Patent Application
20180318778
This invention relates to the field of preparing granular mediums, and more precisely to the mixing of powders, in particular of actinide powders, and to the deagglomeration/reagglomeration thereof in order to obtain a mixture of high homogeneity through a cryogenic fluid, also called a cryogenic median.
In a privileged manner, it applies to high density and/or cohesive powders, such as actinide powders. The invention as such preferably has application for the mixing of actinide powders allowing for the formation of nuclear fuel, in particular pellets of nuclear fuel.
The invention as such proposes a device for mixing powders by a cryogenic fluid, as well as an associated method for mixing powders.
Implementing different steps for preparing a granular medium, in particular from actinide powders in order to form pellets of nuclear fuel after forming by pressing, is essential as it substantially conditions the control of the microstructure of the final produce but also the presence or not of macroscopic aspect defects within a fuel pellet. In particular, the mixture of actinide powders in order to allow for the production of nuclear fuel constitutes a key step in the controlling of the quality of the fuel pellet obtained, which most often is subjected to compliance with strict requirements in terms of microstructure and impurities.
The industrial, conventional and historical method of powder metallurgy applied to the elaboration of nuclear fuel is based on steps of mixing, grinding and/or granulation, all carried out dry. Indeed, implementing liquid in the nuclear industry induces the generation of effluents that can be difficult to treat. Also, for the preparing of a granular medium for the purpose of elaborating nuclear fuel, procedures are not conventionally used other than those that use the dry method.
In order to carry out the mixing of powders, various devices are known in prior art, which can be broken down according to the families described hereinafter.
First of all, there is the principle of the dry phase mixer without internal media. This can in particular be a mixer of the Turbula® type from the company WAB which through movements that are more or less complex of the tank containing the powders to be mixed, allows for a more or less substantial homogenisation of the granular medium. Generally, the effectiveness of this type of mixture is limited. Indeed, according to the type of powders to be mixed, heterogeneous zones can subsist, for which the mixture does not take place or in the least incorrectly and inadmissibly. The kinematics of this type of mixture is generally not complex enough to induce a pushed mixture, i.e. a mixture that is satisfying in terms of homogeneity, without a pushed development itself or a mixing duration that is penalising at the industrial level. Moreover, the energy transmitted to the granular medium in this type of mixer does not make it possible to carry out deagglomeration that is sufficient to reach sufficient degrees of homogeneity in the case where the size of these agglomerates is excessive (in particular to be offset during the step of sintering).
The principle of the media mixture is also known. According to this principle and in order to favour the operation of mixing, one or several mobile facilities can be used within the tank containing the powder to be mixed. These mobile facilities can be blades, turbines, coulters, ribbons, endless screws, among others. In order to improve the mixing, the tank can itself be mobile. This type of mixer can be more effective than the preceding category but still remains insufficient and suffers from limitations. Indeed, the mixing induces a modification in the granular medium via agglomeration or a deagglomeration that is difficult to control, which induces an overrunning of powders and/or a degradation in the flowability of the granular medium. Moreover, the use of mobile facilities (media) for mixing results in pollutions (contaminations) when it concerns mixing abrasive powders such as those that have to be implemented to produce nuclear fuel. In addition, the mobile facilities implemented induce retentions which generate flow rates of doses that have a substantial impact in the case of elaborating nuclear fuel.
There is also the principle of the mixer of the grinder type. Indeed, according to the usage mode and the type of technology of certain grinders, it is possible to produce mixtures of powders via co-grinding. This type of operation makes it possible to obtain a satisfactory mixture, from a homogeneity standpoint, but requires a relatively long grinding time, typically several hours, and also induces grinding phenomena that reduce the size of the particles of powders. This causes the generation of fine particles and a modification in the specific surface which also affects the possibility of using the powders later after the mixing thereof (modification in flowability, reactivity (possible oxidation), sinterability of the powders, etc.). In the framework of manufacturing nuclear fuel, the operation of co-grinding, by generating fine particles causes a non-negligible radiological impact, due to the retention and the propensity of the fine particles to disperse. Moreover, clogging phenomena can be induced.
