31 research outputs found
On the abundance and source contributions of dicarboxylic acids in size-resolved aerosol particles at continental sites in central Europe
Dicarboxylic acids (DCAs) are among the most abundant organic compounds observed in atmospheric aerosol particles and have been extensively studied at many places around the world. The importance of the various primary sources and secondary formation pathways discussed in the literature is often difficult to assess from field studies, though. In the present study, a large data set of size-resolved DCA concentrations from several inland sites in Germany is combined with results from a recently developed approach of statistical back-trajectory analysis and additional data. Principal component analysis is then used to reveal the most important factors governing the abundance of DCAs in different particle size ranges. The two most important sources revealed are (i) photochemical formation during intense radiation days in polluted air masses, likely occurring in the gas phase on short timescales (gasSOA), and (ii) secondary reactions in anthropogenically influenced air masses, likely occurring in the aqueous phase on longer timescales (aqSOA). While the first source strongly impacts DCA concentrations mainly in small and large particles, the second one enhances accumulation mode DCAs and is responsible for the bulk of the observed concentrations. Primary sources were found to be minor (sea salt, soil resuspension) or non-existent (biomass burning, traffic). The results can be regarded as representative for typical central European continental conditions
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Size-segregated chemical, gravimetric and number distribution-derived mass closure of the aerosol in Sagres, Portugal during ACE-2
During the ACE-2 field campaign in the summer of 1997 an intensive, ground-based physical
and chemical characterisation of the clean marine and continentally polluted aerosol was performed
at Sagres, Portugal. Number size distributions of the dry aerosol in the size range
3–10 000 nm were continuously measured using DMPS and APS systems. Impactor samples
were regularly taken at 60% relative humidity (RH) to obtain mass size distributions by
weighing the impactor foils, and to derive a chemical mass balance by ion and carbon analysis.
Hygroscopic growth factors of the metastable aerosol at 60% RH were determined to estimate
the number size distribution at a relative humidity of 60%. A size segregated 3-way mass closure
study was performed in this investigation for the first time. Mass size distributions at 60% RH
derived from number size distribution measurements and impactors samples (weighing and
chemical analysis) are compared. A good agreement was found for the comparison of total
gravimetrically-determined mass with both number distribution-derived (slope=1.23/1.09;
R2>0.97; depending on the parameters humidity growth and density) and chemical mass
concentration (slope=1.02; R2=0.79) for particles smaller than 3 mm in diameter. Except for
the smallest impactor size range relatively good correlations (slope=0.86–1.42) with small
deviations (R2=0.76–0.98) for the different size fractions were found. Since uncertainties in
each of the 3 methods are about 20% the observed differences in the size-segregated mass
fractions can be explained by the measurement uncertainties. However, the number distributionderived
mass is mostly higher than the chemically and gravimetrically determined mass, which
can be explained by sampling losses of the impactor, but as well with measurement uncertainties
as, e.g., the sizing of the DMPS/APS
Hygroscopic properties of different aerosol types over the Atlantic and Indian Oceans
Hygroscopic properties of atmospheric particles were studied in the marine tropospheric boundary layer over the Atlantic and Indian Oceans during two consecutive field studies: the Aerosols99 cruise (Atlantic Ocean) from 15 January to 20 February 1999, and the INDOEX cruise (Indian Ocean Experiment) from 23 February to 30 March 1999. The hygroscopic properties were compared to optical and chemical properties, such as absorption, chemical inorganic composition, and mass concentration of organic and elemental carbon, to identify the influence of these parameters on hygroscopicity.
During the two field studies, four types of aerosol-sampling instruments were used on board the NOAA (National Oceanic and Atmospheric Administration) Research Vessel Ronald H. Brown: Hygroscopicity Tandem Differential Mobility Analyzer (HTDMA), seven-stage cascade impactor, two-stage cascade impactor, and Particle Soot Absorption Photometer (PSAP). The HTDMA was used to determine the hygroscopic properties of atmospheric particles at initial dry sizes (Dp) of 50, 150, and 250 nm and at relative humidities (RH) of 30, 55, 75, and 90%. Simultaneously, a seven-stage cascade impactor of which 3 stages were in the sub-mm size range was used to determine the molar composition of the major inorganic ions such as ammonium and sulfate ions. A two-stage cascade impactor (1 in the sub-mm size range, 1 in the sup-mm size range) was used to determine the mass concentration of organic and elemental carbon. The PSAP was used (at a wavelength of 565 nm) to measure the light absorption coefficient of the aerosol.
