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History of chemically and radiatively important atmospheric gases from the Advanced Global Atmospheric Gases Experiment (AGAGE)

Prinn, Ronald G.; Weiss, Ray F.; Arduini, Jgor; Arnold, Tim; DeWitt, H. Langley; Fraser, Paul J.; Ganesan, Anita L.; Gasore, Jimmy; Harth, Christina M.; Hermansen, Ove; Kim, Jooil; Krummel, Paul B.; Li, Shanlan; Loh, Zöe M.; Lunder, Chris Rene; Maione, Michela; Manning, Alistair J.; Miller, Ben R.; Mitrevski, Blagoj; Muhle, Jens; O'Doherty, Simon; Park, Sunyoung; Reimann, Stefan; Rigby, Matt; Saito, Takuya; Salameh, Peter K.; Schmidt, Roland; Simmonds, Peter G.; Steele, L. Paul; Vollmer, Martin K.; Wang, Ray H.; Yao, Bo; Yokouchi, Yoko; Young, Dickon; Zhou, Lingxi

We present the organization, instrumentation, datasets, data interpretation, modeling, and accomplishments of the multinational global atmospheric measurement program AGAGE (Advanced Global Atmospheric Gases Experiment). AGAGE is distinguished by its capability to measure globally, at high frequency, and at multiple sites all the important species in the Montreal Protocol and all the important non-carbon-dioxide (non-CO2) gases assessed by the Intergovernmental Panel on Climate Change (CO2 is also measured at several sites). The scientific objectives of AGAGE are important in furthering our understanding of global chemical and climatic phenomena. They are the following: (1) to accurately measure the temporal and spatial distributions of anthropogenic gases that contribute the majority of reactive halogen to the stratosphere and/or are strong infrared absorbers (chlorocarbons, chlorofluorocarbons – CFCs, bromocarbons, hydrochlorofluorocarbons – HCFCs, hydrofluorocarbons – HFCs and polyfluorinated compounds (perfluorocarbons – PFCs), nitrogen trifluoride – NF3, sulfuryl fluoride – SO2F2, and sulfur hexafluoride – SF6) and use these measurements to determine the global rates of their emission and/or destruction (i.e., lifetimes); (2) to accurately measure the global distributions and temporal behaviors and determine the sources and sinks of non-CO2 biogenic–anthropogenic gases important to climate change and/or ozone depletion (methane – CH4, nitrous oxide – N2O, carbon monoxide – CO, molecular hydrogen – H2, methyl chloride – CH3Cl, and methyl bromide – CH3Br); (3) to identify new long-lived greenhouse and ozone-depleting gases (e.g., SO2F2, NF3, heavy PFCs (C4F10, C5F12, C6F14, C7F16, and C8F18) and hydrofluoroolefins (HFOs; e.g., CH2 = CFCF3) have been identified in AGAGE), initiate the real-time monitoring of these new gases, and reconstruct their past histories from AGAGE, air archive, and firn air measurements; (4) to determine the average concentrations and trends of tropospheric hydroxyl radicals (OH) from the rates of destruction of atmospheric trichloroethane (CH3CCl3), HFCs, and HCFCs and estimates of their emissions; (5) to determine from atmospheric observations and estimates of their destruction rates the magnitudes and distributions by region of surface sources and sinks of all measured gases; (6) to provide accurate data on the global accumulation of many of these trace gases that are used to test the synoptic-, regional-, and global-scale circulations predicted by three-dimensional models; and (7) to provide global and regional measurements of methane, carbon monoxide, and molecular hydrogen and estimates of hydroxyl levels to test primary atmospheric oxidation pathways at midlatitudes and the tropics. Network Information and Data Repository: http://agage.mit.edu/data or http://cdiac.ess-dive.lbl.gov/ndps/alegage.html (https://doi.org/10.3334/CDIAC/atg.db1001).

