The role of phoretic forces in the identification of particles acting as ice nuclei in mixed phase cloud is discussed. A method used to identify the effective ice nucleating particles is to sample ice crystals, which ...The role of phoretic forces in the identification of particles acting as ice nuclei in mixed phase cloud is discussed. A method used to identify the effective ice nucleating particles is to sample ice crystals, which are afterwards sublimated, and to examine the particles remaining after evaporation. The procedure takes into account only crystal with a maximum diameter of 20 μm, by assuming that small crystals do not scavenge aerosol during growth, and therefore that crystals contain only the effective nucleating particles. This assumption is questionable, however, as experiments have shown that even small ice crystals can scavenge aerosol. Another approach has been to compare the number and elemental composition of residual particles in small ice crystals and of aerosol near the cloud. By considering as example soot and black carbon aerosol, contradictory conclusions on their importance in the processes of ice nucleation have been reported in the literature. We suggest that, in addition to physico-chemical properties of soot/carbon aerosol particles, even the microphysical and environmental parameters involved in the transition of aerosol from gas phase to ice crystals in cloud should be considered. The contribution of phoretic forces should also be considered. After initial growth ice crystals can continue to grow by water vapour diffusion. Laboratory experiments confirm the contribution of diffusiophoresis with Stefan flow in the scavenging by snow crystals up to 3 mm in diameter. The particle scavenging efficiency of snow crystals is related to crystalline shape and depends on air relative humidity and temperature.展开更多
Nanoparticles in air are of particular concern for public health and employee exposure in work-places. Therefore, it is very important to prepare effective filters for their removal. In this work filters were prepared...Nanoparticles in air are of particular concern for public health and employee exposure in work-places. Therefore, it is very important to prepare effective filters for their removal. In this work filters were prepared from nanocellulose, i.e. cellulose nanofibrils (CNF). CNF was produced using two methods giving two different qualities of CNF. One quality had negative charges on the fibril surfaces while the other was neutral, and had in addition thinner fibrils compared to the other qualities. Filter samples were produced from water dispersions of CNF, by removal of the water by freeze drying. The performance of the CNF based filters was assessed and compared with filters based on synthetic polymer fibres. The ability to collect NaCl particles with a broad size distribution, ranging from nanometer to micrometer scale, was determined. CNF filters showed quality values comparable with the synthetic polymer based filters. Filters based on both the two CNF qualities had very good filtration efficiency for a given pressure drop across the filter.展开更多
The paper addresses some of the problems surrounding the relation between ice core chemical signals and atmospheric chemical composition in polar areas. The topic is important as the reconstruction of past climate and...The paper addresses some of the problems surrounding the relation between ice core chemical signals and atmospheric chemical composition in polar areas. The topic is important as the reconstruction of past climate and past atmospheric chemical composition is based on the assumption that chemical concentrations in the air, snow, firn and ice core are correlated. Ice core interpretation of aerosol is more straightforward than that of reactive gases. The transfer functions of gaseous species strongly interacting with ice are complex and additional field and laboratory experiments are required. Ice core chemical signals depend on the chemical composition of precipitations, which are related to the physics of precipitation formation, the chemical composition of the atmosphere, and post-depositional processes. Published papers reporting data on the chemical composition of snow seldom consider the fact that crystal formation and growth in cloud (rimed or unrimed) or near the ground (clear-sky precipitations), hoar-frost formation and surface riming determine different chemical concentrations, even assuming constant background concentration in the atmosphere. This paper discusses the physical and chemical processes affecting the formation of precipitations in polar areas, and the process of scavenging gases from non-growing and growing crystals. Attention is mainly focused on the processes involving nitrate anion in snow, hoar frost and firn. Knowledge of the chemical relationship between surface snow and atmospheric chemical concentration could be enhanced by considering specific events, such as snow falling from cloud, clear sky precipitation, and surface hoar or riming surface, with simultaneous air sampling. In conclusion, field and laboratory experiments are still required to study the scavenging processes during crystal formation.展开更多
Scanning Mobility Particle Sizer (SMPS) spectrometers are subject to several restrictions when a radioactive source is employed to bring the aerosol to a steady-state charge distribution. An alternative solution, comm...Scanning Mobility Particle Sizer (SMPS) spectrometers are subject to several restrictions when a radioactive source is employed to bring the aerosol to a steady-state charge distribution. An alternative solution, commercially available, is represented by the soft X-ray neutralizer. The present study investigates the outcome of a combination of a Grimm SMPS, which employs a 241Am radioactive source, with the soft X-ray advanced aerosol neutralizer (TSI model 3087). To date, the latter device has been interfaced only with TSI’s Electrostatic Classifiers. Particle size distribution of sodium chloride aerosol was measured with both neutralizers and it was found that the particle number concentration agreed to be within 9% for the 10 - 700 nm range. This difference mainly corresponds to the bias reported by TSI, when the X-ray device is mounted on a TSI spectrometer. It was concluded that the X-ray neutralizer could be usefully employed, as a standalone device, in combination with Grimm Electrostatic Classifiers.展开更多
