Polychlorinated biphenyls （PCBs） were measured in atmospheric samples collected from the North Pacific to the Arctic Ocean between July and September 2012 to study the atmospheric concentration characteris-tics of P...Polychlorinated biphenyls （PCBs） were measured in atmospheric samples collected from the North Pacific to the Arctic Ocean between July and September 2012 to study the atmospheric concentration characteris-tics of PCBs and their gas/particle partitioning. The mean concentration of 26 PCBs （vapor plus particulate phase） （∑PCBs） was 19.116 pg/m^3with a standard deviation of 13.833 pg/m^3. Three most abundant conge-ners were CB-28, -52 and -77, accounting for 43.0% to∑PCBs. The predominance of vapor PCBs （79.0% to∑PCBs） in the atmosphere was observed.∑PCBs were negative correlated with the latitudes and inverse of the absolute temperature （1/T）. The significant correlation for most congeners was also observed between the logarithm of gas/particle partition coefficient （logKp） and 1/T. Shallower slopes （from ∑0.15 to ∑0.46, average ∑0.27） were measured from the regression of the logarithm of sub-cooled liquid vapor pressures （logpoL） and logKP for all samples. The difference of the slopes and intercepts among samples was insignifi-cant （p〉0.1）, implying adsorption and/or absorption processes and the aerosol composition did not differ significantly among different samples. By comparing three models, the J-P adsorption model, the octanol/air partition coefficient （KOA） based model and the soot-air model, the gas/particle partitioning of PCBs in the Arctic atmosphere was simulated more precisely by the soot-air model, and the adsorption onto el-emental carbon is more sensitive than the absorption into organic matters of aerosols, especially for low-chlorinated PCB congeners.展开更多
Molecular speciation of atmospheric organic matter was investigated during a short summer field campaign performed in a citrus fruit field in northern Corsica（June 2011）. Aimedat assessing the performance on the fie...Molecular speciation of atmospheric organic matter was investigated during a short summer field campaign performed in a citrus fruit field in northern Corsica（June 2011）. Aimedat assessing the performance on the field of newly developed analytical protocols, this work focuses on the molecular composition of both gas and particulate phases and provides an insight into partitioning behavior of the semi-volatile oxygenated fraction. Limonene ozonolysis tracers were specifically searched for, according to gas chromatography–mass spectrometry（GC–MS） data previously recorded for smog chamber experiments. A screening of other oxygenated species present in the field atmosphere was also performed. About sixty polar molecules were positively or tentatively identified in gas and/or particle phases. These molecules comprise a wide range of branched and linear, mono and di-carbonyls（C_3–C7）,mono and di-carboxylic acids（C_3–C_18）, and compounds bearing up to three functionalities.Among these compounds, some can be specifically attributed to limonene oxidation and others can be related to α- or β-pinene oxidation. This provides an original snapshot of the organic matter composition at a Mediterranean site in summer. Furthermore, for compounds identified and quantified in both gaseous and particulate phases, an experimental gas/particle partitioning coefficient was determined. Several volatile products, which are not expected in the particulate phase assuming thermodynamic equilibrium, were nonetheless present in significant concentrations. Hypotheses are proposed to explain these observations, such as the possible aerosol viscosity that could hinder the theoretical equilibrium to be rapidly reached.展开更多
基金The Chinese Polar Environment Comprehensive Investigation and Assessment Programs under contract Nos 02-01,03-04,04-01 and 04-03the National Natural Science Fundation of China under contract No.21377032
文摘Polychlorinated biphenyls （PCBs） were measured in atmospheric samples collected from the North Pacific to the Arctic Ocean between July and September 2012 to study the atmospheric concentration characteris-tics of PCBs and their gas/particle partitioning. The mean concentration of 26 PCBs （vapor plus particulate phase） （∑PCBs） was 19.116 pg/m^3with a standard deviation of 13.833 pg/m^3. Three most abundant conge-ners were CB-28, -52 and -77, accounting for 43.0% to∑PCBs. The predominance of vapor PCBs （79.0% to∑PCBs） in the atmosphere was observed.∑PCBs were negative correlated with the latitudes and inverse of the absolute temperature （1/T）. The significant correlation for most congeners was also observed between the logarithm of gas/particle partition coefficient （logKp） and 1/T. Shallower slopes （from ∑0.15 to ∑0.46, average ∑0.27） were measured from the regression of the logarithm of sub-cooled liquid vapor pressures （logpoL） and logKP for all samples. The difference of the slopes and intercepts among samples was insignifi-cant （p〉0.1）, implying adsorption and/or absorption processes and the aerosol composition did not differ significantly among different samples. By comparing three models, the J-P adsorption model, the octanol/air partition coefficient （KOA） based model and the soot-air model, the gas/particle partitioning of PCBs in the Arctic atmosphere was simulated more precisely by the soot-air model, and the adsorption onto el-emental carbon is more sensitive than the absorption into organic matters of aerosols, especially for low-chlorinated PCB congeners.
文摘Molecular speciation of atmospheric organic matter was investigated during a short summer field campaign performed in a citrus fruit field in northern Corsica（June 2011）. Aimedat assessing the performance on the field of newly developed analytical protocols, this work focuses on the molecular composition of both gas and particulate phases and provides an insight into partitioning behavior of the semi-volatile oxygenated fraction. Limonene ozonolysis tracers were specifically searched for, according to gas chromatography–mass spectrometry（GC–MS） data previously recorded for smog chamber experiments. A screening of other oxygenated species present in the field atmosphere was also performed. About sixty polar molecules were positively or tentatively identified in gas and/or particle phases. These molecules comprise a wide range of branched and linear, mono and di-carbonyls（C_3–C7）,mono and di-carboxylic acids（C_3–C_18）, and compounds bearing up to three functionalities.Among these compounds, some can be specifically attributed to limonene oxidation and others can be related to α- or β-pinene oxidation. This provides an original snapshot of the organic matter composition at a Mediterranean site in summer. Furthermore, for compounds identified and quantified in both gaseous and particulate phases, an experimental gas/particle partitioning coefficient was determined. Several volatile products, which are not expected in the particulate phase assuming thermodynamic equilibrium, were nonetheless present in significant concentrations. Hypotheses are proposed to explain these observations, such as the possible aerosol viscosity that could hinder the theoretical equilibrium to be rapidly reached.
