On the effects of hydrocarbon and sulphur-containing compounds on the CCN activation of combustion particles

International audienceThe European PartEmis project (''Measurement and prediction of emissions of aerosols and gaseous precursors from gas turbine engines'') was focussed on the characterisation and quantification of exhaust emissions from a gas turbine engine. A comprehensive suite of aerosol, gas and chemi-ion measurements were conducted under different combustor operating conditions and fuel sulphur concentrations. Combustion aerosol characterisation included on-line measurements of mass and number concentration, size distribution, mixing state, thermal stability of internally mixed particles, hygroscopicity, cloud condensation nuclei (CCN) activation potential, and off-line analysis of chemical composition. Modelling of CCN activation of combustion particles was conducted using microphysical and chemical properties obtained from the measurements as input data. Based on this unique data set, the role of sulphuric acid coatings on the combustion particles, formed in the cooling exhaust plume through either direct condensation of gaseous sulphuric acid or coagulation with volatile condensation particles nucleating from gaseous sulphuric acid, and the role of the organic fraction for the CCN activation of combustion particles was investigated. It was found that particles containing a large fraction of non-volatile organic compounds grow significantly less at high relative humidity than particles with a lower content of non-volatile OC. Also the effect of the non-volatile OC fraction on the potential CCN activation is significant. While a coating of water-soluble sulphuric acid increases the potential CCN activation, or lowers the activation diameter, respectively, the non-volatile organic compounds, mainly found at lower combustion temperatures, can partially compensate this sulphuric acid-related enhancement of CCN activation of carbonaceous combustion aerosol particles

On the effects of organic matter and sulphur-containing compounds on the CCN activation of combustion particles

The European PartEmis project (Measurement and prediction of emissions of aerosols and gaseous precursors from gas turbine engines) was focussed on the characterisation and quantification of exhaust emissions from a gas turbine engine. The combustion aerosol characterisation included on-line measurements of mass and number concentration, size distribution, mixing state, thermal stability of internally mixed particles, hygroscopicity, cloud condensation nuclei (CCN) activation potential, and off-line analysis of chemical composition. Based on this extensive data set, the role of sulphuric acid coating and of the organic fraction of the combustion particles for the CCN activation was investigated. Modelling of CCN activation was conducted using microphysical and chemical properties obtained from the measurements as input data. Coating the combustion particles with water-soluble sulphuric acid, increases the potential CCN activation, or lowers the activation diameter, respectively. The adaptation of a Köhler model to the experimental data yielded coatings from 0.1 to 3 vol-% of water-soluble matter, which corresponds to an increase in the fraction of CCN-activated combustion particles from ≤10^−4 to ≌10^−2 at a water vapour saturation ratio S_w=1.006. Additional particle coating by coagulation of combustion particles and aqueous sulphuric acid particles formed by nucleation further reduces the CCN activation diameter. In contrast, particles containing a large fraction of non-volatile organic compounds grow significantly less at high relative humidity than particles with a lower content of non-volatile OC. The resulting reduction in the potential CCN activation with an increasing fraction of non-volatile OC becomes visible as a trend in the experimental data. While a coating of water-soluble sulphuric acid increases the potential CCN activation, or lowers the activation diameter, respectively, the non-volatile organic compounds, mainly found at lower combustion temperatures, can partially compensate this sulphuric acid-related enhancement of CCN activation of carbonaceous combustion aerosol particles

A novel single-cavity three-wavelength photoacoustic spectrometer for atmospheric aerosol research

