• 专利附录
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    • 专利摘要:
    The present invention relates to a device (1) for producing a continuous emulsion of two immiscible fluids, provided with a first microsystem (2) comprising at least two micro-channels (23, 24) for admission of each fluid sections. respective S1 and S2, facing each other along a central axis A of admission and having an ex-centering, at least two microchannels (25, 26) output of said device (1) of the emulsion a formed, and a crossing zone (27) of the inlet and outlet microchannels, capable of generating an interface between the fluids and constituting a pre-emulsion circulating in the output microchannels until the completion emulsion. According to the invention, the device (1) further comprises at least one singularity (31, 32, 33, 34, 35, 36) capable of destabilizing the interfaces between the fluids in the pre-emulsion. The present invention also relates to a method for producing a continuous emulsion of two immiscible liquids implementing the device (1) according to the invention.
    公开号:FR3045404A1
    申请号:FR1562682
    申请日:2015-12-17
    公开日:2017-06-23
    发明作者:Jerome Bellettre；Arab Belkadi；Agnes Montillet
    申请人:Centre National de la Recherche Scientifique CNRS；Universite de Nantes；
    IPC主号:
    专利说明:

    Device and method for producing a continuous emulsion of two immiscible liquids
    The present invention relates to the field of micro-fluidics, and in particular to the field of devices and processes for the continuous emulsification of immiscible fluids, in particular for producing water-in-oil (W / O) type emulsions for immediate use and involving rates compatible with industrial applications.
    More particularly, it is a matter of continuously emulsifying a percentage of essentially aqueous fluid (equal to or less than 20% by volume of the final emulsion formed) in a lipidic fluid (for example a recovery vegetable oil or heavy fuel oil). or an animal fat), to form an emulsion in situ for direct combustion in a boiler, oven, turbine or motor.
    The global problem that the present invention seeks to solve is to propose an emulsification system dedicated in particular to the continuous production of emulsions of two immiscible liquids, and in particular of water-in-oil type emulsions (E / H).
    The applications targeted by the present invention relate to the field of energy conversion, such as turbines, boilers, furnaces or even internal combustion engines in general. Work has shown that the presence of a small fraction of finely emulsified water (droplets of the order of 5 to 10 μm) in the liquid fuel makes it possible to lower the combustion temperature and thus reduce the emissions of gaseous pollutants. and particles resulting from poor combustion. The continuous phase can be of various nature such as conventional diesel, heavy fuel oil or else lipid waste (used vegetable oils, animal fats).
    The constraints associated with the applications envisaged are numerous, whether in terms of the nature of the fluids to be emulsified, the volume ratio of the fluids in the emulsion, or the need to design a compact process that makes it possible to treat the flows required for operation. internal combustion engines. In general, discontinuous devices (for example tanks in discontinuous or "batch" mode) are currently preferred. They are based on the use of suitable agitation mobiles (rotor-stator for example) and are relatively energetic. The stability over time of these emulsions is, in such devices, generally provided by the addition of surfactants. With regard to continuously producing an emulsion, those skilled in the art know different systems operating in continuous mode, such as static mixers (for example those of commercial name SMX SULZER), membranes, high-pressure nozzles, and micro-channels. However, the membranes have the disadvantage of not being able to handle high flow rates (that is to say of the order of a few μΐ / h to a few ml / h). In addition, static mixers do not allow to obtain very fine particle sizes, unless models with very small hydraulic diameters are used.
    Research in the field of microfluidics has been very active for two decades and shows, in particular, an interest in the development of continuous emulsification processes111 '[2]. A large number of studies are known to those skilled in the art which deal with emulsification processes essentially applied to oil-in-water (O / W) mixtures 131 '[4]. This type of dispersion is considered to be less demanding in terms of emulsification energy, because of the use of an aqueous phase (low viscosity) as a continuous phase. Unquestionably, the water-in-oil (W / O) emulsification which is more particularly targeted in the present invention because of the targeted applications requires energy optimization for two main reasons: • a continuous phase whose viscosity represents 50 to 70 times that of water, and • the range of capillary numbers investigated, which is about 1000 times higher than that published in the scientific literature on the subject [1] '[5]' [6] [7].