2018

Discrepancy between simulated and observed ethane and propane levels explained by underestimated fossil emissions

Dalsøren, Stig Bjørløw; Myhre, Gunnar; Hodnebrog, Øivind; Myhre, Cathrine Lund; Stohl, Andreas; Pisso, Ignacio; Schwietzke, Stefan; Höglund-Isaksson, Lena; Helmig, Detlev; Reimann, Stefan; Sauvage, Stéphane; Schmidbauer, Norbert; Read, Katie A.; Carpenter, Lucy J.; Lewis, Alastair C.; Punjabi, Shalini; Wallasch, Markus

2018

Recent Arctic ozone depletion: Is there an impact of climate change?

Pommereau, Jean-Pierre; Goutail, Florence; Pazmino, Andrea; Lefèvre, Franck; Chipperfield, Martyn P.; Feng, Wuhu; Roozendael, Michel van; Jepsen, Nis; Hansen, Georg; Kivi, Rigel; Bognar, Kristof; Strong, Kimberly; Walker, Kaley; Kuzmichev, Alexandr; Khattatov, Slava; Sitnikova, Vera

After the well-reported record loss of Arctic stratospheric ozone of up to 38% in the winter 2010–2011, further large depletion of 27% occurred in the winter 2015–2016. Record low winter polar vortex temperatures, below the threshold for ice polar stratospheric cloud (PSC) formation, persisted for one month in January 2016. This is the first observation of such an event and resulted in unprecedented dehydration/denitrification of the polar vortex. Although chemistry–climate models (CCMs) generally predict further cooling of the lower stratosphere with the increasing atmospheric concentrations of greenhouse gases (GHGs), significant differences are found between model results indicating relatively large uncertainties in the predictions. The link between stratospheric temperature and ozone loss is well understood and the observed relationship is well captured by chemical transport models (CTMs). However, the strong dynamical variability in the Arctic means that large ozone depletion events like those of 2010–2011 and 2015–2016 may still occur until the concentrations of ozone-depleting substances return to their 1960 values. It is thus likely that the stratospheric ozone recovery, currently anticipated for the mid-2030s, might be significantly delayed. Most important in order to predict the future evolution of Arctic ozone and to reduce the uncertainty of the timing for its recovery is to ensure continuation of high-quality ground-based and satellite ozone observations with special focus on monitoring the annual ozone loss during the Arctic winter.

2018

Variability in Atmospheric Methane From Fossil Fuel and Microbial Sources Over the Last Three Decades

Thompson, Rona Louise; Nisbet, E. G.; Pisso, Ignacio; Stohl, Andreas; Blake, D.; Dlugokencky, E. J.; Helmig, D.; White, J. W. C.

Atmospheric measurements show an increase in CH4 from the 1980s to 1998 followed by a period of near‐zero growth until 2007. However, from 2007, CH4 has increased again. Understanding the variability in CH4 is critical for climate prediction and climate change mitigation. We examine the role of CH4 sources and the dominant CH4 sink, oxidation by the hydroxyl radical (OH), in atmospheric CH4 variability over the past three decades using observations of CH4, C2H6, and δ13CCH4 in an inversion. From 2006 to 2014, microbial and fossil fuel emissions increased by 36 ± 12 and 15 ± 8 Tg y−1, respectively. Emission increases were partially offset by a decrease in biomass burning of 3 ± 2 Tg y−1 and increase in soil oxidation of 5 ± 6 Tg y−1. A change in the atmospheric sink did not appear to be a significant factor in the recent growth of CH4.

