83 research outputs found

    Aerosol chemical composition at Cabouw, The Netherlands as observed in two intensive periods in May 2008 and March 2009

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    Observations of aerosol chemical composition in Cabauw, the Netherlands, are presented for two intensive measurement periods in May 2008 and March 2009. Sub-micron aerosol chemical composition was measured by an Aerodyne Aerosol Mass Spectrometer (AMS) and is compared to observations from aerosol size distribution measurements as well as composition measurements with a Monitor for AeRosol and GAses (MARGA) based instrument and a Thermal-Desorption Proton-Transfer-Reaction Mass-Spectrometer (TD-PTR-MS). An overview of the data is presented and the data quality is discussed. In May 2008 enhanced pollution was observed with organics contributing 40% to the PM1 mass. In contrast the observed average mass loading was lower in March 2009 and a dominance of ammonium nitrate (42%) was observed. The semi-volatile nature of ammonium nitrate is evident in the diurnal cycles with maximum concentrations observed in the morning hours in May 2008 and little diurnal variation observed in March 2009. Size dependent composition data from AMS measurements are presented and show a dominance of organics in the size range below 200 nm. A higher O:C ratio of the organics is observed for May 2008 than for March 2009. Together with the time series of individual tracer ions this shows the dominance of OOA over HOA in May 2008

    Effectiveness of ammonia reduction on control of fine particle nitrate

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    In some regions, reducing aerosol ammonium nitrate (NH4NO3) concentrations may substantially improve air quality. This can be accomplished by reductions in precursor emissions, such as nitrogen oxides (NOx) to lower nitric acid (HNO3) that partitions to the aerosol, or reductions in ammonia (NH3) to lower particle pH and keep HNO3 in the gas phase. Using the ISORROPIA-II thermodynamic aerosol model and detailed observational data sets, we explore the sensitivity of aerosol NH4NO3 to gas-phase NH3 and NOx controls for a number of contrasting locations, including Europe, the United States, and China. NOx control is always effective, whereas the aerosol response to NH3 control is highly nonlinear and only becomes effective at a thermodynamic sweet spot. The analysis provides a conceptual framework and fundamental evaluation on the relative value of NOx versus NH3 control and demonstrates the relevance of pH as an air quality parameter. We find that, regardless of the locations examined, it is only when ambient particle pH drops below an approximate critical value of 3 (slightly higher in warm and slightly lower in cold seasons) that NH3 reduction leads to an effective response in PM2.5 mass. The required amount of NH3 reduction to reach the critical pH and efficiently decrease NH4NO3 at different sites is assessed. Owing to the linkage between NH3 emissions and agricultural productivity, the substantial NH3 reduction required in some locations may not be feasible. Finally, controlling NH3 emissions to increase aerosol acidity and evaporate NH4NO3 will have other effects, beyond reduction of PM2.5 NH4NO3, such as increasing aerosol toxicity and potentially altering the deposition patterns of nitrogen and trace nutrients.</p

    Illustrating the benefit of using hourly monitoring data on secondary inorganic aerosol and its precursors for model evaluation

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    Secondary inorganic aerosol, most notably ammonium nitrate and ammonium sulphate, is an important contributor to ambient particulate mass and provides a means for long range transport of acidifying components. The modelling of the formation and fate of these components is challenging. Especially, the formation of the semi-volatile ammonium nitrate is strongly dependent on ambient conditions and the precursor concentrations. For the first time an hourly artefact free data set from the MARGA instrument is available for the period of a full year (1 August 2007 to 1 August 2008) at Cabauw, the Netherlands. This data set is used to verify the results of the LOTOS-EUROS model. The comparison showed that the model underestimates the SIA levels. Closer inspection revealed that base line values appear well estimated for ammonium and sulphate and that the underestimation predominantly takes place at the peak concentrations. For nitrate the variability towards high concentrations is much better captured, however, a systematic relative underestimation was found. The model is able to reproduce many features of the intra-day variability observed for SIA. Although the model captures the seasonal and average diurnal variation of the SIA components, the modelled variability for the nitrate precursor gas nitric acid is much too large. It was found that the thermodynamic equilibrium module produces a too stable ammonium nitrate in winter and during night time in summer, whereas during the daytime in summer it is too unstable. We recommend to improve the model by verification of the equilibrium module, inclusion of coarse mode nitrate and to address the processes concerning SIA formation combined with a detailed analysis of the data set at hand. The benefit of the hourly data with both particulate and gas phase concentrations is illustrated and a continuation of these measurements may prove to be very useful in future model evaluation and improvement studies. Based on our findings we propose to implement a monitoring strategy using three levels of detail within the Netherlands

    Impact of Ammonium Nitrate chemistry on the AOT in Cabauw, the Netherlands

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    A 1D column model representing detailed microphysics and chemistry associated with sulfate, ammonia and nitric acid is applied to study local processes which influence aerosol optical thickness (AOT). We focus on Cabauw, the Netherlands, on May 8th 2008 during the Intensive Measurement campaign At Cabauw Tower (IMPACT). The 8th of May was characterized by a strong diurnal cycle of RH and aerosol concentration in the boundary layer. Furthermore, the lower troposphere was characterized by high concentrations of aerosol ammonium and nitrate as well as ammonia and nitric acid. Production of ammonium nitrate in the aerosol contributes to the particle hygroscopicity. This leads to additional condensational growth, which, in turn, enables further uptake of ammonium nitrate. It is found to predominantly affect particles smaller than 0.1 μm, so that the simulated wet aerosol size distribution is considerably narrower compared to a situation without ammonium nitrate. Our results show that the daily evolution of aerosol ammonium nitrate influences the variability of AOT more than the daily variability of RH and aerosol concentration. On this particular day, aerosol ammonium nitrate effectively enhances AOT by a factor of 2–4, depending on the time of the day. A relatively large discrepancy between modeled and observed AOT in the afternoon of May 8th is probably associated with secondary organic aerosol production in the afternoon which is not considered in our study
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