专利摘要:
The invention relates to a method for selective aerosol purification. The invention consists in an electrostatic collection of all the particles present in an aerosol, but with a decoupling of the mechanisms of one part charge of the particles by diffusion of unipolar ions to charge and then collect the finest particles, and on the other hand charging by electric field with corona effect to charge and collect the largest particles on a substrate different from the collection substrate of the finest particles.
公开号:FR3039433A1
申请号:FR1557224
申请日:2015-07-28
公开日:2017-02-03
发明作者:Michel Pourprix;Christophe Brouard;Simon Clavaguera
申请人:Commissariat a lEnergie Atomique CEA;Commissariat a lEnergie Atomique et aux Energies Alternatives CEA;
IPC主号:
专利说明:

SELECTIVE AEROSOL PURIFICATION METHOD
Technical area
The present invention relates to the aerosol purification area, which may contain suspended particles.
The present invention aims to improve the methods of aerosol purification by electrostatic precipitation in order to allow a collection of particles in suspension in aerosols which is simultaneous but selective according to their dimensions, the selectivity preferably targeting, to collect in them. separating the micron-sized particles and the nanoscale particles.
By "nanoparticle" is meant the usual definition according to ISO TS / 27687: a nano-object whose three dimensions are at the nanoscale, ie a particle whose nominal diameter is less than About 100 nm.
State of the art
Since the 1970s, the awareness of the environmental and health effects caused by aerosols has been at the origin of new technological developments to better assess the associated risks.
The field expanded rapidly in the 1980s to include the use of aerosols in high-tech production processes, and the control of aerosol contamination in ultra-clean atmospheres. Since the 1990s, research has intensified on the properties of ultrafine particles, i.e. those smaller than 100 nm, and on the effect of aerosols on the climate. The field is therefore very broad since it covers the field of industrial hygiene, control of air pollution, inhalation toxicology, physics and atmospheric chemistry, and contamination by radioactive aerosols in facilities or the environment.
More recently, the rapid growth of nanotechnology in various fields such as health, microelectronics, energy technologies or consumer products such as paints and cosmetics makes it essential to continue work on health and environmental impacts. these new materials to surround themselves with optimal safety conditions.
It is therefore necessary to develop methods and tools for assessing the exposure of particles, particularly nanoparticles, to workers, consumers and the environment.
The development of methods and devices for sampling and analyzing aerosols in a wide range of particle sizes up to nanometric sizes is thus a crucial issue in terms of public health and the prevention of associated risks.
In particular, the development of sampling devices adapted to be portable and to be attached to the unit to a combination of work of a worker in the nano-objects manufacturing, nanomaterials production or use of nanomaterials could be imperative.
To collect and collect particles suspended in aerosols, for analysis in situ or in the laboratory, many devices exist. They can implement a collection by filtration on fibers or on porous membranes, a collection by diffusion for the finest particles, a collection under the effect of a field of forces of inertia (impactors, cyclones, centrifuges) or of gravity (sedimentation chambers, elutriators) for larger particles, or a collection under the effect of a field of electrical, thermal or radiative forces.
Among these devices, those electrostatic, that is to say whose operating principle is based on the implementation of an electric field, in particular an intense electric field to create a corona discharge effect (in English " corona discharge ") are commonly used.
When an intense electric field is generated in a volume where aerosol particles are present, these can be electrically charged according to two distinct charge mechanisms and this can occur concomitantly.
Publication [1], particularly Figure 15.4 on page 330 of this book, shows that the unipolar ion diffusion electric charge mechanism associated with the field charge mechanism is applicable to a wide range of sizes. of particles, at least for particles with dimensions of between 0.01 and 10 μm. It also appears that the mechanism of unipolar ion diffusion electric charge is especially predominant for the finest particles, typically nanoparticles, that is to say those of dimensions less than 100 nm. On the other hand, the field charge mechanism is more efficient for large particles, ie micron and submicron sized particles (> 300 nm). For example, if we consider the electrical mobility of a particle, noted Z, of the order of 1 cm2 / st.Vs in electrostatic unit CGS, or 3.3x10 ~ 7 m2 / Vs in SI unit then this particle placed between two plane and parallel plates which generate an electric field E of 105 V / m, acquires a speed W equal to the product Z * E, ie W of the order of 0.033 m / s. It is clearly demonstrated that the electrostatic force generates velocities far superior to the other force fields undergone by a particle, namely the fields of gravity, inertial, thermal and radiative. This advantage is exploited in the operation of commercial electrostatic purifiers, where diffusion charging and field charging processes can act together.
