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Hydrofluorocarbons are powerful greenhouse gases developed by industry after the phase-out of the ozone depleting chlorofluorocarbons and hydrochlorofluorocarbons required by the Montreal Protocol. The climate benefit of reducing the emissions of hydrofluorocarbons has been widely recognised, leading to an amendment of the Montreal Protocol (Kigali Amendment) calling for developed countries to start to phase-down hydrofluorocarbons by 2019 and in developing countries to follow with a freeze between 2024 and 2028. In this way, nearly half a degree Celsius of warming would be avoided by the end of the century. Hydrofluorocarbons are also included in the basket of gases controlled under the Kyoto Protocol of the United Nations Framework Convention on Climate Change. Annex I parties to the Convention submit annual national greenhouse gas inventories based on a bottom-up approach, which relies on declared anthropogenic activities. Top-down methodologies, based on atmospheric measurements and modelling, can be used in support to the inventory compilation. In this study we used atmospheric data from four European sites combined with the FLEXPART dispersion model and a Bayesian inversion method, in order to derive emissions of nine individual hydrofluorocarbons from the whole European Geographic Domain and from twelve regions within it, then comparing our results with the annual emissions that the European countries submit every year to the United Nations Framework Convention on Climate Change, as well as with the bottom-up Emissions Database for Global Atmospheric Research. We found several discrepancies when considering the specific compounds and on the country level. However, an overall agreement is found when comparing European aggregated data, which between 2008 and 2014 are on average 84.2 ± 28.0 Tg-CO2-eq·yr−1 against the 95.1 Tg-CO2-eq·yr−1 reported by UNFCCC in the same period. Therefore, in agreement with other studies, the gap on the global level between bottom-u

Anthropogenic increases in atmospheric greenhouse gas concentrations are the main driver of current and future climate change. The integrated assessment community has quantified anthropogenic emissions for the shared socio-economic pathway (SSP) scenarios, each of which represents a different future socio-economic projection and political environment. Here, we provide the greenhouse gas concentrations for these SSP scenarios – using the reduced-complexity climate–carbon-cycle model MAGICC7.0. We extend historical, observationally based concentration data with SSP concentration projections from 2015 to 2500 for 43 greenhouse gases with monthly and latitudinal resolution. CO2 concentrations by 2100 range from 393 to 1135 ppm for the lowest (SSP1-1.9) and highest (SSP5-8.5) emission scenarios, respectively. We also provide the concentration extensions beyond 2100 based on assumptions regarding the trajectories of fossil fuels and land use change emissions, net negative emissions, and the fraction of non-CO2 emissions. By 2150, CO2 concentrations in the lowest emission scenario are approximately 350 ppm and approximately plateau at that level until 2500, whereas the highest fossil-fuel-driven scenario projects CO2 concentrations of 1737 ppm and reaches concentrations beyond 2000 ppm by 2250. We estimate that the share of CO2 in the total radiative forcing contribution of all considered 43 long-lived greenhouse gases increases from 66 % for the present day to roughly 68 % to 85 % by the time of maximum forcing in the 21st century. For this estimation, we updated simple radiative forcing parameterizations that reflect the Oslo Line-By-Line model results. In comparison to the representative concentration pathways (RCPs), the five main SSPs (SSP1-1.9, SSP1-2.6, SSP2-4.5, SSP3-7.0, and SSP5-8.5) are more evenly spaced and extend to lower 2100 radiative forcing and temperatures. Performing two pairs of six-member historical ensembles with CESM1.2.2, we estimate the effect on