The spectral light-absorbing behavior of carbonaceous aerosols varies depending on the chemical composition and structure of the particles. A new single-cavity three-wavelength photoacoustic spectrometer was developed and characterized for measuring absorption coefficients at three wavelengths across the visible spectral range. In laboratory studies, several types of soot with different organic content were generated by a diffusion flame burner and were investigated for changes in mass-specific absorption cross section (MAC) values, absorption and scattering Angstrom exponents (alpha(abs) and alpha(sca)), and single scattering albedo (omega). By increasing the organic carbonaceous (OC) content of the aerosol from 50 to 90% of the total carbonaceous mass, for 660 nm nearly no change of MAC was found with increasing OC content. In contrast, for 532 nm a significant increase, and for 445 nm a strong increase of MAC was found with increasing OC content of the aerosol. Depending on the OC content, the Angstrom exponents of absorption and scattering as well as the single scattering albedo increased. These laboratory results were compared to a field study at a traffic-dominated urban site, which was also influenced by residential wood combustion. For this site a daily average value of alpha(abs)(445-660) of 1.9 was found

A novel single-cavity three-wavelength photoacoustic spectrometer for atmospheric aerosol research

The spectral light-absorbing behavior of carbonaceous aerosols varies depending on the chemical composition and structure of the particles. A new single-cavity three-wavelength photoacoustic spectrometer was developed and characterized for measuring absorption coefficients at three wavelengths across the visible spectral range. In laboratory studies, several types of soot with different organic content were generated by a diffusion flame burner and were investigated for changes in mass-specific absorption cross section (MAC) values, absorption and scattering Ångström exponents (αabs and αsca), and single scattering albedo (ω). By increasing the organic carbonaceous (OC) content of the aerosol from 50 to 90 % of the total carbonaceous mass, for 660 nm nearly no change of MAC was found with increasing OC content. In contrast, for 532 nm a significant increase, and for 445 nm a strong increase of MAC was found with increasing OC content of the aerosol. Depending on the OC content, the Ångström exponents of absorption and scattering as well as the single scattering albedo increased. These laboratory results were compared to a field study at a traffic-dominated urban site, which was also influenced by residential wood combustion. For this site a daily average value of αabs(445–660) of 1.9 was found

Atmospheric tar balls: Particles from biomass and biofuel burning

"Tar balls'' are amorphous, carbonaceous spherules that occur in the tropospheric aerosol as a result of biomass and biofuel burning. They form a distinct group of particles with diameters typically between 30 and 500 nm and readily identifiable with electron microscopy. Their lack of a turbostratic microstructure distinguishes them from soot, and their morphology and composition (similar to90 mol % carbon) renders them distinct from other carbonaceous particles. Tar balls are particularly abundant in slightly aged (minutes to hours old) biomass smoke, indicating that they likely form by gas-to-particle conversion within smoke plumes. The material of tar balls is initially hygroscopic; however, the particles become largely insoluble as a result of free radical polymerization of their organic molecules. Consequently, tar balls are primarily externally mixed with other particle types, and they do not appreciably increase in size during aging. When tar balls coagulate with water-bearing particles, their material may partly dissolve and no longer be recognizable as distinct particles. Tar balls may contain organic compounds that absorb sunlight. They are an important, previously unrecognized type of carbonaceous (organic) atmospheric particle

Результати ексгумації останків загиблих солдатів у центрі селища Цумань у 2010 р.

В статті висвітлюються результати археологічних досліджень Цуманської рятівної експедицією ДП « Волинські Старожитності» ДП НДЦ ОАСУ ІА НАН України, проведених у червні 2010 р. на місцезнаходженні останків солдатів Червоної армії часів Другої світової війни у центрі селища Цумань Ківерцівського району Волинської області

ECOC comparison exercise with identical thermal protocols after temperature offset correction - Instrument diagnostics by in-depth evaluation of operational parameters