During the two field studies, air masses of several different origins passed the ship's cruise path. The occurrence of different air masses was classified into special time periods signifying the origin of the observed aerosol.
All time periods showed a group of particles with high hygroscopic growth. The measured average hygroscopic growth factors defined by the ratio of dry and wet particle diameter at 90% RH ranged from 1.6 to 2.0, depending on the dry particle size and on the type of air mass. Particles with low hygroscopic growth occurred only when continentally influenced air masses arrived at the ship's position. Distinctions in hygroscopic growth of particles of different air masses were more significant for small relative humidities (30% or 55% RH). High concentrations of elemental carbon corresponded with high light absorption coefficients and with the occurrence of less-hygroscopic and nearly hydrophobic particle fractions in the hygroscopic growth distributions.
A key finding is that clean marine air masses that had no land contact for five to six days could clearly be distinguished from polluted air masses that had passed over a continent several days before reaching the ship
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A comparison of aerosol chemical and optical properties from the 1st and 2nd Aerosol Characterization Experiments
Shipboard measurements of aerosol chemical composition and optical properties were made during both ACE-1 and ACE-2. ACE-1 focused on remote marine aerosol minimally perturbed by continental sources. ACE-2 studied the outflow of European aerosol into the NE Atlantic atmosphere. A variety of air masses were sampled during ACE-2 including Atlantic, polar, Iberian Peninsula, Mediterranean, and Western European. Reported here are mass size distributions of non-sea salt (nss) sulfate, sea salt, and methanesulfonate and submicron and supermicron concentrations of black and organic carbon. Optical parameters include submicron and supermicron aerosol scattering and backscattering coefficients at 550 nm, the absorption coefficient at 550±20 nm, the Ångström exponent for the 550 and 700 nm wavelength pair, and single scattering albedo at 550 nm. All data are reported at the measurement relative humidity of 55%. Measured concentrations of nss sulfate aerosol indicate that, relative to ACE-1, ACE-2 aerosol during both marine and continental flow was impacted by continental sources. Thus, while sea salt controlled the aerosol chemical composition and optical properties of both the submicron and supermicron aerosol during ACE-1, it played a relatively smaller role in ACE-2. This is confirmed by the larger average Ångström exponent for ACE-2 continental aerosol of 1.2±0.26 compared to the ACE-1 average of -0.03±0.38. The depletion of chloride from sea salt aerosol in ACE-2 continental air masses averaged 55±25% over all particle sizes. This compares to the ACE-2 marine average of 4.8±18% and indicates the enhanced interaction of anthropogenic acids with sea salt as continental air masses are transported into the marine atmosphere. Single scattering albedos averaged 0.95±0.03 for ACE-2 continental air masses. Averages for ACE-2 and ACE-1 marine air masses were 0.98±0.01 and 0.99±0.01, respectively
The Molecular Identification of Organic Compounds in the Atmosphere: State of the Art and Challenges
Two-dimensional capillary zone electrophoresis–mass spectrometry for the characterization of intact monoclonal antibody charge variants, including deamidation products.
Capillary zone electrophoresis (CZE) is a powerful tool that is progressively being applied for the separation of monoclonal antibody (mAb) charge variants. Mass spectrometry (MS) is the desired detection method concerning identification of mAb variants. In biopharmaceutical applications, there exist optimized and validated electrolyte systems for mAb variant quantification. However, these electrolytes interfere greatly with the electrospray ionization (ESI) process. Here, a heart-cut CZE–CZE–MS setup with an implemented mechanical four-port valve interface was developed that used a generic ε-aminocaproic acid based background electrolyte in the first dimension and acetic acid in the second dimension. Interference-free, highly precise mass data (deviation less than 1 Da) of charge variants of trastuzumab, acting as model mAb system, were achieved. The mass accuracy obtained (low parts per million range) is discussed regarding both measured and calculated masses. Deamidation was detected for the intact model antibody, and related mass differences were significantly confirmed on the deglycosylated level. The CZE–CZE–MS setup is expected to be applicable to a variety of antibodies and electrolyte systems. Thus, it has the potential to become a compelling tool for MS characterization of antibody variants separated in ESI-interfering electrolytes
Determination of volatile and non-volatile aerosol fractions and degree of mixing of anthropogenically influenced marine aerosols
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