After using these various types of mixers, it is often necessary to carry out an agglomeration or granulation. In addition, these devices are generally discontinuous, which can be an issue in industrial methods.
Generally, the aforementioned mixers are not fully satisfactory for mixing certain powders, such as actinide powders, and it is necessary to follow this with a step of granulation in order to obtain a flowable granular medium.
Other mixtures are also known, implementing a multiphase medium, namely fluid-solid phases. These mixers can be classified into two main categories described hereinafter.
First of all, there are mixers of the liquid/solid type. These mixes do not work for the implementing of powders soluble with the liquid phase used in the mixer or if the powders are modified by the contact with the fluid. Moreover, for powders that have a high density compared to the liquid introduced into the mixer, the mixture is most often not effective or requires substantial agitation speeds. Indeed, the pulling-off speed of a particle from the bottom of the agitator is directly linked to the difference in density between the particles constituting the powders and that of the liquid allowing for the placing in suspension. In this case, viscous liquids can be used but this induces an increased energy demand, and this proportionately to the increase in viscosity before reaching a turbulent regime to favour the mixing. Moreover, in this case of the mixer of the liquid/solid type, there is also the question of the separation of the liquid phase and of the solid phase after mixing. In the case of the mixture of actinide powders, this type of mixture would induce contaminated effluents that are very complicated to retreat, which is prohibitive. Furthermore, in practice, complete and homogeneous placing in suspension cannot be achieved when powders of a low granulometry are to be mixed. More precisely, in order to achieve optimum homogenisation, the so-called Archimedes dimensionless number must be greater than 10 (i.e. the forces of viscosities are less than the forces of gravity and inertia). Knowing that the particles that constitute powders to be mixed have relatively low diameters, typically less than 10 μm, it cannot be considered to produce homogenous and complete suspensions with this type of device without using additional means of mixing. In that respect, technologies, such as that described in patent application CA 2 882 302 A1, have been proposed but nevertheless remain inoperable for an application for mixing actinide powders, the means of vibration used do not allow for sufficient homogenisation with regards to the homogenisation objectives to be achieved and the particularities of actinide powders. In addition, for reasons of controlling criticality, the volume of the mixer has to be limited, in order to prevent any risk of double loading which could induce an exceeding of the permissible critical mass. Indeed, in a conventional liquid/solid mixer, the density of particles per volume of tank cannot be substantial, unless either exceeding an excessive agitation power, or undergoing a mixture kinetics that is too slow.
Finally note that mixers of powders in liquid phase, in particular of the type of those described in patent applications CA 2 882 302 A1, WO 2006/0111266 A1 and WO 1999/010092 A1, are not suited for the problem of a mixture of powders of the actinide powder type, because they would require excessively high agitation speeds to hope to pull off the powders from the bottom of the agitation tank and achieve levels of homogeneity that are in accordance with those sought in the nuclear industry. In addition, once again, they would induce contaminated effluents, difficult to manage industrially but also risks of criticality, even of radiolysis of the liquid phase used due to the fact of the nature of the powders to be implemented (beyond the fact that the latter can interact chemically with the liquid used).
Then, there are also mixers of the gas/solid type. This type of mixer can be operable and does not induce any risk of criticality. However, this type of mixer is hardly operable for powders that do not have sufficient fluidisation properties, conventionally C− type powders according to the classification of D. Geldart such as described in the publication Powder Technology, Vol. 7, 1973. However, this characteristic of poor fluidisation is encountered for cohesive actinide powders such as those implemented for manufacturing nuclear fuel. Moreover, beyond the difficulty in terms of fluidisation, with regards to the densities of the powders to be fluidised for the mixture, the superficial speed of the gas should be substantial and at least equal to the minimum speed of fluidisation. Also, this type of mixer appears hardly suitable for the mixing of cohesive powders and a fortiori with high density.
