scholarly journals Intrusion, retention, and snowpack chemical effects from exhaust emissions at Concordia Station, Antarctica

2018 ◽  
Author(s):  
Detlev Helmig ◽  
Daniel Liptzin ◽  
Jacques Hueber ◽  
Joel Savarino

Abstract. Continuous measurements of reactive gases in the snowpack and above the snowpack surface were conducted at Concordia Station (Dome C), Antarctica, from December 2012–January 2014. Measured species included ozone, nitrogen oxides, gaseous elemental mercury, and formaldehyde, for study of photochemical reactions, surface exchange, and the seasonal cycles and atmospheric chemistry of these gases. The experiment was installed ~ 1 km from the main station infrastructure inside the station clean air sector and within the station electrical power grid boundary. Air was sampled continuously from three inlets on a 10 m meteorological tower, as well as from two above and four below the surface sampling inlets from within the snowpack. Despite being in the clean air sector, over the course of the 1.2-year study, we observed on the order of 15 occasions when exhaust plumes from the camp, most notably from the power generation system, were transported to the study site. Highly elevated levels of nitrogen oxides (up to 1000 x background) and lowered ozone (down to ~ 50 %), most likely from titration with nitric oxide, were measured in the exhaust plumes. Within 5–15 minutes from observing elevated pollutant levels above the snow, rapidly increasing and long-lasting concentration enhancements were measured in snowpack air. While pollution events typically lasted only a few minutes to an hour above the snow surface, elevated nitrogen oxides levels were observed in the snowpack lasting from a few days to one week. These observations add important new insight to the discussion of if and how snow-photochemical experiments within reach of the power grid of polar research sites are possibly compromised by the snowpack being chemically influenced (contaminated) by gaseous and particulate emissions from the research camp activities. This question is critical for evaluating if snowpack trace chemical measurements from within the camp boundaries are representative for the vast polar ice sheets.

2020 ◽  
Vol 14 (1) ◽  
pp. 199-209 ◽  
Author(s):  
Detlev Helmig ◽  
Daniel Liptzin ◽  
Jacques Hueber ◽  
Joel Savarino

Abstract. The chemistry of reactive gases inside the snowpack and in the lower atmosphere was investigated at Concordia Station (Dome C), Antarctica, from December 2012 to January 2014. Measured species included ozone, nitrogen oxides, gaseous elemental mercury (GEM), and formaldehyde, for study of photochemical reactions, surface exchange, and the seasonal cycles and atmospheric chemistry of these gases. The experiment was installed ≈1 km from the station main infrastructure inside the station clean air sector and within the station electrical power grid boundary. Ambient air was sampled continuously from inlets mounted above the surface on a 10 m meteorological tower. In addition, snowpack air was collected at 30 cm intervals to 1.2 m depth from two manifolds that had both above- and below-surface sampling inlets. Despite being in the clean air sector, over the course of the 1.2-year study, we observed on the order of 50 occasions when exhaust plumes from the camp, most notably from the power generation system, were transported to the study site. Continuous monitoring of nitrogen oxides (NOx) provided a measurement of a chemical tracer for exhaust plumes. Highly elevated levels of NOx (up to 1000 × background) and lowered ozone (down to ≈50 %), most likely from reaction of ozone with nitric oxide, were measured in air from above and within the snowpack. Within 5–15 min from observing elevated pollutant levels above the snow, rapidly increasing and long-lasting concentration enhancements were measured in snowpack air. While pollution events typically lasted only a few minutes to an hour above the snow surface, elevated NOx levels were observed in the snowpack lasting from a few days to ≈ 1 week. GEM and formaldehyde measurements were less sensitive and covered a shorter measurement period; neither of these species' data showed noticeable concentration changes during these events that were above the normal variability seen in the data. Nonetheless, the clarity of the NOx and ozone observations adds important new insight into the discussion of if and how snow photochemical experiments within reach of the power grid of polar research sites are possibly compromised by the snowpack being chemically influenced (contaminated) by gaseous and particulate emissions from the research camp activities. This question is critical for evaluating if snowpack trace chemical measurements from within the camp boundaries are representative for the vast polar ice sheets.


1976 ◽  
Vol 10 (9) ◽  
pp. 934-936 ◽  
Author(s):  
B. Dimitriades ◽  
M. C. Dodge ◽  
J. J. Bufalini ◽  
K. L. Demerjian ◽  
A. P. Altshuller

2017 ◽  
Vol 200 ◽  
pp. 693-703 ◽  
Author(s):  
Jos Lelieveld

In atmospheric chemistry, interactions between air pollution, the biosphere and human health, often through reaction mixtures from both natural and anthropogenic sources, are of growing interest. Massive pollution emissions in the Anthropocene have transformed atmospheric composition to the extent that biogeochemical cycles, air quality and climate have changed globally and partly profoundly. It is estimated that mortality attributable to outdoor air pollution amounts to 4.33 million individuals per year, associated with 123 million years of life lost. Worldwide, air pollution is the major environmental risk factor to human health, and strict air quality standards have the potential to strongly reduce morbidity and mortality. Preserving clean air should be considered a human right, and is fundamental to many sustainable development goals of the United Nations, such as good health, climate action, sustainable cities, clean energy, and protecting life on land and in the water. It would be appropriate to adopt “clean air” as a sustainable development goal.