    As regards more particularly the processes for the continuous emulsification of two immiscible fluids, the devices known to those skilled in the art are micromixers with confined impact jets. A first study focused on the use of impact jets in order to achieve a liquid-liquid dispersion of immiscible fluids [8] '[9]. This work is based on the principle of emulsification by the impact of two sprayed jets (or "sprays" in English). These jets are produced by two injectors arranged facing each other within the same chamber [8] '[9].
    Subsequently, we find the use of impact jets in confined systems based on the use of microchannels with high fluid flow rates [10] '[11].
    The first studies carried out on this subject focused on the mixture of miscible fluids. The results obtained then suggested to those skilled in the art to be interested in the fractionation of immiscible fluids, in this case sunflower oil and water to form water-in-oil (W / O) emulsions. while keeping this configuration of impact jet flows confined in a microchannel [12] '[13].
    Then, on the basis of these first studies, the applicant has realized a microsystem of continuous emulsification device, which is illustrated in FIG. 1. Such an emulsification device 1 comprises a microsystem 2 equipped with two micro-channels. , 24 for the admission of each fluid in the device which face each other along a central inlet axis A, and also of two micro-channels 25, 26 for the exit from the device 1 of the emulsion 1 once formed. The micro-input channels 23, 24 and output 25, 26 having a passage section widened relative to the microchannels of the device of the present invention1141. In a first step, the microchannels of the micro-system illustrated in FIG. 3 have been machined so as to have a square section of 600 μια on one side. Then, in order to reduce the volume fraction of the water (</> e) and to generate a coiled flow (usually called "Swirl") favoring the fractionation of the dispersed phase filaments or drops, the section the water admission channel 23 was reduced to 300 μια by 300 μια, the other channels keeping an inlet section of 600 μm by 600 μια, as illustrated in the lateral perspective representation of the microsystem of FIG. 2 Such a micro-system has outstanding continuous emulsification capabilities. In the output microchannels 25, 26, it is observed, during the formation of the emulsion, that a wound flow structure ("swirl") is formed in the center of the microsystem, in the crossing zone 27 of the microsystem or the micro-input channels 23, 24 and the output channels 25, 26 intersect each other. This wound structure consists of an entanglement of filaments and water droplets surrounded by sunflower oil. In particular, FIGS. 3a and 3b are photographs showing a flow structure of the dispersed phase flowing in the microchannels of the micro-system illustrated in FIGS. 1 and 2. FIGS. 3a and 3b show in particular that this flow structure is complex and has a deformed water-oil interface, that is to say with appearance of irregular shapes on the surface of this winding. The latter is actually animated by a combination of two movements: a rotation movement, as explained in FIG. 3d, superimposed on an advection movement (transport), in the direction simultaneously of the two micro-output channels of the micro-system . In such a flow pattern an increase in the flow rate of the dispersed phase accelerates rotation (increasing centrifugal force) and feeding to the outlets.
    Such a device comprising the micro-system illustrated in FIGS. 1 to 3d makes it possible to produce an emulsion continuously, in which the droplets of the dispersed phase have a mean dispersion diameter (dio) of 10 μm with a continuous phase containing 13% by volume of Butanol and a mean diameter (dio) of 30 μm with a pure continuous phase (sunflower oil) without any additive. In the range of flow rates investigated, the emulsification process implemented with such a device consumes 1% of the lower heating value (LHV) of the liquid fuel produced.
    However, such a device has the disadvantage that the filament formed in the output micro-channel is not sufficiently fractionated, which does not allow its immediate use as fuel in internal combustion engines, turbines, boilers and ovens.
    The purpose of the present invention is therefore to overcome all or part of the disadvantages of the prior art, by placing in the device at least one singularity capable of destabilizing the interfaces between the two liquids and thus further fractioning the filament formed in the output micro-channels.
    More particularly, the subject of the present invention is a device for producing a continuous emulsion of two immiscible fluids, said device comprising: at least one first microsystem (for example
    polymethyl methacrylate, in particular PMMA sold under the trademark PLEXIGLAS®) or metal, and preferably stainless steel or aluminum), said first microsystem comprising: o at least two micro-channels for the admission of each fluid into said device, said microchannels, of respective sections S1 and S2 different from S1, facing each other along a central axis A of admission and having an ex-centering, related to their difference in section, o at least two micrometers; channels for the output of said device from the emulsion once formed, o a crossing zone in which said inlet and outlet microchannels intersect, said crossing zone being able to generate an interface between the fluids, and thus constituting a pre-emulsion for circulating in the micro-outlet channels until completion of the formation of the emulsion; said device being characterized in that it further comprises at least one singularity capable of destabilizing the interfaces between the fluids in the pre-emulsion.