Anthropogenic increases in atmospheric greenhouse gas concentrations are the main driver of current and future climate change. The integrated assessment community has quantified anthropogenic emissions for the shared socio-economic pathway (SSP) scenarios, each of which represents a different future socio-economic projection and political environment. Here, we provide the greenhouse gas concentrations for these SSP scenarios – using the reduced-complexity climate–carbon-cycle model MAGICC7.0. We extend historical, observationally based concentration data with SSP concentration projections from 2015 to 2500 for 43 greenhouse gases with monthly and latitudinal resolution. CO2 concentrations by 2100 range from 393 to 1135 ppm for the lowest (SSP1-1.9) and highest (SSP5-8.5) emission scenarios, respectively. We also provide the concentration extensions beyond 2100 based on assumptions regarding the trajectories of fossil fuels and land use change emissions, net negative emissions, and the fraction of non-CO2 emissions. By 2150, CO2 concentrations in the lowest emission scenario are approximately 350 ppm and approximately plateau at that level until 2500, whereas the highest fossil-fuel-driven scenario projects CO2 concentrations of 1737 ppm and reaches concentrations beyond 2000 ppm by 2250. We estimate that the share of CO2 in the total radiative forcing contribution of all considered 43 long-lived greenhouse gases increases from 66 % for the present day to roughly 68 % to 85 % by the time of maximum forcing in the 21st century. For this estimation, we updated simple radiative forcing parameterizations that reflect the Oslo Line-By-Line model results. In comparison to the representative concentration pathways (RCPs), the five main SSPs (SSP1-1.9, SSP1-2.6, SSP2-4.5, SSP3-7.0, and SSP5-8.5) are more evenly spaced and extend to lower 2100 radiative forcing and temperatures. Performing two pairs of six-member historical ensembles with CESM1.2.2, we estimate the effect on

Anthropogenic increases in atmospheric greenhouse gas concentrations are the main driver of current and future climate change. The integrated assessment community has quantified anthropogenic emissions for the shared socio-economic pathway (SSP) scenarios, each of which represents a different future socio-economic projection and political environment. Here, we provide the greenhouse gas concentrations for these SSP scenarios – using the reduced-complexity climate–carbon-cycle model MAGICC7.0. We extend historical, observationally based concentration data with SSP concentration projections from 2015 to 2500 for 43 greenhouse gases with monthly and latitudinal resolution. CO2 concentrations by 2100 range from 393 to 1135 ppm for the lowest (SSP1-1.9) and highest (SSP5-8.5) emission scenarios, respectively. We also provide the concentration extensions beyond 2100 based on assumptions regarding the trajectories of fossil fuels and land use change emissions, net negative emissions, and the fraction of non-CO2 emissions. By 2150, CO2 concentrations in the lowest emission scenario are approximately 350 ppm and approximately plateau at that level until 2500, whereas the highest fossil-fuel-driven scenario projects CO2 concentrations of 1737 ppm and reaches concentrations beyond 2000 ppm by 2250. We estimate that the share of CO2 in the total radiative forcing contribution of all considered 43 long-lived greenhouse gases increases from 66 % for the present day to roughly 68 % to 85 % by the time of maximum forcing in the 21st century. For this estimation, we updated simple radiative forcing parameterizations that reflect the Oslo Line-By-Line model results. In comparison to the representative concentration pathways (RCPs), the five main SSPs (SSP1-1.9, SSP1-2.6, SSP2-4.5, SSP3-7.0, and SSP5-8.5) are more evenly spaced and extend to lower 2100 radiative forcing and temperatures. Performing two pairs of six-member historical ensembles with CESM1.2.2, we estimate the effect on

Heavy metals which accumulate in soils may be harmful to soil and its boundary ecosystems. In this paper a unified risk assessment and risk management concept is proposed followed by a discussion on its practical implementation. To assess and manage risk, the application of a three-level evaluation system is presented, incorporating the degree of metal contamination. Levels for guide values, trigger values and clean up values are used. In order to assess exposure to heavy metals, three metal fractions like mobile, mobilisable and pseudo total metal fractions are introduced. Exceeding trigger and guide values at a site may be harmful to the risk receptors. Adequate site-specific mild remediation measures aim to diminish or eliminate risk without adversely affecting basic functions of soil. The importance of mobile and mobilisable metal concentrations is discussed in relation to the development of ecological and economical sound remediation techniques.

