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Four periods of EMEP (European Monitoring and Evaluation Programme) intensive measurement campaigns (June 2006, January 2007, September-October 2008 and February-March 2009) were modelled using the regional air quality model CAMx with VBS (Volatility Basis Set) approach for the first time in Europe within the framework of the EURODELTA-III model intercomparison exercise. More detailed analysis and sensitivity tests were performed for the period of February-March 2009 and June 2006 to investigate the uncertainties in emissions as well as to improve the modelling of organic aerosols (OA). Model performance for selected gas phase species and PM2.5 was evaluated using the European air quality database Airbase. Sulfur dioxide (SO2) and ozone (O3) were found to be overestimated for all the four periods with O3 having the largest mean bias during June 2006 and January-February 2007 periods (8.93 and 12.30 ppb mean biases, respectively). In contrast, nitrogen dioxide (NO2) and carbon monoxide (CO) were found to be underestimated for all the four periods. CAMx reproduced both total concentrations and monthly variations of PM2.5 very well for all the four periods with average biases ranging from -2.13 to 1.04 µg m-3. Comparisons with AMS (Aerosol Mass Spectrometer) measurements at different sites in Europe during February-March 2009, showed that in general the model over-predicts the inorganic aerosol fraction and under-predicts the organic one, such that the good agreement for PM2.5 is partly due to compensation of errors. The effect of the choice of volatility basis set scheme (VBS) on OA was investigated as well. Two sensitivity tests with volatility distributions based on previous chamber and ambient measurements data were performed. For February-March 2009 the chamber-case reduced the total OA concentrations by about 43 % on average. On the other hand, a test based on ambient measurement data increased OA concentrations by about 47 % for the same period bringing model and observations into better agreement. Comparison with the AMS data at the rural Swiss site Payerne in June 2006 shows no significant improvement in modelled OA concentration. Further sensitivity tests with increased biogenic and anthropogenic emissions suggest that OA in Payerne was largely dominated by residential heating emissions during the February-March 2009 period and by biogenic precursors in June 2006. [ABSTRACT FROM AUTHOR]

We use a three dimensional regional chemical transport model (PMCAMx) with high grid resolution and high resolution emissions (4km×4km) over the Paris greater area to simulate the formation of carbonaceous aerosol during a summer (July 2009) and a winter (January/February 2010) period as part of the MEGAPOLI (Megacities: Emissions, urban, regional, and Global Atmospheric POLlution and climate effects, and Integrated tools for assessment and mitigation) campaigns. Model predictions of carbonaceous aerosol are compared against Aerodyne aerosol mass spectrometer and black carbon (BC) high time resolution measurements from three ground sites. PM CAMx predicts BC concentrations reasonably well reproducing the majority (70%) of the hourly data within a factor of two during both periods. The agreement for the summertime secondary organic aerosol (OA) concentrations is also encouraging (mean bias= 0.1 μgm-3) during a photochemically intense period. The model tends to underpredict the summertime primary OA concentrations in the Paris greater area (by approximately 0.8 μgm-3) mainly due to missing primary OA emissions from cooking activities. The total cooking emissions are estimated to be approximately 80mgd-1 per capita and have a distinct diurnal profile in which 50%of the daily cooking OA is emitted during lunch time (12:00-14:00 LT) and 20% during dinner time (20:00-22:00 LT). Results also show a large underestimation of secondary OA in the Paris greater area during wintertime (mean bias= -2.3 μgm-3) pointing towards a secondary OA formation process during low photochemical activity periods that is not simulated in the model. [ABSTRACT FROM AUTHOR]

