjonale grenseverdier for beskyttelse av menneskets helse og økosystemet. Vind fra nordlige sektorer ga de høyeste gjennomsnittskonsentrasjonene av nitrogenoksider og svoveldioksid, noe som peker på kraftstasjonen og havnen som mulige kilder. Måleresultatene for CO2 viser en årlig variasjon, med høyere konsentrasjoner om vinteren og lavere om sommeren. Kilder for de målte konsentrasjonene av CO var mest sannsynlig lokal snøskutertrafikk.

Based on observations of the chlorofluorocarbons CFC-13 (chlorotrifluoromethane), ΣCFC-114 (combined measurement of both isomers of dichlorotetrafluoroethane), and CFC-115 (chloropentafluoroethane) in atmospheric and firn samples, we reconstruct records of their tropospheric histories spanning nearly 8 decades. These compounds were measured in polar firn air samples, in ambient air archived in canisters, and in situ at the AGAGE (Advanced Global Atmospheric Gases Experiment) network and affiliated sites. Global emissions to the atmosphere are derived from these observations using an inversion based on a 12-box atmospheric transport model. For CFC-13, we provide the first comprehensive global analysis. This compound increased monotonically from its first appearance in the atmosphere in the late 1950s to a mean global abundance of 3.18 ppt (dry-air mole fraction in parts per trillion, pmol mol1) in 2016. Its growth rate has decreased since the mid-1980s but has remained at a surprisingly high mean level of 0.02 ppt yr⁻¹ since 2000, resulting in a continuing growth of CFC-13 in the atmosphere. ΣCFC-114 increased from its appearance in the 1950s to a maximum of 16.6 ppt in the early 2000s and has since slightly declined to 16.3 ppt in 2016. CFC-115 increased monotonically from its first appearance in the 1960s and reached a global mean mole fraction of 8.49 ppt in 2016. Growth rates of all three compounds over the past years are significantly larger than would be expected from zero emissions. Under the assumption of unchanging lifetimes and atmospheric transport patterns, we derive global emissions from our measurements, which have remained unexpectedly high in recent years: mean yearly emissions for the last decade (2007–2016) of CFC-13 are at 0.48 ± 0.15 kt yr⁻¹ (> 15 % of past peak emissions), of ΣCFC-114 at 1.90 ± 0.84 kt yr⁻¹ (∼ 10 % of peak emissions), and of CFC-115 at 0.80 ± 0.50 kt yr⁻¹(> 5 % of peak emissions). Mean yearly emissions of CFC-115 for 2015–2016 are 1.14 ± 0.50 kt yr⁻¹ and have doubled compared to the 2007–2010 minimum. We find CFC-13 emissions from aluminum smelters but if extrapolated to global emissions, they cannot account for the lingering global emissions determined from the atmospheric observations. We find impurities of CFC-115 in the refrigerant HFC-125 (CHF₂CF₃) but if extrapolated to global emissions, they can neither account for the lingering global CFC-115 emissions determined from the atmospheric observations nor for their recent increases. We also conduct regional inversions for the years 2012–2016 for the northeastern Asian area using observations from the Korean AGAGE site at Gosan and find significant emissions for ΣCFC-114 and CFC-115, suggesting that a large fraction of their global emissions currently occur in northeastern Asia and more specifically on the Chinese mainland.

In support of the first Tropospheric Ozone Assessment Report (TOAR) a relational database of global surface ozone observations has been developed and populated with hourly measurement data and enhanced metadata. A comprehensive suite of ozone data products including standard statistics, health and vegetation impact metrics, and trend information, are made available through a common data portal and a web interface. These data form the basis of the TOAR analyses focusing on human health, vegetation, and climate relevant ozone issues, which are part of this special feature. Cooperation among many data centers and individual researchers worldwide made it possible to build the world’s largest collection of in-situ hourly surface ozone data covering the period from 1970 to 2015. By combining the data from almost 10,000 measurement sites around the world with global metadata information, new analyses of surface ozone have become possible, such as the first globally consistent characterisations of measurement sites as either urban or rural/remote. Exploitation of these global metadata allows for new insights into the global distribution, and seasonal and long-term changes of tropospheric ozone and they enable TOAR to perform the first, globally consistent analysis of present-day ozone concentrations and recent ozone changes with relevance to health, agriculture, and climate. Considerable effort was made to harmonize and synthesize data formats and metadata information from various networks and individual data submissions. Extensive quality control was applied to identify questionable and erroneous data, including changes in apparent instrument offsets or calibrations. Such data were excluded from TOAR data products. Limitations of a posteriori data quality assurance are discussed. As a result of the work presented here, global coverage of surface ozone data for scientific analysis has been significantly extended. Yet, large gaps remain in the surface observation network both in terms of regions without monitoring, and in terms of regions that have monitoring programs but no public access to the data archive. Therefore future improvements to the database will require not only improved data harmonization, but also expanded data sharing and increased monitoring in data-sparse regions. This work is part of the Tropospheric Ozone Assessment Report (TOAR) which was supported by the International Global Atmospheric Chemistry (IGAC) project, the National Oceanic and Atmospheric Administration (NOAA), Forschungszentrum Jülich, and the World Meteorological Organisation (WMO). Many institutions and agencies sup¬ported the implementation of the measurements, and the processing, quality assurance, and submission of the data contained in the TOAR database.