Heavy metals which accumulate in soils may be harmful to soil and its boundary ecosystems. In this paper a unified risk assessment and risk management concept is proposed followed by a discussion on its practical implementation. To assess and manage risk, the application of a three-level evaluation system is presented, incorporating the degree of metal contamination. Levels for guide values, trigger values and clean up values are used. In order to assess exposure to heavy metals, three metal fractions like mobile, mobilisable and pseudo total metal fractions are introduced. Exceeding trigger and guide values at a site may be harmful to the risk receptors. Adequate site-specific mild remediation measures aim to diminish or eliminate risk without adversely affecting basic functions of soil. The importance of mobile and mobilisable metal concentrations is discussed in relation to the development of ecological and economical sound remediation techniques.

The performance of 18 European institutions involved in long-term non-methane hydrocarbon (NMHC) measurements in ambient air within the framework of the Global Atmosphere Watch (GAW) and the European Monitoring and Evaluation Programme (EMEP) was assessed with respect to data quality objectives (DQOs) of ACTRIS (Aerosols, Clouds, and Trace gases Research InfraStructure Network) and GAW. Compared to previous intercomparison studies the DQOs define a novel approach to assess and ensure a high quality of the measurements. Having already been adopted by GAW, the ACTRIS DQOs are demanding with deviations to a reference value of less than 5 % and a repeatability of better than 2 % for NMHC mole fractions above 0.1 nmol mol−1. The participants of the intercomparison analysed two dry gas mixtures in pressurised cylinders, a 30-component NMHC mixture in nitrogen (NMHC_N2) at approximately 1 nmol mol−1 and a whole air sample (NMHC_air), following a standardised operation procedure including zero- and calibration gas measurements. Furthermore, participants had to report details on their instruments and assess their measurement uncertainties. The NMHCs were analysed either by gas chromatography–flame ionisation detection (GC-FID) or by gas chromatography–mass spectrometry (GC-MS). For the NMHC_N2 measurements, 62 % of the reported values were within the 5 % deviation class corresponding to the ACTRIS DQOs. For NMHC_air, generally more frequent and larger deviations to the assigned values were observed, with 50 % of the reported values within the 5 % deviation class. Important contributors to the poorer performance in NMHC_air compared to NMHC_N2 were a more complex matrix and a larger span of NMHC mole fractions (0.03–2.5 nmol mol−1). The performance of the participating laboratories were affected by the different measurement procedures such as the usage of a two-step vs. a one-step calibration, breakthroughs of C2–C3 hydrocarbons in the focussing trap, blank values in zero-gas

The performance of 18 European institutions involved in long-term non-methane hydrocarbon (NMHC) measurements in ambient air within the framework of the Global Atmosphere Watch (GAW) and the European Monitoring and Evaluation Programme (EMEP) was assessed with respect to data quality objectives (DQOs) of ACTRIS (Aerosols, Clouds, and Trace gases Research InfraStructure Network) and GAW. Compared to previous intercomparison studies the DQOs define a novel approach to assess and ensure a high quality of the measurements. Having already been adopted by GAW, the ACTRIS DQOs are demanding with deviations to a reference value of less than 5 % and a repeatability of better than 2 % for NMHC mole fractions above 0.1 nmol mol−1. The participants of the intercomparison analysed two dry gas mixtures in pressurised cylinders, a 30-component NMHC mixture in nitrogen (NMHC_N2) at approximately 1 nmol mol−1 and a whole air sample (NMHC_air), following a standardised operation procedure including zero- and calibration gas measurements. Furthermore, participants had to report details on their instruments and assess their measurement uncertainties. The NMHCs were analysed either by gas chromatography–flame ionisation detection (GC-FID) or by gas chromatography–mass spectrometry (GC-MS). For the NMHC_N2 measurements, 62 % of the reported values were within the 5 % deviation class corresponding to the ACTRIS DQOs. For NMHC_air, generally more frequent and larger deviations to the assigned values were observed, with 50 % of the reported values within the 5 % deviation class. Important contributors to the poorer performance in NMHC_air compared to NMHC_N2 were a more complex matrix and a larger span of NMHC mole fractions (0.03–2.5 nmol mol−1). The performance of the participating laboratories were affected by the different measurement procedures such as the usage of a two-step vs. a one-step calibration, breakthroughs of C2–C3 hydrocarbons in the focussing trap, blank values in zero-gas