    By immiscible fluids is meant, in the sense of the present invention, a hydrophilic liquid and a hydrophobic liquid.
    As regards the nature of the fluids circulating in the device according to the invention, it is possible in particular to use a hydrophilic (preferably aqueous) fluid and a hydrophobic fluid (preferably a lipid or hydrocarbon fluid).
    For the purposes of the present invention, the term "microsystem" means a system of millimeter or submillimetric dimensions, comprising a cross-section formed by submillimeter-sized channels.
    By micro-channel means, within the meaning of the present invention, submillimeter hydraulic diameter channels, that is to say less than one millimeter.
    In the microsystem of the device according to the invention, at least two intake micro-channels of respective sections S1 and S2 are facing each other along a central axis A of admission and having an ex-centering, linked to their section difference, in a direction different from the central axis of admission. However, these channels are not necessarily arranged symmetrically with respect to this central axis of admission (as illustrated in FIG. 3d). In fact, the intake channels are shifted deep into the microsystem, thus forming a step.
    In addition to the micro-intake channels, the microsystem of the device according to the invention further comprises at least two micro-channels for the output of said device of the emulsion once formed, and a crossing zone in which said micro-channels inlet and outlet channels intersect.
    Advantageously, the micro-output channels may be arranged in the microsystem of the device according to the invention, so as to face each other along a central output axis different from the central axis of admission, and preferably symmetrically, with respect to the central axis of admission. More preferably, the output micro-channels may be arranged perpendicular to the inlet axis facing each other along the central output axis.
    The device according to the invention is characterized in that it furthermore comprises at least one singularity capable of destabilizing the interfaces between the two liquids in the pre-emulsion (or offset impacting jet), these interfaces being created in the crossing zone. of the microsystem and being completed by the singularity (s).
    The crossing zone of the microsystem according to the invention allows the propulsion and the impact of the two fluids to be emulsified at relatively high speeds. From these impacts, a pre-emulsion of the two fluids is created in the crossing zone. This pre-emulsion is in the form of a wound structure, consisting of an entanglement of filaments and droplets of fluid of the dispersed phase surrounded by fluid of the continuous phase. This structure begins to split in the crossing zone, resulting in an emulsion at the outlet of the outlet channels. The fractionation is continued is refined during the passage of the pre-emulsion in the singularity or singularities (especially the elbow or bends). These speeds are of the order of 1 to 3 meters per second, which is well above the fluid velocities usually observed in microchannels.
    The device according to the invention is therefore particularly suitable for emulsifying a low-viscosity fluid circulating in a micro-inlet channel (for example water), in a fluid of much higher viscosity (for example a lipid or hydrocarbon fluid). circulating in a second microchannel intake. In addition, the device according to the invention has the advantage of being compact and offers the possibility of producing continuously and on demand an in-situ emulsion by avoiding the use of surfactant. This is of considerable interest in the case of an emulsion for use as a fuel, since the use of surfactant in a fuel increases the carbon and economic footprint of the process.
    According to a first advantageous embodiment of the device according to the invention, the singularity can be a bend formed in each micro-channel output of the microsystem.
    In this first embodiment, the device according to the invention may comprise two to six elbows formed in each micro-channel output of the microsystem.
    According to a second advantageous embodiment of the device according to the invention, the singularity may be an enlargement or a sudden narrowing formed in each output micro-channel of said microsystem.
    According to a third embodiment of the device according to the invention, the device according to the invention may further comprise a second microsystem in series or in parallel comprising: at least two micro-channels for admission into said device of each fluid , facing each other along a central inlet axis, o at least two micro-channels for the exit of the emulsion formed of said device according to the invention.
    Preferably, in this third embodiment, it is possible to use as a second microsystem a microsystem identical to the first microsystem.
    Advantageously, irrespective of the embodiment of the device according to the invention, the inlet and outlet micro-channels have a square or rectangular section S1, S2 and whose hydraulic diameter can advantageously be between 100 and 800 micrometers.