Atmosphere ◽  
2020 ◽  
Vol 11 (7) ◽  
pp. 685
Author(s):  
Fanxiu Li ◽  
Hengyuan Wang ◽  
Xuezhong Wang ◽  
Zhigang Xue ◽  
Liqin Duan ◽  
...  

Atmospheric carbonyls (aldehyde and ketone compounds) can be precursors for ozone and PM2.5, and they play an essential role in atmospheric chemistry. Linfen is a basin between mountains on the east and west, and there are many coking plants on the north and south sides of its urban area. The special topography and unfortunate industrial layout have frequently contributed to serious air pollution in Linfen. In order to investigate the pollution characteristics of atmospheric carbonyls in winter in urban Linfen, the carbonyl compounds were collected from the Municipal Committee site (MC) and the Yaowangtai site (YWT) from 16 to 25 January 2019, and their concentrations were analyzed by a high performance liquid chromatography-ultraviolet detector (HPLC-UV). The results show that formaldehyde, acetaldehyde, and acetone were the most abundant compounds, accounting for more than 70% of the total mass concentration of carbonyls in urban Linfen. Levels of these three carbonyls increased during the morning and evening traffic rush hours. The mass concentration of formaldehyde at both sites reached peak values at around noon (10:00–14:00). In addition, the mass concentrations of formaldehyde, acetaldehyde, and acetone were positively correlated with CO mass concentrations, whereas only formaldehyde and acetaldehyde were positively correlated with temperature. Therefore, atmospheric formaldehyde in urban Linfen’s winter mainly came from vehicle exhaust emissions and the secondary generation of photochemical reactions. Most of the acetaldehyde came from vehicle exhaust emissions, and photochemical reactions also partially contributed to it. For acetone, vehicle exhaust emissions were the main source. In addition, coking industry emissions from Northern Linfen′s Hongtong County may also have contributed to the atmospheric carbonyls in the urban area of Linfen. For the first time, this study found that formaldehyde showed different behavior to acetaldehyde and acetone; that is, the nighttime decrease in formaldehyde mass concentration was greater than that of acetaldehyde and acetone.


2005 ◽  
Vol 5 (4) ◽  
pp. 6295-7168 ◽  
Author(s):  
R. Atkinson ◽  
D. L. Baulch ◽  
R. A. Cox ◽  
J. N. Crowley ◽  
R. F. Hampson ◽  
...  

Abstract. This article, the second in the series, presents kinetic and photochemical data evaluated by the IUPAC Subcommittee on Gas Kinetic Data Evaluation for Atmospheric Chemistry. It covers the gas phase and photochemical reactions of Organic species, which were last published in 1999, and were updated on the IUPAC website in late 2002. The article consists of a summary sheet, containing the recommended kinetic parameters for the evaluated reactions, and eight appendices containing the data sheets, which provide information upon which the recommendations are made.


2007 ◽  
Vol 4 (4) ◽  
pp. 238 ◽  
Author(s):  
S. Morin ◽  
J. Savarino ◽  
S. Bekki ◽  
A. Cavender ◽  
P. B. Shepson ◽  
...  

Environmental context. Ozone depletion events (ODEs) in the Arctic lower atmosphere drive profound changes in the chemistry of nitrogen oxides (NOx) because of the presence of bromine oxide (BrO). These are investigated using the isotopic composition of atmospheric nitrate (NO3–), which is a ubiquitous species formed through the oxidation of nitrogen oxides. Since BrO is speculated to play a key role in the atmospheric chemistry of marine regions and in the free troposphere, our studies contribute to the improvement of the scientific knowledge on this new topic in atmospheric chemistry. Abstract. The triple oxygen isotopic composition of atmospheric inorganic nitrate was measured in samples collected in the Arctic in springtime at Alert, Nunavut and Barrow, Alaska. The isotope anomaly of nitrate (Δ17O = δ17O–0.52δ18O) was used to probe the influence of ozone (O3), bromine oxide (BrO), and peroxy radicals (RO2) in the oxidation of NO to NO2, and to identify the dominant pathway that leads to the production of atmospheric nitrate. Isotopic measurements confirm that the hydrolysis of bromine nitrate (BrONO2) is a major source of nitrate in the context of ozone depletion events (ODEs), when brominated compounds primarily originating from sea salt catalytically destroy boundary layer ozone. They also show a case when BrO is the main oxidant of NO into NO2.