Measurements of ice crystal concentrations in mixed clouds tend to exceed ice nucleus concentrations measured in nearby clear air. This discrepancy is a source of uncertainty in climate change projections as the radia...Measurements of ice crystal concentrations in mixed clouds tend to exceed ice nucleus concentrations measured in nearby clear air. This discrepancy is a source of uncertainty in climate change projections as the radiative properties of mixed phase clouds are largely determined by their liquid and ice water content. The ice enhancement process can sometimes depend on secondary ice production, which can occur through ice crystal fracture during sublimation, cloud drop shattering during freezing or following collision with ice particles. However, the discrepancy is observed even in mixed clouds where only primary ice nucleation processes occur. Several hypotheses have been suggested for the observed discrepancies. One factor could be the existence in clouds of pockets of high vapor supersaturation formed by droplet freezing or removal of small droplets by collision with larger droplets, associated with the fact that ice crystal concentration increases with water supersaturation. However, ice crystal concentrations are usually measured at near water saturation. Additional factors could be drop freezing during evaporation and activation of droplet evaporation residues. Here we suggest that a major factor could be underestimation of the contact freezing mode as it is not measured in experimental campaigns and seldom considered in nucleation models. Laboratory experiments give only incomplete answers to the important questions concerning the contact freezing mode, e.g. what fraction of the aerosol particles that come into contact with the droplet surface results in a freezing event and what is the influence of particle type and size, air temperature and relative humidity. As supercooled droplets grow or evaporate in mixed clouds, phoretic forces should play an important role in the collision efficiency between aerosol and droplets, and consequently in contact freezing. A further question is the possibility that aerosol, usually not active in deposition or condensation/immersion freezing, can trigger ice nucleation by colliding with supercooled droplets.展开更多
Most conventional aerosol neutralizers are based on radioactive sources, which are controlled by strict regulations restricting their handling, transport, and storage. The TSI 3087 soft X-ray （SXR） neutralizer circu...Most conventional aerosol neutralizers are based on radioactive sources, which are controlled by strict regulations restricting their handling, transport, and storage. The TSI 3087 soft X-ray （SXR） neutralizer circumvents these legal restrictions. The aim of the present work is to compare the performance of a standalone SXR aerosol neutralizer with that of conventional radioactive aerosol neutralizers based on 85Kr （TSI 3077） and 241Am （Grimm 5522） by performing field tests in a real environmental scenario. The results obtained when the SXR neutralizer was connected to a mobility particle sizer spectrometer （MPS）, different from the device suggested by the manufacturer, were comparable with those obtained with the use of radioactive aerosol neutralizers. In changing the neutralizer, the particle number concentrations, measured with the MPS connected to the SXR neutralizer, almost remained within the 10% uncertainty bounds for the particle size interval 10-300 nm, when diffusion losses inside the SXR tube were considered. Based on our comparisons, the SXR neutralizer can be regarded as a standalone instrument that could solve the problems associated with legal restrictions on radioactive neutralizers and fulfil the need for a portable instrument for different field test purposes.展开更多
文摘The role of phoretic forces in the identification of particles acting as ice nuclei in mixed phase cloud is discussed. A method used to identify the effective ice nucleating particles is to sample ice crystals, which are afterwards sublimated, and to examine the particles remaining after evaporation. The procedure takes into account only crystal with a maximum diameter of 20 μm, by assuming that small crystals do not scavenge aerosol during growth, and therefore that crystals contain only the effective nucleating particles. This assumption is questionable, however, as experiments have shown that even small ice crystals can scavenge aerosol. Another approach has been to compare the number and elemental composition of residual particles in small ice crystals and of aerosol near the cloud. By considering as example soot and black carbon aerosol, contradictory conclusions on their importance in the processes of ice nucleation have been reported in the literature. We suggest that, in addition to physico-chemical properties of soot/carbon aerosol particles, even the microphysical and environmental parameters involved in the transition of aerosol from gas phase to ice crystals in cloud should be considered. The contribution of phoretic forces should also be considered. After initial growth ice crystals can continue to grow by water vapour diffusion. Laboratory experiments confirm the contribution of diffusiophoresis with Stefan flow in the scavenging by snow crystals up to 3 mm in diameter. The particle scavenging efficiency of snow crystals is related to crystalline shape and depends on air relative humidity and temperature.
文摘Nanoparticles in air are of particular concern for public health and employee exposure in work-places. Therefore, it is very important to prepare effective filters for their removal. In this work filters were prepared from nanocellulose, i.e. cellulose nanofibrils (CNF). CNF was produced using two methods giving two different qualities of CNF. One quality had negative charges on the fibril surfaces while the other was neutral, and had in addition thinner fibrils compared to the other qualities. Filter samples were produced from water dispersions of CNF, by removal of the water by freeze drying. The performance of the CNF based filters was assessed and compared with filters based on synthetic polymer fibres. The ability to collect NaCl particles with a broad size distribution, ranging from nanometer to micrometer scale, was determined. CNF filters showed quality values comparable with the synthetic polymer based filters. Filters based on both the two CNF qualities had very good filtration efficiency for a given pressure drop across the filter.