    The present invention also relates to a method for producing a continuous emulsion of two immiscible liquids implementing the device according to the invention, said method comprising the following steps: 1) the arrival of each fluid in the microchannels admission of said microsystem; - 2) the frontal collision (or jet impactant) of the fluids at the intersection of the micro-channels of admission and exit, so as to generate an interface between the two liquids constituting a pre-emulsion (or filament), - 3) admission of the pre-emulsion in said output channels, - 4) output of the microsystem by said output channels of the finalized emulsion comprising a continuous phase and a dispersed phase, said method being characterized in that the flow rate of the continuous phase is 8.3-10-7 m3 / s at 20.10-7 m3 / s (that is, between 50 and 200 ml / min), and the fluid of the dispersed phase is between 3 and 20% by volume the continuous phase, and in that it further comprises between a step of fractionation of the pre-emulsion between steps 3 and 4, to obtain an emulsion with an average diameter of the drops of the dispersed phase of between 5 and 20 micrometers.
    Advantageously, the fluid of the dispersed phase represents between 5 and 10% by volume of the continuous phase.
    Advantageously, the flow rate of the continuous phase is between 8.3 × 10 -7 m 3 / s and 12 × 10 -7 m 3 / s (that is to say between 50 and 120 ml / min).
    Advantageously, the fluids to be emulsified comprise a hydrophilic fluid, which is preferably an aqueous phase, and a hydrophobic fluid, preferably a lipid or hydrocarbon fluid.
    Preferably, the hydrophilic fluid is a salt-free aqueous phase and the lipid or hydrocarbon fluid is free of surfactant.
    The present invention also relates to the use of the emulsion obtainable by the process according to the invention as a fuel for internal combustion engines, turbines, furnaces and boilers, if the hydrophilic fluid is a salt-free aqueous phase and the lipid or hydrocarbon fluid is free of surfactant.
    Thus, the device and the method according to the invention therefore operate on principles for the emulsification of two immiscible fluids, which are different from those known from the prior art, for the mainly intended application: production of emulsified fuel, especially intended for use in internal combustion engines. Thanks to the device and to the process according to the invention, a better combustion of the fuel is obtained by a microexplosion effect. The microsystems of the device according to the invention combine an impactant jet (frontal collision of the intake fluids intended to be emulsified) generated by the crossing of the microsystem and the intake carnaux shifted in depth (so as to form a step) and the or singularities (eg bends in the output channels). The right length of the channels can be dimensioned in order to minimize the pressure drops in the microsystem. Moreover, the different geometries of the singularities that can be implemented in the device according to the invention serve to promote the flow effects favorable to the fluid / fluid fractionation: in particular, the formation of a winding at the level of the step (offset in the depth between the intake channels) increases the stresses experienced by pre-emulsion. The number and positioning of the singularity (s) in the output micro-channels make it possible to optimize the splitting. Thanks to these different mechanisms, it is possible to produce a continuous emulsion without additives (especially surfactant). Other advantages and features of the present invention will result from the description which follows, given by way of nonlimiting example and with reference to the following examples and the corresponding appended figures: FIG. 1 represents two views of a microsystem device according to the prior art (a side perspective view and a front view); FIG. 2 also represents a side perspective view of the crossing zone of the microsystem illustrated in FIG. 1; FIG. 3a shows a display at a frequency of 10 kHz of a W / O pre-emulsion flowing in a micro-outlet channel of the microsystem illustrated in FIGS. 1 and 2 under the following flow conditions: flow of water in a micro-inlet channel 23 Qe = 9.7 mL / min, and o oil flow in the other micro-inlet channel 24 Qh = 74.0 mL / min; FIG. 3b shows a display at a frequency of 10 kHz of the W / O pre-emulsion flowing in the same micro-channel as that illustrated in FIG. 3, but under different flow conditions: water in a micro-inlet channel 23 Qe = 10.0 mL / min, and o oil flow in the other micro-inlet channel 24 Qh = 59.5 mL / min; FIG. 3c also shows a side perspective view of the crossing zone illustrated in FIG. 1, showing the arrival of water in an intake channel 23 and the arrival of the oil in the other channel; admission 24; FIG. 3d schematically represents the frontal collision (or impacted jet) of water and oil in the crossing zone of the microsystem