scholarly journals The role of long-range transport and domestic emissions in determining atmospheric secondary inorganic particle concentrations across the UK

2014 ◽  
Vol 14 (16) ◽  
pp. 8435-8447 ◽  
Author(s):  
M. Vieno ◽  
M. R. Heal ◽  
S. Hallsworth ◽  
D. Famulari ◽  
R. M. Doherty ◽  
...  

Abstract. Surface concentrations of secondary inorganic particle components over the UK have been analysed for 2001–2010 using the EMEP4UK regional atmospheric chemistry transport model and evaluated against measurements. Gas/particle partitioning in the EMEP4UK model simulations used a bulk approach, which may lead to uncertainties in simulated secondary inorganic aerosol. However, model simulations were able to accurately represent both the long-term decadal surface concentrations of particle sulfate and nitrate and an episode in early 2003 of substantially elevated nitrate measured across the UK by the AGANet network. The latter was identified as consisting of three separate episodes, each of less than 1 month duration, in February, March and April. The primary cause of the elevated nitrate levels across the UK was meteorological: a persistent high-pressure system, whose varying location impacted the relative importance of transboundary versus domestic emissions. Whilst long-range transport dominated the elevated nitrate in February, in contrast it was domestic emissions that mainly contributed to the March episode, and for the April episode both domestic emissions and long-range transport contributed. A prolonged episode such as the one in early 2003 can have substantial impact on annual average concentrations. The episode led to annual concentration differences at the regional scale of similar magnitude to those driven by long-term changes in precursor emissions over the full decade investigated here. The results demonstrate that a substantial part of the UK, particularly the south and southeast, may be close to or exceeding annual mean limit values because of import of inorganic aerosol components from continental Europe under specific conditions. The results reinforce the importance of employing multiple year simulations in the assessment of emissions reduction scenarios on particulate matter concentrations and the need for international agreements to address the transboundary component of air pollution.

2013 ◽  
Vol 13 (12) ◽  
pp. 33433-33462
Author(s):  
M. Vieno ◽  
M. R. Heal ◽  
S. Hallsworth ◽  
D. Famulari ◽  
R. M. Doherty ◽  
...  

Abstract. Surface concentrations of secondary inorganic particle components over the UK have been analysed for 2001–2010 using the EMEP4UK regional atmospheric chemistry transport model. In early 2003 an episode of substantially elevated surface concentrations of ammonium nitrate was measured across the UK by the AGANET network. The EMEP4UK model was able accurately to represent both the long-term decadal surface concentrations and the episode in 2003. The latter was identified as consisting of three separate episodes, each of less than 1 month duration, in February, March and April. The primary cause of the elevated nitrate levels across the UK was meteorological, a persistent high pressure system, but whose varying location impacted the relative importance of transboundary vs. domestic emissions. Whilst long-range transport dominated the elevated nitrate in February, in contrast it was domestic emissions that mainly contributed to the March episode, and for the April episode both domestic emissions and long-range transport contributed. A prolonged episode such as the one in early 2003 can have substantial impact on annual average concentrations. The episode led to annual concentration differences at the regional scale of similar magnitude to those driven by long-term changes in precursor emissions over the full decade investigated here. The results demonstrate that a substantial part of the UK, particularly the south and south-east, may be close to or actually exceeding annual mean limit values because of import of inorganic aerosol components from continental Europe under specific conditions. The results reinforce the importance of employing multiple year simulations in the assessment of emissions reduction scenarios on PM concentrations and the need for international agreements to address the transboundary component of air pollution.


2000 ◽  
Vol 18 (11) ◽  
pp. 1447-1466 ◽  
Author(s):  
D. S. Lee ◽  
R. D. Kingdon ◽  
J. A. Garland ◽  
B. M. R. Jones

Abstract. Orographic enhancement of wet deposition arising from the 'seeder-feeder' effect is, by necessity, highly parametrised in long-range transport models of acid deposition that are long-term (i.e. annual average) and spatially resolved at tens of kilometres. Here, we describe a mechanistic approach to the incorporation of these mechanisms into such a model. The model formulation required the following: precipitation rate by direction and quantification of the fractions that are orographic and non-orographic; treatment of the fast oxidation of sulfur dioxide in clouds; the directionality of the seeder-feeder process; and a quantitative basis for increasing wet deposition factors to account for the seeder-feeder process. The directionality of non-orographic precipitation was determined from meteorological data at 47 sites across the UK. Orographic precipitation varies on a much finer scale than can be interpolated from measurements, and thus a modelling approach was adopted. The directionality of the seeder-feeder effect was taken from measurements. The enhancement factor of the orographic component of precipitation, assumed to represent feeder-rain, was determined from a review of measurements. Fast oxidation of sulfur dioxide is an observed phenomenon in cap-cloud, but limited in duration. An adjustment was made to the sulfur dioxide oxidation rate in the model in locations where cap-cloud was assumed to be present. The results from the model were compared with UK deposition budgets and enhanced wet deposition maps. The revised parametrisation underestimated the UK wet deposition budgets of oxidised N and S, but spatial patterns of deposition were improved for much of the UK. It was concluded that this was a satisfactory outcome given the constraints of the statistical approach of weighting of deposition at receptors utilising straight line trajectories. The sensitivity of the model to directional constraints of seeder-feeder enhancement was tested and it was concluded that a fairly narrow constraint resulted in similar estimations to a broader one, and the broader constraint was thus adopted as frontal conditions which result in the process arrive from a fairly broad band of directions. When enhancement was allowed to occur from all directions, UK wet deposition of oxidised N and S was increased by 10%. The sensitivity to the enhancement factor on wet deposition was tested and found to be relatively robust. An increase in the enhancement factor from 2 to 6 resulted in increases in UK wet deposition of oxidised N and S of 9 and 6%, respectively.Key words: Atmospheric composition and structure (pollution – urban and regional) – Meteorology and atmospheric dynamics (precipitation)