©2015. The Authors. We have developed a chemical mechanism describing the tropospheric degradation of chlorine containing very short-lived substances (VSLS). The scheme was included in a global atmospheric model and used to quantify the stratospheric injection of chlorine from anthropogenic VSLS (ClyVSLS) between 2005 and 2013. By constraining the model with surface measurements of chloroform (CHCl3), dichloromethane (CH2Cl2), tetrachloroethene (C2Cl4), trichloroethene (C2HCl3), and 1,2-dichloroethane (CH2ClCH2Cl), we infer a 2013 ClyVSLS mixing ratio of 123 parts per trillion (ppt). Stratospheric injection of source gases dominates this supply, accounting for ∼83% of the total. The remainder comes from VSLS-derived organic products, phosgene (COCl2, 7%) and formyl chloride (CHClO, 2%), and also hydrogen chloride (HCl, 8%). Stratospheric ClyVSLS increased by ∼52% between 2005 and 2013, with a mean growth rate of 3.7 ppt Cl/yr. This increase is due to recent and ongoing growth in anthropogenic CH2Cl2 - the most abundant chlorinated VSLS not controlled by the Montreal Protocol.

Molecular hydrogen (H2), its stable isotope signature ( D), and the key combustion parameters carbon monoxide (CO), carbon dioxide (CO2), and methane (CH4) were measured from various combustion processes. H2 in the exhaust of gas and oil-fired heaters and of waste incinerator plants was generally depleted compared to ambient intake air, while CO was significantly elevated. These findings contradict the often assumed co-occurring net H2 and CO emissions in combustion processes and suggest that previous H2 emissions from combustion may have been overestimated when scaled to CO emissions. For the gas and oil-fired heater exhausts, H2 and D generally decrease with increasing CO2, from ambient values of 0.5 ppm and +130‰ to 0.2 ppm and −206 ‰, respectively. These results are interpreted as a combination of an isotopically light H2 source from fossil fuel combustion and a D/H kinetic isotope fractionation of hydrogen in the advected ambient air during its partial removal during combustion. Diesel exhaust measurements from dynamometer test stand driving cycles show elevated H2 and CO emissions during cold-start and some acceleration phases. While H2 and CO emissions from diesel vehicles are known to be significantly less than those from gasoline vehicles (on a fuel-energy base), we find that their molar H2/CO ratios (median 0.026, interpercentile range 0.12) are also significantly less compared to gasoline vehicle exhaust. Using H2/CO emission ratios, along with CO global emission inventories, we estimate global H2 emissions for 2000, 2005, and 2010. For road transportation (gasoline and diesel), we calculate 8.3±2.2 Tg, 6.0±1.5 Tg, and 3.8±0.94 Tg, respectively, whereas the contribution from diesel vehicles is low (0.9–1.4 %). Other fossil fuel emissions are believed to be negligible but H2 emissions from coal combustion are unknown. For residential (domestic) emissions, which are likely dominated by biofuel combustion, emissions for the same years are estimated at 2.7±0.

HCFC-22 (CHClF2, chlorodifluoromethane) is an ozone-depleting substance (ODS) as well as a significant greenhouse gas (GHG). HCFC-22 has been used widely as a refrigerant fluid in cooling and air-conditioning equipment since the 1960s, and it has also served as a traditional substitute for some chlorofluorocarbons (CFCs) controlled under the Montreal Protocol. A low frequency record on tropospheric HCFC-22 since the late 1970s is available from measurements of the Southern Hemisphere Cape Grim Air Archive (CGAA) and a few Northern Hemisphere air samples (mostly from Trinidad Head) using the Advanced Global Atmospheric Gases Experiment (AGAGE) instrumentation and calibrations. Since the 1990s high-frequency, high-precision, in situ HCFC-22 measurements have been collected at these AGAGE stations. Since 1992, the Global Monitoring Division of the National Oceanic and Atmospheric Administration/Earth System Research Laboratory (NOAA/ESRL) has also collected flasks on a weekly basis from remote sites across the globe and analyzed them for a suite of halocarbons including HCFC-22. Additionally, since 2006 flasks have been collected approximately daily at a number of tower sites across the US and analyzed for halocarbons and other gases at NOAA. All results show an increase in the atmospheric mole fractions of HCFC-22, and recent data show a growth rate of approximately 4% per year, resulting in an increase in the background atmospheric mole fraction by a factor of 1.7 from 1995 to 2009. Using data on HCFC-22 consumption submitted to the United Nations Environment Programme (UNEP), as well as existing bottom-up emission estimates, we first create globally-gridded a priori HCFC-22 emissions over the 15 yr since 1995. We then use the three-dimensional chemical transport model, Model for Ozone and Related Chemical Tracers version 4 (MOZART v4), and a Bayesian inverse method to estimate global as well as regional annual emissions. Our inversion indicates that the global HCFC