shown in FIG. 3c; FIG. 4 is a block diagram of an emulsification bench comprising a first example of a device according to the invention, in which each micro-outlet channel 25, 26 of the microsystem 2 comprises a bend 31 (ie two bends per microsystem); FIG. 5 is a block diagram of the crossing zone 27 of the micro-system illustrated in FIG. 4; FIG. 6 is also a schematic diagram of the crossing zone 27 of a microsystem of a second exemplary device according to the invention, in which each micro-outlet channel 25, 26 of the microsystem comprises two elbows (either four elbows per micro-system); FIG. 7 is also a schematic diagram of the crossing zone 27 of a microsystem of a third example of a device according to the invention, in which each micro-outlet channel 25, 26 of the microsystem comprises three elbows ( six elbows per micro-system); FIG. 8 is also a schematic diagram of the crossing zone 27 of a microsystem of a fourth example of a device according to the invention, in which each micro-outlet channel 25, 26 of the microsystem comprises four elbows ( eight elbows per micro-system); FIG. 9 is also a schematic diagram of the crossing zone 27 of a microsystem of a fifth exemplary device according to the invention, in which each micro-outlet channel 25, 26 of the microsystem comprises six elbows ( twelve bends per micro-system); FIG. 10 shows a photograph, at the level of the first and second elbows of an output micro-channel, of a W / O pre-emulsion flowing in a micro-output channel; of the micro-system shown in FIG. 8 (microsystem with eight elbows in total) with the following flow conditions: o flow of water in a micro-inlet channel 23 Qe - 14.9 mL / min, and o oil flow in the other micro-inlet channel 24 Qh = 62.5 mL / min; FIG. 11 represents a photograph, at the level of the second, third and fourth elbows of an output micro-channel, of an W / O pre-emulsion flowing in a micro-output channel of the microsystem illustrated on FIG. Figure 8 (microsystem with eight bends in total) under the same flow conditions as in Figure 10; FIG. 12 represents a photograph, at the level of the first and second elbows, of a W / O pre-emulsion flowing in a micro-outlet channel of the micro-system illustrated in FIG. 9 (micro-system with six elbows per microchannel and 12 elbows in total) with the following flow conditions: o flow of water in one micro-inlet channel 23 Qe = 15.0 mL / min, and o flow of oil in the other micro- intake channel 24 Qh = 62.35 mL / min; FIG. 13 shows a photograph, at the level of the fifth and sixth elbows, of an W / O pre-emulsion flowing in a micro-outlet channel of the microsystem illustrated in FIG. 9 (twelve-elbow microsystem in total) under the same flow conditions as in Figure 12; FIG. 14 represents a photograph, at the level of the fifth and sixth elbows, of a W / O pre-emulsion flowing in a microchannel output from the micro-system illustrated in FIG. 9 (twelve-elbow microsystem) under the same flow conditions as in Figure 12; FIG. 15 is a histogram showing the influence of the flow rate of the dispersed phase and the number of elbows on the mean dio diameter of the droplets in the obtained emulsion.
    Figures 1 to 3d are discussed in the description of the prior art.
    FIG. 4 is a block diagram of an emulsification bench 1 comprising a first example of device 1 according to the invention, in which each micro-outlet channel 25, 26 of the microsystem 2 comprises a bend 31 (ie two elbows). by microsystem 2). In other words, the microsystem 2 of the device according to the invention differs from that illustrated in FIGS. 1 to 3d by the presence of a bend 31 in each output microchannel 25, 26.
    This emulsification bench 1 was developed and used (see example below) to test under the emulsification conditions corresponding to the targeted applications (properties of the fluids and flow rates involved) the microsystems according to the invention as represented in Figures 5 to 14.
    This emulsification bench constitutes a device 1 according to the invention, in which the microsystem 2 consists of two transparent PMMA plates (for example made of PMMA marketed under the trademark PLEXIGLAS®) in order to facilitate optical investigations. The microchannels are etched using a micro-milling cutter on a plate called the base (in the same way as for the microsystem 2 without elbow shown in FIG. 1), the second plate serving solely as a cover.
    The microsystem 2 emulsification bench shown in Figure 4 corresponds to that shown in Figures 5, having two elbows (one at each output microchannel 25, 26). But, the configurations of microsystems according to the invention as shown in Figures 6 and 10 (4 elbows in total), 7 (6 elbows in total), 8, 10 and 11 (8 elbows in total) and 9, and 12 at 14 (12 elbows in total) were also tested. These configurations of microsystems 2 according to the invention represent significantly improved versions of the reference configuration shown in Figures 1 to 3d.