2019 ◽  
Author(s):  
Yugo Kanaya ◽  
Kazuyo Yamaji ◽  
Takuma Miyakawa ◽  
Fumikazu Taketani ◽  
Chunmao Zhu ◽  
...  

Abstract. A long-term, robust observational record of atmospheric black carbon (BC) concentrations at Fukue Island for 2009–2019 was produced by unifying data from a continuous soot-monitoring system and a multi-angle absorption photometer. This record was then used to analyze emission trends from China. We identified a rapid reduction in BC concentrations of (−5.8 ± 1.5) % y−1 or −48 % from 2010 to 2018. We concluded that an emission change of (−5.3 ± 0.7) % y−1, related to changes in China of as much as −4.6 % y−1, was the main underlying driver. This evaluation was made after correcting for the interannual meteorological variability, by using regional atmospheric chemistry model simulations (WRF/CMAQ) with constant emissions. This resolves current fundamental disagreements about the sign of the BC emission trend from China over the past decade, assessed from bottom-up emission inventories; our analysis supported inventories reflecting the governmental clean air actions after 2010 (e.g., MEIC1.3, ECLIPSE v5a and v6b, and REAS updated) and recommended revision to those not (e.g., CEDS). Our estimated emission trends were fairly uniform over seasons but diverse among air-mass origins. Stronger BC reductions occurred in regions of South-Central East China, accompanied by CO emission reduction, while weaker BC reductions occurred in North-Central East China and Northeast China. Prior to 2017, the BC and CO emission trends were both unexpectedly positive in Northeast China during winter months, possibly influencing climate at higher latitudes. The pace of emission reduction over China surpasses those of SSP1 scenarios (SSP: shared socioeconomic pathways) for 2015–2030, suggesting highly successful emission control policies. At Fukue Island, the BC fraction of PM2.5 also steadily decreased over the last decade, suggesting that BC emission reduction started without significant delay with respect to other pollutants, such as NOx and SO2, which are among key precursors of scattering PM2.5.


1976 ◽  
Vol 10 (9) ◽  
pp. 936-937 ◽  
Author(s):  
H. E. Jeffries ◽  
M. Saeger

2015 ◽  
Vol 15 (14) ◽  
pp. 7859-7875 ◽  
Author(s):  
M. M. Frey ◽  
H. K. Roscoe ◽  
A. Kukui ◽  
J. Savarino ◽  
J. L. France ◽  
...  

Abstract. Mixing ratios of the atmospheric nitrogen oxides NO and NO2 were measured as part of the OPALE (Oxidant Production in Antarctic Lands & Export) campaign at Dome C, East Antarctica (75.1° S, 123.3° E, 3233 m), during December 2011 to January 2012. Profiles of NOx mixing ratios of the lower 100 m of the atmosphere confirm that, in contrast to the South Pole, air chemistry at Dome C is strongly influenced by large diurnal cycles in solar irradiance and a sudden collapse of the atmospheric boundary layer in the early evening. Depth profiles of mixing ratios in firn air suggest that the upper snowpack at Dome C holds a significant reservoir of photolytically produced NO2 and is a sink of gas-phase ozone (O3). First-time observations of bromine oxide (BrO) at Dome C show that mixing ratios of BrO near the ground are low, certainly less than 5 pptv, with higher levels in the free troposphere. Assuming steady state, observed mixing ratios of BrO and RO2 radicals are too low to explain the large NO2 : NO ratios found in ambient air, possibly indicating the existence of an unknown process contributing to the atmospheric chemistry of reactive nitrogen above the Antarctic Plateau. During 2011–2012, NOx mixing ratios and flux were larger than in 2009–2010, consistent with also larger surface O3 mixing ratios resulting from increased net O3 production. Large NOx mixing ratios at Dome C arise from a combination of continuous sunlight, shallow mixing height and significant NOx emissions by surface snow (FNOx). During 23 December 2011–12 January 2012, median FNOx was twice that during the same period in 2009–2010 due to significantly larger atmospheric turbulence and a slightly stronger snowpack source. A tripling of FNOx in December 2011 was largely due to changes in snowpack source strength caused primarily by changes in NO3− concentrations in the snow skin layer, and only to a secondary order by decrease of total column O3 and associated increase in NO3− photolysis rates. A source of uncertainty in model estimates of FNOx is the quantum yield of NO3− photolysis in natural snow, which may change over time as the snow ages.


1976 ◽  
Vol 10 (2) ◽  
pp. 150-153 ◽  
Author(s):  
William L. Chameides ◽  
Donald H. Stedman

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