There is therefore a need to propose a new type of device for mixing powders for the preparation of granular mediums, and in particular for the mixing of actinide powders.
In particular, there is a need to be able at the same time to:
The invention has for purpose to overcome at least partially the needs mentioned hereinabove and the disadvantages pertaining to embodiments of prior art.
The invention has for object, according to one of its aspects, a device for mixing powders, in particular of actinide powders, by a cryogenic fluid, characterised in that it comprises at least:
Note that, usually, a cryogenic fluid here designates a liquefied gas retained in liquid state at low temperature. This liquefied gas is chemically inert in the conditions for implementing the invention, for the powders to be mixed and deagglomerated.
The device for mixing powders according to the invention can furthermore comprise one or several of the following characteristics taken individually or according to any technically possible combinations.
The cryogenic fluid can comprise a slightly hydrogenated liquid, which is a liquid comprising at most one hydrogen atom per molecule of liquid, having a boiling temperature less than that of water.
According to a first embodiment of the invention, the device can comprise means for mixing of the mixing chamber according to a movement of the gyroscopic type.
In particular, the means for mixing according to a movement of the gyroscopic type can allow for the putting into motion, even the rotation, of the mixing chamber according to the three axes of three-dimensional metrology. This type of agitation via gyroscopic movement can in particular make it possible to favour the mixing of powders when they have high densities compared to the density of the fluid phase of the cryogenic fluid located in the mixing chamber.
According to a second embodiment of the invention, the device can comprise:
Each mixing chamber can then comprise a cryogenic fluid, being in particular filled with a cryogenic fluid, and means for agitation, being in particular provided with means of agitation, so as to allow the mixing of the powders placed in suspension in the cryogenic fluid.
Moreover, the means of agitation can comprise mobile mixing facilities, in particular blades, turbines and/or mobile facilities with a duvet effect, among others.
These mobile mixing facilities can comprise grinding facilities, for example of the ball, roller type, among others.
In addition, the means of agitation can also comprise means for generating vibrations, in particular ultrasonic vibrations, in particular sonotrodes.
Furthermore, the systems for restricting the passage can comprise screens. The systems for restricting the passage can further comprise diaphragms.
The systems for restricting the passage can be adjusted and configured so that their section of passage is decreasing according to the flow of the powders through the plurality of mixing chambers, the section of passage of an (n−1)th system for restricting the passage being as such greater than the section of passage of an nth system of restricting the passage by following the flow of the powders.
In addition, the section of passage of the systems for restricting the passage can be less than the natural section of flow of the powders, in such a way that these powders are necessarily deagglomerated when they pass from one mixing chamber to the other. As such, the residence time of the particles to be mixed is intrinsically sufficient to allow for deagglomeration.
Moreover, the plurality of mixing chambers and the plurality of the systems for restricting the passage of the powders can advantageously be arranged according to the same vertical direction in such a way as to allow for a flow of the powders under the effect of gravity.
In addition, the device preferably comprises a system of electrostatic charge of the powders intended to be introduced into the mixing chamber or chambers.
A portion of the powders can in particular be placed in contact with a portion of the electrostatic charge system in order to be positively electrostatically charged and the other portion of the powders can be placed in contact with the other portion of the electrostatic charge system in order to be negatively electrostatically charged, in order to allow for a differentiated local agglomeration. In case of mixture of more than two types of powders, certain powders can be either positively charged, or negatively charged, or without charge.
The cryogenic fluid can moreover be of any type, being in particular liquefied nitrogen or argon. Note that the use of nitrogen is pertinent due to its low price but also due to the fact that the glove boxes and the methods implemented for the elaboration of the nuclear fuel with a plutonium base are inerted with nitrogen and the liquid nitrogen is itself used in certain operations on the fuel (BET measurement, etc.). The usage of this type of cryogenic fluid therefore does not induce any particular additional risk in the method of elaboration.
The device can very particularly comprise at least two chamber for supplying powders, and in particular as many chambers for supplying powders as there are types of powders to be fixed.