    The emulsification bench 1 of FIG. 4 is furthermore equipped with two dual piston displacement pumps 40, 41 (for example those marketed by ARMEN under the trade designation APF-100). The maximum pressure and the maximum working rate of these pumps 40, 41 are respectively 25 bar and 100 ml / min (maximum flow rate in the case of the use of water). In order to allow an accurate measurement of the flow rate, the bench 1 is equipped with two scales 50, 51 (for example Sartorius® brand scales (model MSE2203) allowing an acquisition of the mass weighed over time whose accuracy is ± 10 ~ 3 g The pressure measurement is carried out by two compact pressure transmitters 60, 61 (for example, sold under the trade name Gems®, model 3100.) The measuring range of the pressure sensor is 0 - 25 bars for an accuracy of ± 0.25% of the full scale These pressure sensors 60, 61 are connected to the water and oil circuit between the pump and the inlet of the micro-channel. , 61 measure the static pressure for each of the two mixed liquids All connections between the pumps and the microchannels are made with Fluoropolymer (FEP) tubes, the dimensions of which are as follows: an inside diameter (ID) 1.55 mm and an outside diameter (OD) 3.125 mm The following example illustrates the invention without limiting its scope.
    EXAMPLE
    The emulsification bench previously described and illustrated in FIG. 4 was used to test, under different flow conditions close to the targeted applications (in terms of the properties of the fluids and the flow rates involved), the microsystems according to the invention such as as shown in Figures 5 to 14, comparing them to the microsystem without bend as shown in Figures 1 to 3d.
    Fluids used
    During these tests, the emulsification bench illustrated in FIG. 4 was emulsified continuously, in accordance with the process according to the invention, an aqueous phase (dispersed phase) and a lipid phase (continuous phase). Water was used as the aqueous phase in a small amount, not exceeding 20% by volume, compared to the sunflower oil which represents the continuous phase and therefore the majority phase. Sunflower oil was chosen to work on the principle of a cold model. The viscosity of this oil, at ambient temperature, corresponds to the temperature of the heavy fuel oil preheated in an engine. The characteristics of the various fluids employed are shown in Table 1 below.
    Table 1
    All the emulsification tests were conducted at a temperature of 25 ° C. Because of the effects of the friction of the fluids, the emulsion at the outlet of the emulsification circuit o experiences a heating of the order of +5 C with respect to the admission temperature.
    For all the tests carried out, the flow rate Qh of oily phase in an intake microchannel was set at approximately 60 ml / min, for three flow rates of water Qe tested (approximately 5 ml / min, 10 ml / min and 15 ml / min). Emulsification results
    The properties of the pre-emulsion formed after the impact (frontal collision) are studied at the intersection of the jet of water and that of sunflower oil in the crossing zone 27 of the microsystem 2 (by visualization at high altitude). frequency of the flow in the output microchannels), as well as by measuring the dio diameter of the droplets formed in the emulsion at the output of the microchannels (histogram shown in FIG. 15).
    High-frequency visualization of flows As flows of two-phase type characterized by high flow rates and implemented in complex geometries, it is not feasible to make numerical simulations.
    High frequency visualizations are therefore an essential means for monitoring the fractionation of fluids in the elbows or bends present in the emulsion channel. The purpose of these visualizations allows to show the privileged places of the fractionation, and also the zones where the coalescence of the droplets can possibly occur.
    FIGS. 10 and 11 illustrate the transformations occurring on the filament in the 4-bend microsystem by micro-outlet channel (eight bends in total), while FIGS. 12 to 14 relate to the micro-channel 6-bend microsystem (FIG. 12 elbows in total: see also figure 9).
    Histogram (Figure 15)
    FIG. 15 is a histogram showing the influence of the flow rate of the dispersed phase and the number of elbows on the average diameter dio of the droplets in the emulsion obtained, obtained by calculating the arithmetic average of the droplet diameters (dio) for the analyzed sample (dio = Σίά ± / η ±).