2018

Developmental toxicity of perfluorooctanesulfonate (PFOS) and its chlorinated polyfluoroalkyl ether sulfonate alternative F-53B in the domestic chicken

Briels, Nathalie; Ciesielski, Tomasz Maciej; Herzke, Dorte; Jaspers, Veerle

The chlorinated polyfluoroalkyl ether sulfonate F-53B is used as a mist suppressant in the Chinese electroplating industry. Because of the regulations on perfluorooctanesulfonate (PFOS), its use is expected to increase. Until now, F-53B toxicity data have been scarce and are, to our knowledge, lacking for birds. This study therefore investigated the effects of PFOS and F-53B, separately and as mixtures, on the development of the chicken (Gallus gallus domesticus). Compounds were injected in ovo, before incubation, at 150 and 1500 ng/g egg. At embryonic day 20, a significantly lower heart rate was observed in all treated groups compared to the control group and hatchlings exposed to the high dose of F-53B had a significantly enlarged liver (8%). Embryonic survival was not affected and no significant effects on hatchling body mass or oxidative stress parameters were found. Our results suggest that these compounds likely have different toxicity thresholds for the investigated endpoints, and/or different modes of action. This study thereby underlines the potential developmental toxicity of PFOS and F-53B at environmentally relevant concentrations. Assessment of PFOS alternatives should therefore continue, preferably prior to their large scale use, as they should be ensured to be less harmful than PFOS itself.

2018

A DPSIR-analysis of water uses and related water quality issues in the Colombian Alto and Medio Dagua Community Council

Gari, Sirak Robele; Guerrero, Cesar E. Ortiz; A-Uribe, Bryann; Icely, John D.; Newton, Alice

A portion of Colombia’s water resources is located on the Pacific coast within the territory of the Community Council of Alto and Medio Dagua (CC-AMDA). Though a harmonious balance between the communities’ subsistent activities and nature was maintained for centuries, the appearance of modern modes of resource extraction has negatively affected the environment, especially the water resources. The Driver-Pressure-State- Impact-Response (DPSIR) framework was used to analyze water quality problems within this community council. The DPSIR analysis revealed that agriculture, mining, logging and infrastructure development constitute important sectoral drivers with some contribution from tourism and fisheries. Pressures included inputs of organic matter, sediment, nutrients and chemical contaminants to the Dagua river, and to the Bay of Buenaventura. These produced corresponding State changes in the water bodies. Impacts on human welfare were poor public health, reduced food and water security, economic loss and some displacement. Societal Responses included public protests and campaigns, legal actions and policy changes for improved governance. As a future policy option, the formation of community-based water resources management is recommended. Though DPSIR was able to link cause-effect relations, further empirical research on these water bodies is necessary to fill in existing gaps in the data set, particularly for public health threatening contaminants.

2018

Modeling the Time-Variant Dietary Exposure of PCBs in China over the Period 1930 to 2100

Zhao, Shizhen; Breivik, Knut; Jones, Kevin C; Sweetman, Andrew J

This study aimed for the first time to reconstruct historical exposure profiles for PCBs to the Chinese population, by examining the combined effect of changing temporal emissions and dietary transition. A long-term (1930–2100) dynamic simulation of human exposure using realistic emission scenarios, including primary emissions, unintentional emissions, and emissions from e-waste, combined with dietary transition trends was conducted by a multimedia fate model (BETR-Global) linked to a bioaccumulation model (ACC-HUMAN). The model predicted an approximate 30-year delay of peak body burden for PCB-153 in a 30-year-old Chinese female, compared to their European counterpart. This was mainly attributed to a combination of change in diet and divergent emission patterns in China. A fish-based diet was predicted to result in up to 8 times higher body burden than a vegetable-based diet (2010–2100). During the production period, a worst-case scenario assuming only consumption of imported food from a region with more extensive production and usage of PCBs would result in up to 4 times higher body burden compared to consumption of only locally produced food. However, such differences gradually diminished after cessation of production. Therefore, emission reductions in China alone may not be sufficient to protect human health from PCB-like chemicals, particularly during the period of mass production. The results from this study illustrate that human exposure is also likely to be dictated by inflows of PCBs via the environment, waste, and food.