© Author(s) 2015. A comparison exercise on thermal-optical elemental carbon/organic carbon (ECOC) analysers was carried out among 17 European laboratories. Contrary to previous comparison exercises, the 17 participants made use of an identical instrument set-up, after correcting for temperature offsets with the application of a recently developed temperature calibration kit (Sunset Laboratory Inc, OR, US). Temperature offsets reported by participants ranged from -93 to +100 °C per temperature step. Five filter samples and two sucrose solutions were analysed with both the EUSAAR2 and NIOSH870 thermal protocols. z scores were calculated for total carbon (TC); nine outliers and three stragglers were identified. Three outliers and eight stragglers were found for EC. Overall, the participants provided results between the warning levels with the exception of two laboratories that showed poor performance, the causes of which were identified and corrected through the course of the comparison exercise. The TC repeatability and reproducibility (expressed as relative standard deviations) were 11 and 15% for EUSAAR2 and 9.2 and 12% for NIOSH870; the standard deviations for EC were 15 and 20% for EUSAAR2 and 20 and 26% for NIOSH870. TC was in good agreement between the two protocols, TCNIOSH870 =0.98 × TCEUSAAR2 (R2 = 1.00, robust means). Transmittance (TOT) calculated EC for NIOSH870 was found to be 20% lower than for EUSAAR2, ECNIOSH870 = 0.80 × ECEUSAAR2 (R2 = 0.96, robust means). The thermograms and laser signal values were compared and similar peak patterns were observed per sample and protocol for most participants. Notable deviations from the typical patterns indicated either the absence or inaccurate application of the temperature calibration procedure and/or pre-oxidation during the inert phase of the analysis. Low or zero pyrolytic organic carbon (POC), as reported by a few participants, is suggested as an indicator of an instrument-specific pre-oxidation. A sample-specific pre-oxidation effect was observed for filter G, for all participants and both thermal protocols, indicating the presence of oxygen donors on the suspended particulate matter. POC (TOT) levels were lower for NIOSH870 than for EUSAAR2, which is related to the heating profile differences of the two thermal protocols

Intercomparison of shortwave radiative transfer schemes in global aerosol modeling: results from the AeroCom Radiative Transfer Experiment

In this study we examine the performance of 31 global model radiative transfer schemes in cloud-free conditions with prescribed gaseous absorbers and no aerosols (Rayleigh atmosphere), with prescribed scattering-only aerosols, and with more absorbing aerosols. Results are compared to benchmark results from high-resolution, multi-angular line-by-line radiation models. For purely scattering aerosols, model bias relative to the line-by-line models in the top-of-the atmosphere aerosol radiative forcing ranges from roughly −10 to 20%, with over- and underestimates of radiative cooling at lower and higher solar zenith angle, respectively. Inter-model diversity (relative standard deviation) increases from ~10 to 15% as solar zenith angle decreases. Inter-model diversity in atmospheric and surface forcing decreases with increased aerosol absorption, indicating that the treatment of multiple-scattering is more variable than aerosol absorption in the models considered. Aerosol radiative forcing results from multi-stream models are generally in better agreement with the line-by-line results than the simpler two-stream schemes. Considering radiative fluxes, model performance is generally the same or slightly better than results from previous radiation scheme intercomparisons. However, the inter-model diversity in aerosol radiative forcing remains large, primarily as a result of the treatment of multiple-scattering. Results indicate that global models that estimate aerosol radiative forcing with two-stream radiation schemes may be subject to persistent biases introduced by these schemes, particularly for regional aerosol forcing

Properties of jet engine combustion particles during the partemis experiment: Microphysics and chemistry, Geophys

[1] The particles emitted from an aircraft engine combustor were investigated in the European project PartEmis. Measured aerosol properties were mass and number concentration, size distribution, mixing state, thermal stability of internally mixed particles, hygroscopicity, and cloud condensation nuclei (CCN) activation potential. The combustor operation conditions corresponded to modern and older engine gas path temperatures at cruise altitude, with fuel sulphur contents (FSC) of 50, 410, and 1270 mg g À1 . Operation conditions and FSC showed only a weak influence on the microphysical aerosol properties, except for hygroscopic and CCN properties. Particles of size D ! 30 nm were almost entirely internally mixed. Particles of sizes D < 20 nm showed a considerable volume fraction of compounds that volatilise at 390 K (10 -15%) and 573 K (4 -10%), while respective fractions decreased to <5% for particles of size D ! 50 nm