文摘The paper addresses some of the problems surrounding the relation between ice core chemical signals and atmospheric chemical composition in polar areas. The topic is important as the reconstruction of past climate and past atmospheric chemical composition is based on the assumption that chemical concentrations in the air, snow, firn and ice core are correlated. Ice core interpretation of aerosol is more straightforward than that of reactive gases. The transfer functions of gaseous species strongly interacting with ice are complex and additional field and laboratory experiments are required. Ice core chemical signals depend on the chemical composition of precipitations, which are related to the physics of precipitation formation, the chemical composition of the atmosphere, and post-depositional processes. Published papers reporting data on the chemical composition of snow seldom consider the fact that crystal formation and growth in cloud (rimed or unrimed) or near the ground (clear-sky precipitations), hoar-frost formation and surface riming determine different chemical concentrations, even assuming constant background concentration in the atmosphere. This paper discusses the physical and chemical processes affecting the formation of precipitations in polar areas, and the process of scavenging gases from non-growing and growing crystals. Attention is mainly focused on the processes involving nitrate anion in snow, hoar frost and firn. Knowledge of the chemical relationship between surface snow and atmospheric chemical concentration could be enhanced by considering specific events, such as snow falling from cloud, clear sky precipitation, and surface hoar or riming surface, with simultaneous air sampling. In conclusion, field and laboratory experiments are still required to study the scavenging processes during crystal formation.
文摘Scanning Mobility Particle Sizer (SMPS) spectrometers are subject to several restrictions when a radioactive source is employed to bring the aerosol to a steady-state charge distribution. An alternative solution, commercially available, is represented by the soft X-ray neutralizer. The present study investigates the outcome of a combination of a Grimm SMPS, which employs a 241Am radioactive source, with the soft X-ray advanced aerosol neutralizer (TSI model 3087). To date, the latter device has been interfaced only with TSI’s Electrostatic Classifiers. Particle size distribution of sodium chloride aerosol was measured with both neutralizers and it was found that the particle number concentration agreed to be within 9% for the 10 - 700 nm range. This difference mainly corresponds to the bias reported by TSI, when the X-ray device is mounted on a TSI spectrometer. It was concluded that the X-ray neutralizer could be usefully employed, as a standalone device, in combination with Grimm Electrostatic Classifiers.
文摘Measurements of ice crystal concentrations in mixed clouds tend to exceed ice nucleus concentrations measured in nearby clear air. This discrepancy is a source of uncertainty in climate change projections as the radiative properties of mixed phase clouds are largely determined by their liquid and ice water content. The ice enhancement process can sometimes depend on secondary ice production, which can occur through ice crystal fracture during sublimation, cloud drop shattering during freezing or following collision with ice particles. However, the discrepancy is observed even in mixed clouds where only primary ice nucleation processes occur. Several hypotheses have been suggested for the observed discrepancies. One factor could be the existence in clouds of pockets of high vapor supersaturation formed by droplet freezing or removal of small droplets by collision with larger droplets, associated with the fact that ice crystal concentration increases with water supersaturation. However, ice crystal concentrations are usually measured at near water saturation. Additional factors could be drop freezing during evaporation and activation of droplet evaporation residues. Here we suggest that a major factor could be underestimation of the contact freezing mode as it is not measured in experimental campaigns and seldom considered in nucleation models. Laboratory experiments give only incomplete answers to the important questions concerning the contact freezing mode, e.g. what fraction of the aerosol particles that come into contact with the droplet surface results in a freezing event and what is the influence of particle type and size, air temperature and relative humidity. As supercooled droplets grow or evaporate in mixed clouds, phoretic forces should play an important role in the collision efficiency between aerosol and droplets, and consequently in contact freezing. A further question is the possibility that aerosol, usually not active in deposition or condensation/immersion freezing, can trigger ice nucleation by colliding with supercooled droplets.
文摘Most conventional aerosol neutralizers are based on radioactive sources, which are controlled by strict regulations restricting their handling, transport, and storage. The TSI 3087 soft X-ray （SXR） neutralizer circumvents these legal restrictions. The aim of the present work is to compare the performance of a standalone SXR aerosol neutralizer with that of conventional radioactive aerosol neutralizers based on 85Kr （TSI 3077） and 241Am （Grimm 5522） by performing field tests in a real environmental scenario. The results obtained when the SXR neutralizer was connected to a mobility particle sizer spectrometer （MPS）, different from the device suggested by the manufacturer, were comparable with those obtained with the use of radioactive aerosol neutralizers. In changing the neutralizer, the particle number concentrations, measured with the MPS connected to the SXR neutralizer, almost remained within the 10% uncertainty bounds for the particle size interval 10-300 nm, when diffusion losses inside the SXR tube were considered. Based on our comparisons, the SXR neutralizer can be regarded as a standalone instrument that could solve the problems associated with legal restrictions on radioactive neutralizers and fulfil the need for a portable instrument for different field test purposes.