2018

Observation of turbulent dispersion of artificially released SO2 puffs with UV cameras

Dinger, Anna Solvejg; Stebel, Kerstin; Cassiani, Massimo; Ardeshiri, Hamidreza; Bernardo, Cirilo; Kylling, Arve; Park, Soon-Young; Pisso, Ignacio; Schmidbauer, Norbert; Wasseng, Jan Henrik; Stohl, Andreas

In atmospheric tracer experiments, a substance is released into the turbulent atmospheric flow to study the dispersion parameters of the atmosphere. That can be done by observing the substance's concentration distribution downwind of the source. Past experiments have suffered from the fact that observations were only made at a few discrete locations and/or at low time resolution. The Comtessa project (Camera Observation and Modelling of 4-D Tracer Dispersion in the Atmosphere) is the first attempt at using ultraviolet (UV) camera observations to sample the three-dimensional (3-D) concentration distribution in the atmospheric boundary layer at high spatial and temporal resolution. For this, during a three-week campaign in Norway in July 2017, sulfur dioxide (SO2), a nearly passive tracer, was artificially released in continuous plumes and nearly instantaneous puffs from a 9m high tower. Column-integrated SO2 concentrations were observed with six UV SO2 cameras with sampling rates of several hertz and a spatial resolution of a few centimetres. The atmospheric flow was characterised by eddy covariance measurements of heat and momentum fluxes at the release mast and two additional towers. By measuring simultaneously with six UV cameras positioned in a half circle around the release point, we could collect a data set of spatially and temporally resolved tracer column densities from six different directions, allowing a tomographic reconstruction of the 3-D concentration field. However, due to unfavourable cloudy conditions on all measurement days and their restrictive effect on the SO2 camera technique, the presented data set is limited to case studies. In this paper, we present a feasibility study demonstrating that the turbulent dispersion parameters can be retrieved from images of artificially released puffs, although the presented data set does not allow for an in-depth analysis of the obtained parameters. The 3-D trajectories of the centre of mass of the puffs were reconstructed enabling both a direct determination of the centre of mass meandering and a scaling of the image pixel dimension to the position of the puff. The latter made it possible to retrieve the temporal evolution of the puff spread projected to the image plane. The puff spread is a direct measure of the relative dispersion process. Combining meandering and relative dispersion, the absolute dispersion could be retrieved. The turbulent dispersion in the vertical is then used to estimate the effective source size, source timescale and the Lagrangian integral time. In principle, the Richardson–Obukhov constant of relative dispersion in the inertial subrange could be also obtained, but the observation time was not sufficiently long in comparison to the source timescale to allow an observation of this dispersion range. While the feasibility of the methodology to measure turbulent dispersion could be demonstrated, a larger data set with a larger number of cloud-free puff releases and longer observation times of each puff will be recorded in future studies to give a solid estimate for the turbulent dispersion under a variety of stability conditions.

2018

hackAIR: Towards raising awareness about air quality in Europe by developing a collective online platform

Kosmidis, Evangelos; Syropoulou, Panagiota; Tekes, Stavros; Schneider, Philipp; Spyromitros-Xioufis, Eleftherios; Riga, Marina; Charitidis, Polychronis; Moumtzidou, Anastasia; Papadopoulos, Symeon; Vrochidis, Stefanos; Kompatsiaris, Ioannis; Stavrakas, Ilias; Hloupis, George; Loukidis, Andronikos; Kourtidis, Konstantinos; Georgoulias, Aristeidis K.; Alexandri, Georgia

Although air pollution is one of the most significant environmental factors posing a threat to human health worldwide, air quality data are scarce or not easily accessible in most European countries. The current work aims to develop a centralized air quality data hub that enables citizens to contribute to air quality monitoring. In this work, data from official air quality monitoring stations are combined with air pollution estimates from sky-depicting photos and from low-cost sensing devices that citizens build on their own so that citizens receive improved information about the quality of the air they breathe. Additionally, a data fusion algorithm merges air quality information from various sources to provide information in areas where no air quality measurements exist.

2018

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