A study of the phase transition behavior of mixed ammonium sulfate ? malonic acid aerosols

International audienceThis is a study into the phase transitions of aerosol composed of the ternary system ammonium sulfate (AS) ? malonic acid (MA) ? water using infrared extinction spectroscopy. Twelve compositions were studied in both deliquescence and efflorescence mode experiments. The presence of a MA fraction, by dry mass, (fMA) of 0.1 in an AS aerosol altered the relative humidity at which the phase transitions occur in an atmospherically significant manner. For compositions with 0.25fMAfMA=0.9, the crystallization relative humidity of MA was lowered from RH=6% to less than 1%. Similarly, at fMA=0.4, the AS component did not crystallize. The atmospheric implications of the results are discussed

A study of the phase transition behavior of internally mixed ammonium sulfate - malonic acid aerosols

International audienceThis is a study into the phase transitions of aerosol composed of the ternary system ammonium sulfate (AS) - malonic acid (MA) - water using infrared extinction spectroscopy. Twelve compositions were studied in both deliquescence and efflorescence mode experiments. The presence of a MA fraction, by dry mass, (fMA) of 0.1 in an AS aerosol altered the relative humidity at which the phase transitions occur in an atmospherically significant manner. For compositions with 0.25fMAfMA=0.9, the crystallization relative humidity of MA was lowered from RH=6% to less than 1%. Similarly, at fMA=0.4, the AS component did not crystallize. The atmospheric implications of the results are discussed

Phase transitions and hygroscopic growth of aerosol particles containing humic acid and mixtures of humic acid and ammonium sulphate

International audienceThe phase transitions and hygroscopic growth of two humic acid aerosols (Aldrich sodium salt and Leonardite Standard (IHSS)) and their mixtures with ammonium sulphate have been investigated using a combination of two techniques, Fourier transform infra-red (FTIR) spectroscopy and tandem differential mobility analysis (TDMA). A growth factor of 1.16 at 85% relative humdity (RH) was found for the Aldrich humic acid which can be regarded as an upper limit for growth factors of humic-like substances (HULIS) found in atmospheric aerosol and is significantly smaller than that of typical atmospheric inorganics. We find that the humic acid aerosols exhibit water uptake over all relative humidites with no apparent phase changes, suggesting that these aerosols readily form supersaturated droplets. In the mixed particles, the humic acid component decreases the deliquescence relative humidity (DRH) and increases the efflorescence relative humidity (ERH) of the ammonium sulphate component, and there is some degree of water uptake prior to ammonium sulphate deliquescence. In addition, at low RH, the FTIR spectra show that the ammonium is present in a different chemical environment in the mixed aerosols than in crystalline ammonium sulphate, perhaps existing as a complex with the humic materials. The growth factors of the mixed aerosols are intermediate between those of the single component aerosols and can be predicted assuming that the inorganic and organic fractions take up water independently

Estimation of nitrogen budgets for contrasting catchments at the landscape scale

A comprehensive assessment of nitrogen (N) flows at the landscape scale is fundamental to understand spatial interactions in the N cascade and to inform the development of locally optimised N management strategies. To explore these interactions, complete N budgets were estimated for two contrasting hydrological catchments (dominated by agricultural grassland vs. semi-natural peat-dominated moorland), forming part of an intensively studied landscape in southern Scotland. Local scale atmospheric dispersion modelling and detailed farm and field inventories provided high resolution estimations of input fluxes. Direct agricultural inputs (i.e. grazing excreta, N<sub>2</sub> fixation, organic and synthetic fertiliser) accounted for most of the catchment N inputs, representing 82% in the grassland and 62% in the moorland catchment, while atmospheric deposition made a significant contribution, particularly in the moorland catchment, contributing 38% of the N inputs. The estimated catchment N budgets highlighted areas of key uncertainty, particularly N<sub>2</sub> exchange and stream N export. The resulting N balances suggest that the study catchments have a limited capacity to store N within soils, vegetation and groundwater. The "catchment N retention", i.e. the amount of N which is either stored within the catchment or lost through atmospheric emissions, was estimated to be 13% of the net anthropogenic input in the moorland and 61% in the grassland catchment. These values contrast with regional scale estimates: Catchment retentions of net anthropogenic input estimated within Europe at the regional scale range from 50% to 90%, with an average of 82% (Billen et al., 2011). This study emphasises the need for detailed budget analyses to identify the N status of European landscapes

Evaluation of the performance of different atmospheric chemical transport models and inter-comparison of nitrogen and sulphur deposition estimates for the UK

An evaluation has been made of a number of contrasting atmospheric chemical transport models, of varying complexity, applied to estimate sulphur and nitrogen deposition in the UK. The models were evaluated by comparison with annually averaged measurements of gas, aerosol and precipitation concentrations from the national monitoring networks. The models were evaluated in relation to performance criteria. They were generally able to satisfy a criterion of ‘fitness for purpose’ that at least 50% of modelled concentrations should be within a factor of two of measured values. The second criterion, that the magnitude of the normalised mean bias should be less than 20%, was not always satisfied. Considering known uncertainties in measurement techniques, this criterion may be too strict. Overall, simpler models were able to give a good representation of measured gas concentrations whilst the use of dynamic meteorology, and complex photo-chemical reactions resulted in a generally better representation of measured aerosol and precipitation concentrations by more complex models. The models were compared graphically by plotting maps and cross-country transects of wet and dry deposition as well as calculating budgets of total wet and dry deposition to the UK for sulphur, oxidised nitrogen and reduced nitrogen. The total deposition to the UK varied by ±22–36% amongst the different models depending on the deposition component. At a local scale estimates of both dry and wet deposition for individual 5 km × 5 km model grid squares were found to vary between the different models by up to a factor of 4.This work was funded by the Department for the Environment, Food and Rural Affairs. Additional support was provided by the Joint Environmental Program, the Natural Environment Research Council and the Environment Agency.This is the final version of the article. It first appeared from Elsevier via http://dx.doi.org/10.1016/j.atmosenv.2015.08.00

Identification of potential “Remedies” for Air Pollution (nitrogen) Impacts on Designated Sites (RAPIDS)

Atmospheric nitrogen (N) deposition is a significant threat to semi-natural habitats and species in the UK, resulting in on-going erosion of habitat quality and declines in many species of high conservation value. The project focused on impacts and remedies for designated conservation sites, especially Natura 2000 sites protected under the EU Habitats Directive. However, the approach and certainly the measures could be equally applied to other areas of high conservation value. Evidence was drawn together to develop a framework for identifying key N threats at individual sites as a basis to target mitigation options in the context of potential legislative, voluntary and financial instruments