The chamber or chambers for supplying can comprise hoppers with adjustable supply and/or systems of the metering type, in particular vibrating plates or tunnels.
Furthermore, the invention further has for object, according to another of its aspects, a method for mixing powders, in particular of actinide powders, by a cryogenic fluid, characterised in that it is implemented by means of a device such as defined hereinabove, and in that it comprises the following steps:
a) introduction of powders intended to be mixed into the mixing chamber or chambers through the chamber or chambers for supplying,
b) mixing of the powders in the mixing chamber or chambers, placed in suspension in a cryogenic fluid, through means for agitation,
c) obtaining of a mixture formed from powders.
During the first step a), the powders can advantageously be electrostatically charged differently, in particular oppositely in the presence of at least two types of powders, in order to favour differentiated local agglomeration.
According to a first embodiment of the method, the device can comprise a single mixing chamber, and said mixing chamber can be moved by a movement of the gyroscopic type in order to allow for the mixing of the powders.
According to a second embodiment of the method, the device can comprise a plurality of mixing chambers of the powders, arranged successively in series one after the other, the chamber or chambers for supplying with powders allowing for the introduction of powders into at least the first mixing chamber, and a plurality of systems for restricting the passage of the powders, with each system for restricting the passage being located between two successive mixing chambers, in order to constrain the distribution of powders from one mixing chamber to the next, with each mixing chamber comprising a cryogenic fluid and means for agitation so as to allow the mixing of the powders placed in suspension in the cryogenic fluid, the method then being able to comprise the step consisting in progressively restraining the passage of the flow of the powders through the mixing chambers through systems for restricting the passage with a decreasing section of passage according to the flow of the powders.
The device and the method for mixing powders according to the invention can comprise any of the characteristics mentioned in the description, taken individually or according to any technically possible combinations with other characteristics.
The invention can be better understood when reading the following detailed description, of non-limiting embodiments of the latter, as well as examining the figures, diagrammatical and partial, of the annexed drawing, wherein:
In all of these figures, identical references can designate identical or similar elements.
In addition, the various portions shown in the figures are not necessarily shown according to a uniform scale, in order to render the figures more legible.
Note that in the embodiments described hereinafter, the powders P considered are actinide powders that allow for the manufacture of pellets of nuclear fuel.
In addition, the cryogenic fluid considered here is liquefied nitrogen. However, the invention is not limited to these choices.
In reference to
According to this principle, the device 1 comprises a number n of mixing chambers E1, . . . , En of the powders P, arranged successively in series one after the other according to the same vertical direction in such a way that the powders can circulate through the mixing chambers E1, . . . , En under the effect of the force of gravity. Moreover, the device 1 comprises a number n−1 of systems for restricting the passage R1, . . . , Rn−1 of the powders P, with each system for restricting the passage R1, . . . , Rn−1 being located between two successive mixing chambers E1, . . . , En, in order to constrain the distribution of powders P from one mixing chamber E1, . . . , En to the next. Examples of such systems for restricting the passage R1, . . . , Rn−1 are shown in what follows in reference in particular to
In addition, the device 1 also comprises two chambers A1 and A2 for supplying powders P, provided in particular for distributing powders of different types.
The two chambers A1 and A2 for supplying powders P allows for the introduction of the powders P into the first mixing chamber E1 in contact with the cryogenic fluid FC of the first chamber E1. Then the powders P successively pass through the systems for restricting the passage R1, . . . , Rn−1 and the mixing chambers E2, . . . , En, with each mixing chamber comprising a cryogenic fluid FC.
In addition, each mixing chamber E1, . . . , En comprises means for agitation 2 allowing for the mixing of powders P placed in suspension in the cryogenic fluid FC. Examples of such means of agitation 2 are provided in what follows in reference in particular to
The two chamber for supplying A1 and A2 comprise for example hoppers with adjustable supply, using for example an endless screw, and/or systems of the metering type, in particular vibrating plates or tunnels.