Electrically charging aerosol particles requires the presence of unipolar ions in high concentration. By far the most effective method for creating these ions in atmospheric air is the corona discharge.
To produce a corona discharge, an electrostatic field must be established in a geometry that makes it non-uniform. More precisely, this high electric field (several thousands to tens of thousands of volts per centimeter in the vicinity of the discharge electrode) is induced by two electrodes arranged close to each other: a first polarized electrode or electrode of discharge, generally in the form of wire or tip, being disposed opposite a second electrode, the latter being in the form of a counter-electrode, generally flat or cylindrical geometry. The electric field existing between the two electrodes ionizes the volume of gas located in the inter-electrode space, and in particular a sheath or ring of ionized gas located around the discharge electrode. The charges created, migrating towards the counter electrode, charge the particles to be separated contained in the gas. The charged particles thus created migrate to the counter electrode, where they can be collected. This counterelectrode is usually called a collection electrode. Due to the level of the required electric field, it is necessary to use a discharge electrode which has a (very) small radius of curvature. The discharge electrodes encountered are therefore generally either fine points or small diameter wires. Thus, by a process that originates from the electrons and ions created by natural irradiation, the electrons are accelerated in the intense electric field created near the (very) small radius of curvature electrode. By the high voltage imposed, if this field exceeds a critical value, an avalanche effect causes the ionization of the air in this space. This phenomenon is called corona discharge. By way of example, FIGS. 1A to 1E show a few configurations of electrodes most suitable for obtaining a corona discharge, namely respectively a tip-plane arrangement (FIG. 1A), plane-blade (FIG. plane (Figure IC), wire-wire (Figure 1D), wire-cylinder (Figure 1E).
For example, in the tip-plane configuration, if the tip is positive with respect to the plane, the electrons move rapidly towards the tip while the positive ions move towards the plane, thus creating a positive unipolar space. In addition, a wind of ions, also called ionic wind, is established, characterized by a flow of air directed from the point towards the plane, having as origin the shocks of the positive ions with the surrounding neutral molecules. Conversely, if the tip is negative to the plane, the positive ions move toward the tip, and the electrons move toward the plane by attaching themselves to the air molecules to form negative ions. In all cases, even if the process of creating positive or negative ions is not exactly symmetrical, the unipolar ions migrate from the tip to the plane with a high concentration of the order of 106 to 109 / cm3 and, whatever the polarity, it appears an electric wind directed from the point towards the plane.
Thus, the introduction of aerosol particles in the tip-plane space makes it possible to charge them with the same polarity as the tip, according to a field charging process. In addition, the field used to create the corona effect and the electric wind also participate in the field charging process.
For the other configurations shown in FIGS. 1B to 1E, the processes of ion generation and field charge of the particles are in all respects similar. It is on this principle that certain commercially available electrostatic precipitators are used which are used to collect and collect particles on a support allowing the analysis.
For example, FIG. 15.9 on page 341 of the publication [1] already cited shows an arrangement for the deposition of aerosol particles on an electron microscope grid, the particles being charged and precipitated in a tip-plane configuration.
Another example is illustrated in Figure 10.10 of page 223 of this same publication [1] and implements the charge and precipitation technique in point-plane geometry for collecting aerosol particles on a piezoelectric crystal.
As already mentioned, the unipolar ion diffusion charging mechanism applies predominantly to the finest particles. This mechanism is increasingly used in the metrology of nanoparticles, in particular to determine their particle size. In fact, many authors have studied and are still studying devices capable of conferring high electrical mobilities on the finest particles, in order to be able to select them in instruments adapted to this new domain. One can cite here in particular the article [2] which makes an inventory of most of the technologies developed to date, or the principle developed by the author of the publication [3], which uses a thread configuration. cylinder, much studied more recently as indicated in the publication [4], but also before (publication [5]).
FIG. 2 schematically reproduces a charging device, also known as a charger, for unipolar ion diffusion whose geometry is of the wire-cylinder type, as illustrated in the publication [4]. The charger 10 comprises a two-part symmetrical body of revolution 1 which holds a hollow metal cylinder 11 forming an external electrode connected to an AC power supply and a central wire 12 arranged along the axis of the body and connected to a power supply. high voltage not shown. Around the central wire 12 is also annularly arranged a cylindrical grid 14 forming an inner electrode. The aerosol containing the particles to be charged flows in the charger 10 from the inlet orifice 17 to the outlet orifice 18 by passing through the space delimited between the inner electrode 14 formed by the gate and the outer electrode 11 formed by the cylinder.