HCFC-22 (CHClF2, chlorodifluoromethane) is an ozone-depleting substance (ODS) as well as a significant greenhouse gas (GHG). HCFC-22 has been used widely as a refrigerant fluid in cooling and air-conditioning equipment since the 1960s, and it has also served as a traditional substitute for some chlorofluorocarbons (CFCs) controlled under the Montreal Protocol. A low frequency record on tropospheric HCFC-22 since the late 1970s is available from measurements of the Southern Hemisphere Cape Grim Air Archive (CGAA) and a few Northern Hemisphere air samples (mostly from Trinidad Head) using the Advanced Global Atmospheric Gases Experiment (AGAGE) instrumentation and calibrations. Since the 1990s high-frequency, high-precision, in situ HCFC-22 measurements have been collected at these AGAGE stations. Since 1992, the Global Monitoring Division of the National Oceanic and Atmospheric Administration/Earth System Research Laboratory (NOAA/ESRL) has also collected flasks on a weekly basis from remote sites across the globe and analyzed them for a suite of halocarbons including HCFC-22. Additionally, since 2006 flasks have been collected approximately daily at a number of tower sites across the US and analyzed for halocarbons and other gases at NOAA. All results show an increase in the atmospheric mole fractions of HCFC-22, and recent data show a growth rate of approximately 4% per year, resulting in an increase in the background atmospheric mole fraction by a factor of 1.7 from 1995 to 2009. Using data on HCFC-22 consumption submitted to the United Nations Environment Programme (UNEP), as well as existing bottom-up emission estimates, we first create globally-gridded a priori HCFC-22 emissions over the 15 yr since 1995. We then use the three-dimensional chemical transport model, Model for Ozone and Related Chemical Tracers version 4 (MOZART v4), and a Bayesian inverse method to estimate global as well as regional annual emissions. Our inversion indicates that the global HCFC

Biologically produced molecular hydrogen (H-2) is characterised by a very strong depletion in deuterium. Although the biological source to the atmosphere is small compared to photochemical or combustion sources, it makes an important contribution to the global isotope budget of H-2. Large uncertainties exist in the quantification of the individual production and degradation processes that contribute to the atmospheric budget, and isotope measurements are a tool to distinguish the contributions from the different sources. Measurements of delta D from the various H-2 sources are scarce and for biologically produced H-2 only very few measurements exist. Here the first systematic study of the isotopic composition of biologically produced H-2 is presented. In a first set of experiments, we investigated delta D of H-2 produced in a biogas plant, covering different treatments of biogas production. In a second set of experiments, we investigated pure cultures of several H-2 producing microorganisms such as bacteria or green algae. A Keeling plot analysis provides a robust overall source signature of delta D = -712 parts per thousand (+/-13 parts per thousand) for the samples from the biogas reactor (at 38 degrees C, delta D-H2O = +73.4 parts per thousand), with a fractionation constant epsilon H-2-H2O of -689 parts per thousand (+/-20 parts per thousand) between H-2 and the water. The five experiments using pure culture samples from different microorganisms give a mean source signature of delta D = -728 parts per thousand (+/-28 parts per thousand), and a fractionation constant epsilon H-2-H2O of -711 parts per thousand (+/-34 parts per thousand) between H-2 and the water. The results confirm the massive deuterium depletion of biologically produced H-2 as was predicted by the calculation of the thermodynamic fractionation factors for hydrogen exchange between H-2 and water vapour. Systematic errors in the isotope scale are difficult to assess in the absence of international