The EDGAR (Emissions Database for Global Atmospheric Research) v4.3 global anthropogenic emissions inventory of several gaseous (SO2, NOx, CO, non-methane volatile organic compounds (NMVOCs) and NH3) and particulate (PM10, PM2.5, black and organic carbon (BC and OC)) air pollutants for the period 1970-2010 is used to develop retrospective air pollution emission scenarios to quantify the roles and contributions of changes in fuels consumption, technology, end-of-pipe emission reduction measures and their resulting impact on health and crop yields. This database presents changes in activity data, fuels and air pollution abatement technology for the past 4 decades, using international statistics and following guidelines for bottom-up emission inventory at the Tier 1 and Tier 2 levels with region-specific default values. With two further retrospective scenarios we assess (1) the impact of the technology and end-of-pipe (EOP) reduction measures in the European Union (EU) by considering a stagnation of technology with constant emission factors from 1970 and with no further abatement measures and improvement in European emissions standards, but fuel consumption occurring at historical pace, and (2) the impact of increased fuel consumption by considering unchanged energy use with constant fuel consumption since 1970, but technological development and end-of-pipe reductions. Our scenario analysis focuses on the three most important and most regulated sectors (power generation, the manufacturing industry and road transport), which are subject of multi-pollutant EU Air Quality regulations. If technology and European EOP reduction measures had stagnated at 1970 levels, EU air quality in 2010 would have suffered from 129% higher SO2, 71 % higher NOx and 69% higher PM2.5 emissions, demonstrating the large role of technology in reducing emissions in 2010. However, if fuel consumption had remained constant starting in 1970, the EU would have benefited from current technology and emission control standards, with reductions in NOx by even 13% more. Such further savings are not observed for SO2 and PM2.5. If the EU consumed the same amount of fuels as in 1970 but with the current technology and emission control standards, then the emissions of SO2 and PM2.5 would be 42% respectively 10% higher. This scenario shows the importance for air quality of abandoning heavy residual fuel oil and shifting fuel types (from, e.g., coal to gas) in the EU. A reduced-form TM5-FASST (Fast Screening Scenario Tool based on the global chemical Transport Model 5) is applied to calculate regional and global levels of aerosol and ozone concentrations and to assess the impact of air quality improvements on human health and crop yield loss, showing substantial impacts of export of EU technologies and standards to other world regions. [ABSTRACT FROM AUTHOR]

Field deployments of the Aerodyne Aerosol Mass Spectrometer (AMS) have significantly advanced real-time measurements and source apportionment of non-refractory particulate matter. However, the cost and complex maintenance requirements of the AMS make impractical its deployment at suffcient sites to determine regional characteristics. Furthermore, the negligible transmission efficiency of the AMS inlet for supermicron particles significantly limits the characterization of their chemical nature and contributing sources. In this study, we utilize the AMS to characterize the water-soluble organic fingerprint of ambient particles collected onto conventional quartz filters, which are routinely sampled at many air quality sites. The method was applied to 256 particulate matter (PM) filter samples (PM1, PM2.5, PM10) collected at 16 urban and rural sites during summer and winter. We show that the results obtained by the present technique compare well with those from co-located online measurements, e.g. AMS or Aerosol Chemical Speciation Monitor (ACSM). The bulk recoveries of organic aerosol (60-91%) achieved using this technique, together with low detection limits (0.8 μg of organic aerosol on the analyzed filter fraction) allow its application to environmental samples. We will discuss the recovery variability of individual hydrocarbon, oxygen containing and other ions. The performance of such data in source apportionment is assessed in comparison to ACSM data. Recoveries of organic components related to different sources as traffic, wood burning and secondary organic aerosol are presented. This technique, while subjected to the limitations inherent to filter-based measurements (e.g. filter artifacts and limited time resolution) may be used to enhance the AMS capabilities in measuring size-fractionated, spatially-resolved long-term datasets. [ABSTRACT FROM AUTHOR]