The operation of this charger 10 is as follows: ions are produced by corona effect at the central wire 12 and are collected by the inner mesh electrode 14 brought to a low potential, typically grounded. Part of these ions out of this gate 14 to go to the inner surface of the peripheral cylinder 11 due to the voltage applied to the latter. The aerosol particles pass through the space between grid 14 and cylinder 11 and are therefore diffusion-loaded by the unipolar ions coming out of gate 14. The diffusion charging mechanism operates according to product N * t, where N represents the concentration of unipolar ions and t the residence time of the particles. The diffusion charging mechanism is the only one that can occur because there can be no field charge mechanism since the electric field is very small in space 15.
It is interesting to note that the unipolar ion diffusion aerosol loading process makes it possible to confer a given number of electric charges on a particle of a given size.
This principle is also implemented in differential electric mobility analyzers (DMA), which are instruments capable of providing the particle size distribution of fine particles by counting the particle concentration in a given class of electric mobility. Such a device is for example implemented in US Patent 8044350 B2. It emerges from the study of the state of the art that it has not been proposed to simultaneously collect particles present in an aerosol which are of different sizes in a wide range, typically between a few nanometers and a few tens of micrometers, and to separate them in restricted size ranges, preferably separate nanoparticles from micron-size particles.
Different methods of electrostatic precipitation exist to purify an aerosol. To the inventors' knowledge, none of these methods makes it possible to collect and separate the particles contained in the aerosol, according to their restricted size range.
However, there is a need for such a method, in particular to remove fine particles to keep only large ones. A concrete application is the measurement of atmospheric contamination by radioactive aerosols.
The general object of the invention is then to respond at least in part to this need.
Presentation of the invention
To do this, the invention firstly relates to a selective aerosol purification method comprising the following steps: aerosol suction in a conduit, preferably cylindrical, from its inlet, charging the thinnest particles downstream of the inlet port by diffusion of unipolar ions in a space between an electrode in the form of a grid surrounding an electrode in the form of a wire, and a first conductive portion of the inner wall of the duct, - generation of an electric field without corona effect in the space between an electrode and a second conductive portion of the inner wall of the duct, in order to collect by deposition on a first collection substrate (Zn) the finest particles charged by the diffusion charger, - generation of an electric field with a corona effect in the space between the wire or tip of an electrode and a third portio n conductor of the inner wall of the conduit, to collect by depositing on a second collection substrate (Zm) separate from the first collection substrate, the largest particles, not loaded by the diffusion charger, - extraction of air clean of the outlet of the conduit.
The method may further comprise at least one step of recycling or recovering the finest particles collected on the first substrate and / or the largest particles collected on the second substrate.
Thus, the invention consists in an electrostatic collection of all the particles present in an aerosol, but with a decoupling of the mechanisms on the one hand charge of the particles by diffusion of unipolar ions to charge and then collect the finest particles and on the other hand corona electric field charging to charge and collect the largest particles on a substrate different from the collection substrate of the finest particles.
In other words, the invention consists in first electrically charging the fine particles by diffusion of unipolar ions, then charging the large particles by an electric field and collecting each group of charged particles according to their size on a adequate support.
Thus, the invention makes it possible judiciously to classify the particles according to their particle size by depositing them in physically distinct zones.
For particular applications, the method according to the invention makes it possible to separate the finest fraction of the particles while allowing the larger fraction to pass through. The application to the early detection of incidents by measurement of atmospheric contamination by radioactive aerosols in certain workshops is proposed.
An alternative is the collection of particles of recoverable material or strategic raw materials present in particulate form in aerosols.
According to an advantageous variant of the invention, the method further comprises the following steps: a / collection of radioactive particles on the first and / or second collection substrate for a time t1; b / count of pulses generated by the air ionization current in the spaces during a time t2.
DETAILED DESCRIPTION Other advantages and features will become more apparent upon reading the detailed description, given by way of nonlimiting illustration, with reference to the following figures in which: FIGS. 1A to 1E are schematic views of different electrode configurations to obtain a corona effect by electric discharge; - Figure 2 is a longitudinal sectional view of a charging device, or unipolar ion diffusion charger; FIG. 3 is a diagrammatic view in longitudinal section of a first example of a device for collecting particles according to the invention.
Throughout the present application, the terms "inlet", "outlet", "upstream" and "downstream" are to be understood by reference to the direction of the suction flow through a collection device according to the invention. 'invention. Thus, the inlet port refers to the orifice of the device by which the aerosol containing the particles is sucked while the outlet means the one through which the air flow exits.
Figures IA to 1E and 2 have already been commented on in the preamble. They are not detailed below.