Atmosphere ◽  
2019 ◽  
Vol 10 (2) ◽  
pp. 59 ◽  
Author(s):  
Chunshui Lin ◽  
Darius Ceburnis ◽  
Ru-Jin Huang ◽  
Francesco Canonaco ◽  
André Prévôt ◽  
...  

The chemical composition and sources of non-refractory submicron aerosol (NR-PM1) on Galway, a west coast city of Ireland, were characterized using an aerosol chemical speciation monitor during summertime in June 2016. Organic aerosol (OA) was found to be the major part of NR-PM1 (54%), followed by secondary inorganic sulfate (25%), ammonium (11%), and nitrate (10%). Factor analysis revealed that oxygenated OA (OOA) was the dominant OA factor, on average accounting for 84% of the total OA. The remaining 16% of OA was attributed to primary peat burning associated with domestic heating activities. As a result, secondary organic and inorganic aerosol together accounted for 91% of the total NR-PM1, pointing to an aged aerosol population originating from secondary formation during long-range transport. Concentration-weighted trajectory analysis indicated that these secondary aerosols were mainly associated with easterly long-range transport from the UK and/or France.


2017 ◽  
Author(s):  
Zhe Jiang ◽  
Helen Worden ◽  
John R. Worden ◽  
Daven K. Henze ◽  
Dylan B. A. Jones ◽  
...  

Abstract. Decreases in surface emissions of nitrogen oxides (NOx = NO + NO2) in North America have led to substantial improvements in air-quality over the last several decades. Here we show that satellite observations of tropospheric nitrogen dioxide (NO2) columns over the contiguous United States (US) do not decrease after about 2009, while surface NO2 concentrations continue to decline through to the present. This divergence, if it continues, could have a substantial impact on surface air quality due to mixing of free-tropospheric air into the boundary layer. Our results show only limited contributions from local effects such as fossil fuel emissions, lightning, or instrument artifacts, but we do find a possible relationship of NO2 changes to decadal climate variability. Our analysis demonstrates that the intensity of transpacific transport is stronger in El Niño years and weaker in La Niña years, and consequently, that decadal-scale climate variability impacts the contribution of Asian emissions on North American atmospheric composition. Because of the short lifetime, it is usually believed that the direct contribution of long-range transport to tropospheric NOx distribution is limited. If our hypothesis about transported Asian emissions is correct, then this observed divergence between satellite and surface NOx could indicate mechanisms that allow for either NOx or its reservoir species to have a larger than expected effect on North American tropospheric composition. These results therefore suggest more aircraft and satellite studies to determine the possible missing processes in our understanding of the long-range transport of tropospheric NOx.


2000 ◽  
Vol 10 (3) ◽  
pp. 229-238 ◽  
Author(s):  
Iain J. Beverland ◽  
Trygve Tunes ◽  
Malgorzata Sozanska ◽  
Robert A. Elton ◽  
Raymond M. Agius ◽  
...  

2008 ◽  
Vol 8 (18) ◽  
pp. 5551-5563 ◽  
Author(s):  
J. Sciare ◽  
K. Oikonomou ◽  
O. Favez ◽  
E. Liakakou ◽  
Z. Markaki ◽  
...  

Abstract. Long-term (5-year) measurements of Elemental Carbon (EC) and Organic Carbon (OC) in bulk aerosols are presented here for the first time in the Mediterranean Basin (Crete Island). A multi-analytical approach (including thermal, optical, and thermo-optical techniques) was applied for these EC and OC measurements. Light absorbing dust aerosols were shown to poorly contribute (+12% on a yearly average) to light absorption coefficient (babs) measurements performed by an optical method (aethalometer). Long-range transport of agricultural waste burning from European countries surrounding the Black Sea was shown for each year during two periods (March–April and July–September). The contribution of biomass burning to the concentrations of EC and OC was shown to be rather small (20 and 14%, respectively, on a yearly basis), although this contribution could be much higher on a monthly basis and showed important seasonal and interannual variability. By removing the biomass burning influence, our data revealed an important seasonal variation of OC, with an increase by almost a factor of two for the spring months of May and June, whereas BC was found to be quite stable throughout the year. Preliminary measurements of Water Soluble Organic Carbon (WSOC) have shown that the monthly mean WSOC/OC ratio remains stable throughout the year (0.45±0.12), suggesting that the partitioning between water soluble and water insoluble organic matter is not significantly affected by biomass burning and secondary organic aerosol (SOA) formation. A chemical mass closure performed in the fine mode (Aerodynamic Diameter, A.D.<1.5μm) showed that the mass contribution of organic matter (POM) was found to be essentially invariable during the year (monthly average of 26±5%).


2000 ◽  
Vol 34 (6) ◽  
pp. 881-894 ◽  
Author(s):  
A.L. Malcolm ◽  
R.G. Derwent ◽  
R.H. Maryon

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