Multi-model study of mercury dispersion in the atmosphere: vertical and interhemispheric distribution of mercury species

Atmospheric chemistry and transport of mercury play a key role in the global mercury cycle. However, there are still considerable knowledge gaps concerning the fate of mercury in the atmosphere. This is the second part of a model intercomparison study investigating the impact of atmospheric chemistry and emissions on mercury in the atmosphere. While the first study focused on ground-based observations of mercury concentration and deposition, here we investigate the vertical and interhemispheric distribution and speciation of mercury from the planetary boundary layer to the lower stratosphere. So far, there have been few model studies investigating the vertical distribution of mercury, mostly focusing on single aircraft campaigns. Here, we present a first comprehensive analysis based on various aircraft observations in Europe, North America, and on intercontinental flights. The investigated models proved to be able to reproduce the distribution of total and elemental mercury concentrations in the troposphere including interhemispheric trends. One key aspect of the study is the investigation of mercury oxidation in the troposphere. We found that different chemistry schemes were better at reproducing observed oxidized mercury patterns depending on altitude. High concentrations of oxidized mercury in the upper troposphere could be reproduced with oxidation by bromine while elevated concentrations in the lower troposphere were better reproduced by OH and ozone chemistry. However, the results were not always conclusive as the physical and chemical parameterizations in the chemistry transport models also proved to have a substantial impact on model results

The impact of the chemical production of methyl nitrate from the NO + CH3O2 reaction on the global distributions of alkyl nitrates, nitrogen oxides and tropospheric ozone: a global modelling study

The impact of the chemical production of methyl nitrate from the NO + CH3O2 reaction on the global distributions of alkyl nitrates, nitrogen oxides and tropospheric ozone: a global modelling study

NO and NOy in the upper troposphere: Nine years of CARIBIC measurements onboard a passenger aircraft

Nitrogen oxide (NO and NOy) measurements were performed onboard an in-service aircraft within the framework of CARIBIC (Civil Aircraft for the Regular Investigation of the atmosphere Based on an Instrument Container). A total of 330 flights were completed from May 2005 through April 2013 between Frankfurt/Germany and destination airports in Canada, the USA, Brazil, Venezuela, Chile, Argentina, Colombia, South Africa, China, South Korea, Japan, India, Thailand, and the Philippines. Different regions show differing NO and NOy mixing ratios. In the mid-latitudes, observed NOy and NO generally shows clear seasonal cycles in the upper troposphere with a maximum in summer and a minimum in winter. Mean NOy mixing ratios vary between 1.36 nmol/mol in summer and 0.27 nmol/mol in winter. Mean NO mixing ratios range between 0.05 nmol/mol and 0.22 nmol/mol. Regions south of 40°N show no consistent seasonal dependence. Based on CO observations, low, median and high CO air masses were defined. According to this classification, more data was obtained in high CO air masses in the regions south of 40°N compared to the midlatitudes. This indicates that boundary layer emissions are more important in these regions. In general, NOy mixing ratios are highest when measured in high CO air masses. This dataset is one of the most comprehensive NO and NOy dataset available today for the upper troposphere and is therefore highly suitable for the validation of atmosphere-chemistry-models

Preparation and antifouling properties of PVDF ultrafiltration membranes with polyaniline (PANI) nanofibers and hydrolysed PSMA (H-PSMA) as additives

Polyaniline (PANI) nanofibers were used as hydrophilic additives to study their effect on the performance of polyvinylidene fluoride (PVDF) ultrafiltration (UF) membranes. PVDF UP membranes were prepared by the phase inversion method with hydrolyzed polystyrene-co-maleic anhydride (H-PSMA) and PANI nanofibers as additives. PANI nanofibers were synthesized by rapid mixing reaction and were used as a hydrophilic modifying agent with varying concentrations (0-1.5 wt.%) in the membranes. The synthesized PANI nanofibers were characterized by Fourier transform infrared spectroscopy (FTIR), X-ray diffraction (XRD), scanning electron microscope (SEM) and transmission electron microscope (TEM) analysis. Hydrolyzed PSMA was prepared by the hydrolysis of PSMA and was used as a novel pore forming additive. The addition of PANI nanofibers into the membranes increased the membrane hydrophilicity, porosity, water uptake and permeability. The membranes also showed good antifouling nature during BSA (bovine serum albumin) filtration when compared to the pristine membrane without PANI nanofibers. Membrane with 1.0 wt.% PANI content showed highest permeability among the synthesized membranes. The membrane having highest permeability was subjected to heavy metal ion rejection which showed high rejection of 98.52% and 9738% for heavy metal ions Pb2+ and Cd2+ respectively

Origin of aerosol particles in the mid-latitude and subtropical upper troposphere and lowermost stratosphere from cluster analysis of CARIBIC data

The origin of aerosol particles in the upper troposphere and lowermost stratosphere over the Eurasian continent was investigated by applying cluster analysis methods to in situ measured data. Number concentrations of submicrometer aerosol particles and trace gas mixing ratios derived by the CARIBIC (Civil Aircraft for Regular Investigation of the Atmosphere Based on an Instrument Container) measurement system on flights between Germany and South-East Asia were used for this analysis. Four cluster analysis methods were applied to a test data set and their capability of separating the data points into scientifically reasonable clusters was assessed. The best method was applied to seasonal data subsets for summer and winter resulting in five cluster or air mass types: stratosphere, tropopause, free troposphere, high clouds, and boundary layer influenced. Other source clusters, like aircraft emissions could not be resolved in the present data set with the used methods. While the cluster separation works satisfactory well for the summer data, in winter interpretation is more difficult, which is attributed to either different vertical transport pathways or different chemical lifetimes in both seasons. The geographical distribution of the clusters together with histograms for nucleation and Aitken mode particles within each cluster are presented. Aitken mode particle number concentrations show a clear vertical gradient with the lowest values in the lowermost stratosphere (750�2820 particles/cm3 STP, minimum of the two 25% � and maximum of the two 75%-percentiles of both seasons) and the highest values for the boundary-layer-influenced air (4290�22 760 particles/cm3 STP). Nucleation mode particles are also highest in the boundary-layer-influenced air (1260� 29 500 particles/cm3 STP), but are lowest in the free troposphere (0�450 particles/cm3 STP). The given submicrometer particle number concentrations represent the first large-scale seasonal data sets for the upper troposphere and lowermost stratosphere over the Eurasian continen