FIG. 3 shows an example of an electrostatic device according to the invention 1 for the selective purification of an aerosol capable of containing particles.
Such a device according to the invention makes it possible to purify the aerosol by collecting at the same time the finest particles, such as the nanoparticles and the larger particles, such as those of micron size while separating them from one another. other according to their size range.
The purification device 1 comprises first a conduit 11 which is a hollow cylinder of revolution about the longitudinal axis X and which is electrically connected to the zero potential.
The collection device 1 comprises inside the duct 11, upstream to downstream, between its inlet orifice 17 and its outlet orifice 18, four distinct stages 10, 20, 30, 40.
The first stage consists of a unipolar ion diffusion charger 10, and is similar to that previously described in connection with FIG.
The charger 10 thus comprises a central electrode which extends along the X axis in the form of a wire 12 connected to a supply delivering a high voltage 13, adapted to thereby create a corona discharge in the vicinity of the wire 12.
It also comprises a peripheral electrode in the form of a gate 14 connected to a low voltage power supply 16. The stage 20, downstream of the charger 10, comprises a central electrode which extends along the X axis in the form of a rod 22 connected to a power supply delivering a medium voltage 23, adapted to create without corona effect an electric field of collection in the space 21 between the central electrode 22 and the wall of the conduit 11. A hollow cylinder 24 conforming to the wall of the duct and constituting a first collection substrate Zn is arranged around the rod 22 facing it. The stage 30, downstream of the stage 20, comprises a central electrode which extends along the X axis in the form of a wire 32 connected to a high voltage supply 33, adapted to create a corona effect in the vicinity the wire 32 and therefore an intense electric field in the space 31 separating the central wire 32 of the conduit 11. A hollow cylinder 34 conforming to the wall of the conduit and constituting a second collection substrate Zm is arranged around the wire 32 opposite the one -this.
Stage 40 comprises a structure 41, for example "honeycomb", adapted to prevent the appearance of a vortex in the conduit 11, and downstream a suction device 42. Depending on the configurations, the collection device according to the invention can overcome the 4L structure
The operation of the collection device which has just been described with reference to FIG. 3 is as follows. The air containing the particles to be collected is sucked by the inlet orifice 17 by the action of the suction device 42.
The finest particles of the aerosol are electrically charged by diffusion of unipolar ions in the space 15 separating the gate 14 from the conduit 11.
These finest particles, with high electrical mobility, and the other larger particles with lower electric mobility, penetrate into stage 20.
The electric field without corona effect created in the space 21 between the rod 22 and the cylinder 24 ensures the collection of the finest particles on the latter by defining the first collection substrate Zn.
The other larger particles are not collected and still present in the aerosol that enters the third stage 30.
These larger particles are then electrically charged under the effect of the corona discharge near the wire 32 and the intense field prevailing in the space 31 and are collected on the inner wall of the cylinder 34 by defining the second collection substrate Zm . The purified air of both the finest particles deposited on the first collection substrate Zn and larger particles Zm deposited on the second collection substrate Zm is then discharged through the outlet 18 of the device.
Each collection cylinder 24, 34 can be easily extracted from the duct once the targeted collection has been carried out.
Depending on the application sought, each of the Zn and Zm substrates can then be analyzed by conventional physical or physico-chemical characterization techniques, such as optical or electronic microscopy, surface scanner, α, β, γ spectrometry if the particles are radioactive. , X-ray fluorescence spectroscopy (XRF), X-ray fluorescence (μ-XRF), laser-induced breakdown spectroscopy particle size on the one hand of the finest particles and on the other hand the largest particles, their concentration, their chemical composition and / or their morphology.
One particular application relates to the detection of the presence of radioactive particles on the collection substrates without it being necessary to extract them.
In fact, sequentially, after a collection phase for a time t1, the device as illustrated in FIG. 3 makes it possible to operate the stages 20 and 30 as an ionization chamber for a time t2.
By an appropriate electronic device, but conventional in nuclear instrumentation, the measurement of the ionization current in each stage 20 and 30 makes it possible to detect the presence of radioactive particles with a double interest: - early detection of an incident in a nuclear installation by a monitoring the atmospheric contamination of the air in the premises, - separating radionuclides into two fractions of different sizes: the smallest particles in space 20, the largest particles in space 30.