Furthermore, advantageously, the device 1 further comprises an electrostatic charge system C+, C− of the powders P introduced into the mixing chambers E1, . . . , En.
In particular, the portion of the powders P contained in the first chamber for supplying A1 is put into contact with the positive portion C+ of the electrostatic charge system in order to be positively electrostatically charged, while the portion of the powders P contained in the second chamber for supplying A2 is put into contact with the negative portion C− of the electrostatic charge system in order to be negatively electrostatically charged.
In this way, it is possible to allow for a differentiated local agglomeration, in other words prevent self-agglomeration. As shown in
The invention as such makes use of various technical effects that make it possible in particular to achieve the desired level of homogenisation, such as those described hereinafter:
In reference now to
In each one of these two examples, the device 1 comprises, in addition to the elements described hereinabove in reference to
These mobile mixing facilities 2a can comprise mobile grinding facilities. These mobile mixing facilities 2a can further comprise blades, mobile facilities with a duvet effect, turbines and/or blades, with these types of mobile facilities being respectively shown in the
Moreover, in each one of these two examples, the device 1 further comprises second means of agitation 2b in the form of means for generating ultrasonic vibrations comprising sonotrodes 2b.
In addition, the two embodiments shown in the
As such, in the embodiment of
In the embodiment of
In these two examples, the systems for restricting the passage R1, . . . , Rn−1 have a section of passage that can be adjusted and as such arranged in such a way that their sections of passage are ranked from the largest to the finest in the descending direction of the flow of powders P. Advantageously also, the sections of passage of these systems for restricting the passage R1, . . . , Rn−1 are less than the section of natural flow of the powders P in order to force the deagglomeration before the passage through these sections.
An example of dimensioning of a device shall now be described 1 in accordance with the invention according to the first embodiment of the invention.
For the dimensioning of the mixing chambers E1, . . . , En, it is necessary to evaluate in particular:
For this, the equation given by the Zwietering correlation can be used, namely:
wherein in particular:
Moreover, the following equations can also be used:
Q
p=0.73·ND3, Qc=2·Qp, tm=3·tc, tc=V/Qc and P=Np·ρ·N3·d5,
wherein in particular:
The table 1 hereinafter as such gives the dimensioning obtained of a device 1 according to the invention in order to obtain 1 kg/h of shred.
The device 1 obtained then has a mixing response shown by the graph of
Advantageously, the putting into series of n mixing chambers E1, . . . , En having a unit volume Vn such that the global volume V of the mixing chambers E1, etc., is such that V=n·Vn.
In this case indeed, the global mixing time t′m is less than the mixing time tm for the volume V. The difference is as great between these mixing times as n is large, as shown by the graph of
Also shown, in reference to
In this example, the device 1 comprises a single mixing chamber E1 and means for mixing MG of this mixing chamber E1 according to a movement of the gyroscopic type.
More precisely, these means of mixing MG are according to a movement of the gyroscopic type, or close to being so, allowing for the rotation of the mixing chamber E1 according to the three axes X1, X2 and X3 of three-dimensional metrology. This type of agitation by gyroscopic movement favours the mixture of powders P when they have high densities compared to the density of the phase of the cryogenic fluid FC located in the mixing chamber E1.
In addition, the mixing chamber E1 comprises means for agitation 2a, for example in the form of turbines.
The effectiveness of the mixture that can be achieved through this invention can be characterised by the homogeneity of the granular medium obtained after mixing. As such,
More precisely,
It is then observed, despite a short mixing time (30 s) of the aforementioned powders and implemented in an equimassic manner (equal proportion in mass of the two powders), good homogeneity of the granular medium after mixing, as shown in
Of course, the invention is not limited to the embodiments that have just been described. Various modifications can be made thereto by those skilled in the art.
| Number | Date | Country | Kind |
|---|---|---|---|
| 15 60570 | Nov 2015 | FR | national |
| Filing Document | Filing Date | Country | Kind |
|---|---|---|---|
| PCT/EP2016/076506 | 11/3/2016 | WO | 00 |