The mandate of the Task Force Hemispheric Transport of Air Pollution (HTAP) under the Convention on Long-Range Transboundary Air Pollution (CLRTAP) is to improve the scientific understanding of the intercontinental air pollution transport, to quantify impacts on human health, vegetation and climate, to identify emission mitigation options across the regions of the Northern Hemisphere, and to guide future policies on these aspects. The harmonization and improvement of regional emission inventories is imperative to obtain consolidated estimates on the formation of global-scale air pollution. An emissions dataset has been constructed using regional emission gridmaps (annual and monthly) for SO2, NOx, CO, NMVOC, NH3, PM10, PM2.5, BC and OC for the years 2008 and 2010, with the purpose of providing consistent information to global and regional scale modelling efforts. This compilation of different regional gridded inventories, including the Environmental Protection Agency (EPA)'s for USA, EPA and Environment Canada's for Canada, the European Monitoring and Evaluation Programme (EMEP) and Netherlands Organisation for Applied Scientific Research (TNO)'s for Europe, and the Model Intercomparison Study in Asia (MICS-Asia)'s for China, India and other Asian countries, was gap-filled with the emission gridmaps of the Emissions Database for Global Atmospheric Research (EDGARv4.3) for the rest of the world (mainly South-America, Africa, Russia and Oceania). Emissions from seven main categories of human activities (power, industry, residential, agriculture, ground transport, aviation and shipping) were estimated and spatially distributed on a common grid of 0.1° x 0.1° longitude-latitude, to yield monthly, global, sector-specific gridmaps for each substance and year. The HTAP_v2.2 air pollutant gridmaps are considered to combine latest available regional information within a complete global dataset. The disaggregation by sectors, high spatial and temporal resolution and detailed information on the data sources and references used will provide the user the required transparency. Because HTAP_v2.2 [ABSTRACT FROM AUTHOR]

A detailed characterization of air quality in Paris (France), a megacity of more than 10 million inhabitants, during two one month intensive campaigns and from additional one year observations, revealed that about 70% of the fine particulate matter (PM) at urban background is transported on average into the megacity from upwind regions. This dominant influence of regional sources was confirmed by in-situ measurements during short intensive and longer term campaigns, aerosol optical depth (AOD) measurements from ENVISAT, and modeling results from PMCAMx and CHIMERE. While advection of sulfate is well documented for other megacities, there was surprisingly high contribution from long-range transport for both nitrate and organic aerosol. The origin of organic PM was investigated by a comprehensive analysis of aerosol mass spectrometer (AMS), radiocarbon and tracer measurements during two intensive campaigns. Primary fossil fuel combustion emissions contributed less than 20% in winter and 40% in summer to carbonaceous fine PM, unexpectedly little for a megacity. Cooking activities and, during winter, residential wood burning are the major primary organic PM sources. This analysis suggests that the major part of secondary organic aerosol is of modern origin, i.e. from biogenic precursors and from wood burning. Black carbon concentrations are on the lower end of values encountered in megacities worldwide, but still represent an issue for air quality. These comparatively low air pollution levels are due to a combination of low emissions per inhabitant, flat terrain, and a meteorology that is in general not conducive to local pollution build-up. This revised picture of a megacity only controlling part of its own average and peak PM levels has important implications for air pollution regulation policies. [ABSTRACT FROM AUTHOR]

Ambient particle number size distributions were measured in Paris, France during summer (1-31 July 2009) and winter (15 January-15 February 2010) at three fixed ground sites and using two mobile laboratories and one airplane. The campaigns were part of the MEGAPOLI project. New particle formation (NPF) was observed only during summer at approximately 50% of the campaign days, assisted by the low condensation sink (about 10.7 ± 5.9 × 10-3 s-1). NPF events inside the Paris plume were also observed at 600 m altitude onboard an aircraft simultaneously with regional events identified on the ground. Increased particle number concentrations were measured aloft also outside of the Paris plume at the same altitude, and were attributed to NPF. The Paris plume was identified, based on increased particle number and black carbon concentration, up to 200 km away from Paris center during summer. The number concentration of particles with diameter exceeding 2.5 nm measured on the surface at Paris center was on average 6.9 ± 8.7 × 104 and 12.1 ± 8.6 × 104 cm-3 during summer and winter, respectively, and was found to decrease exponentially with distance from Paris. However, further than 30 km from the city center, the particle number concentration at the surface was similar during both campaigns. During summer one suburban site in the NE was not significantly affected by Paris emissions due to higher background number concentrations, while the particle number concentration at the second suburban site in the SW increased by a factor of three when it was downwind of Paris. [ABSTRACT FROM AUTHOR]