This last point is of major importance. Indeed, it is often necessary to separate, on the one hand, the aerosol particles that we want to detect (such as plutonium particles in the workshops where the aerosol size is of the order of 5 μm (diameter median aerodynamic)), on the other hand the natural aerosol carrying the descendants of radon (a much thinner aerosol) which constitutes an undesirable background noise. This natural background may mask the measurement of the desired radionuclide traces. The interest of such a separation is well described in the book in reference [6] page 647 in the paragraph entitled "Mitigation of Interference front Radon Progeny", and in the article [7]. Other variants and improvements can be made without departing from the scope of the invention, especially for other applications where the interest of separating an aerosol into two distinct particle size classes is sought, in particular for valuing the most fines collected on the first substrate and / or larger particles on the second substrate. The invention is not limited to the examples which have just been described; it is possible in particular to combine with one another characteristics of the illustrated examples within non-illustrated variants. References cited [1]: W. Hinds, "Aerosol Technology", 2nd Edition, 1999.
[2]: P. Intra and N. Tippayawong, "Aerosol an Air Quality Research", 11: 187-209, 2011; [3]: G.W. Hewitt, "The Charging of Small Particle for Electrostatic Precipitation", ATF.F, Trans., 76: 300-306, 1957; [4]: G. Biskos, K. Reavell, N. Collings, "Electrostatic Characterization of Corona-Wire Aerosol Chargers", J. Electrostat. 63: 69-82, 2005; [5]: D.Y.H. Pui, S. Fruin, P. H. McMurry, "Unipolar Diffusion Charging of Ultrafine Aerosols", Aerosol Science Technology 8: 173-187, 1988; [6]: P. Kulkarni, P. A. Baron, K. Willeke, "Aerosol Measurement", 3rd Edition, 2011.
[7]: C. Monsanglant-Louvet, F. Gensdarmes, N. Liatimi, S. Pontreau "Evaluation of the performance of monitors of atmospheric contamination in real operating conditions", Scientific and technical report, IRSN: 251-259, 2008.
权利要求:
Claims (3)
[1" id="c-fr-0001]
1. A method of selective aerosol purification comprising the following steps: - aspiration (18, 42) of the aerosol in a conduit, preferably cylindrical (11) from its inlet (17), - particle charge the thinnest ones, downstream of the inlet, by diffusion of unipolar ions (10) in a space (15) between an electrode in the form of a grid (14) surrounding an electrode in the form of a wire (12), and a first conductive portion of the inner wall of the conduit; - generation of a non-corona electric field in the space (21) between an electrode (22) and a second conducting portion (24) of a wall interior of the duct, in order to collect by deposition on a first collecting collection substrate (Zn) the finest particles charged by the diffusion charger, - generating an electric field with a corona effect in the space (31) between the wire or tip of an electrode (32) and a third conductive portion (34, 6) of the inner wall of the conduit, for depositing on a second collection substrate (Zm) separate from the first collection substrate, the largest particles, not loaded by the diffusion charger, extraction of the purified air from the outlet orifice (18) of the duct.
[2" id="c-fr-0002]
2. The purification method according to claim 1, further comprising at least one step of recycling or recovery of the finest particles collected on the first substrate and / or the largest particles collected on the second substrate.
[3" id="c-fr-0003]
The purification method according to claim 1 or 2, further comprising the steps of: a) collecting radioactive particles on the first and / or second collection substrate for a time t1; b / counting of pulses generated by the ionization current of the air in the spaces (21, 31) for a time t2.
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FR3039433B1|2015-07-28|2017-08-18|Commissariat Energie Atomique|SELECTIVE AEROSOL PURIFICATION METHOD|FR3039433B1|2015-07-28|2017-08-18|Commissariat Energie Atomique|SELECTIVE AEROSOL PURIFICATION METHOD|
FR3039435B1|2015-07-28|2017-08-18|Commissariat Energie Atomique|METHOD AND DEVICE FOR COLLECTING AEROSOL PARTICLES, WITH SELECTIVE COLLECTION BASED ON PARTICLE GRANULOMETRY|
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2016-07-29| PLFP| Fee payment|Year of fee payment: 2 |
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优先权:
申请号 | 申请日 | 专利标题
FR1557224A|FR3039433B1|2015-07-28|2015-07-28|SELECTIVE AEROSOL PURIFICATION METHOD|FR1557224A| FR3039433B1|2015-07-28|2015-07-28|SELECTIVE AEROSOL PURIFICATION METHOD|
PCT/EP2016/068002| WO2017017185A1|2015-07-28|2016-07-28|Method for the selective purification of aerosols|
US15/744,362| US10799883B2|2015-07-28|2016-07-28|Method for the selective purification of aerosols|
CN201680043735.XA| CN107847945B|2015-07-28|2016-07-28|Method for selectively purifying aerosols|
EP16750678.1A| EP3328549B1|2015-07-28|2016-07-28|Method for the selective purification of aerosols|
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