    This histogram makes it possible to judge the relevance of the addition of one or more additional bends. The letters a, b and c represent the three ranges of flow rates of the dispersed phase. The data show the advantage of putting two elbows in series and causing two impacts within the microsystem (configuration shown in FIG. 6) when a large flow of water is used ("c" range of water flow rate). the order of 15 ml / min). The comparison of the diode average diameters shows that the reference system without a bend is less suitable for the water-in-oil dispersion (see the histogram of FIG. 15).
    The purpose of the elbows is to generate, in addition to the viscous forces whose role is predominant over the fractionation, 515 additional stresses serving to break up the initially formed water filament (see FIGS. 3a and 3b) at the crossing at the time of the impact between the water jet and the jet of oil. The different versions have been designed to experimentally study the effect of a sudden change of direction in one or several successive bends. The configuration comprising two elbows and the one comprising six elbows also include a second impact of the flows at the output of the device. This second impact involves the emulsion flows initially formed at the first impact and refined by their passage through the elbows.
    List of references [1] C.-X. Zhao, A.P.J. Middelberg. "Two-phase microfluidic flows." Chemical Engineering Science 66.7 (2011): 1394-1411.
    [2] H. Schubert, R. Engel. "Product and formulation engineering of emulsions." Chemical Engineering 82: 1137-1143.
    [3] T. Nisisako, T. Hatsuzawa. "A microfluidic cross-flowing emulsion generator for producing biphasic droplets and anisotropically shaped polymer particles." Microfluidics and Nanofluidics 9.2-3 (2009): 427-437.
    [4] N. Kiss, H. Pucher J. Wieser S. Scheler H. Jennewein D. Suzzi J. Khinast, G. Brenn. "Formation of O / W emulsions by static mixers for pharmaceutical applications." Chemical Engineering Science 66: 5084-5094.
    [5] Belkadi, A. Experimental study of liquid-liquid fractionation in micro-channels for the continuous production of emulsified biodiesels. Ph.D. thesis, SPIGA, University of Nantes, France, 2015.
    [6] T. Nisisako, Toshiro Higuchi, Toru Torii. "Droplet training in a microchannel network." Lab on a chip 2.1 (2002b): 24-6.
    [7] T. Nisisako, T. Higuchi, T. Torii. "Training of droplets using branch channels in a microfluidic circuit." Proceedings of the 41st SICE Annual Conference. SICE 2002 .. vol. 2. 2002a, 957-959.
    [8] A. Tamir, S. Sobhi. "A new Two-Impinging-Emulsifying Streams." AIChE Journal 31.12 (1985): 2089-2092.
    [9] Kiljanski, Tomasz. "Preparation of emulsions using impinging streams." AIChE Journal 50: 1636-1639.
    [10] Ait-Mouheb, N. "Experimental and numerical characterization of the flow and transfer of matter in micromixers." Ph.D. thesis, University of Nantes, France, 2010.
    [11] N. Ait Mouheb, C. Solliec J. Havlica P. Legentilman J. Comiti J. Tihon, A. Montillet. "Flow characterization in T-shaped and crossshaped micromixers." Microfluidics and Nanofluidics 10.6 (2010): 1185-1197.
    [12] S. Nedjar, M. Tazerout, A. Montillet. "Continuous synthesis of" water-in-oil "emulsions using micromixers." the French Society of Process Engineering. Poster - 13th Congress of the French Society of Process Engineering, 2011.
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    权利要求:
    Claims (14)
    [1" id="c-fr-0001]
    1) Device (1) for producing a continuous emulsion of two immiscible fluids, comprising: - at least a first microsystem (2) comprising: o at least two micro-channels (23, 24) for the admission of each fluid in said device (1), said micro-channels (23, 24), of respective sections S1 and S2 different from S1, facing each other along a central inlet axis A and having an ex-centering, connected to their difference in section, o at least two micro-channels (25, 26) for the output of said device (1) from the emulsion once formed, o a crossing zone (27) in which said micro-admission channels (23, 24) and output (26, 27) intersect, said crossing zone (27) being able to generate an interface between the fluids and thus constitute a pre-emulsion for circulating in said output microchannels (25, 26) until the completion of the formation of the emulsion; said device (1) being characterized in that it further comprises at least one singularity (31, 32, 33, 34, 35, 36) capable of destabilizing the interfaces between the fluids in the pre-emulsion.
    [0002]
    2) Device (1) according to claim 1, wherein the output microchannels (25, 26) are arranged in said microsystem (2) symmetrically with respect to said central axis of admission (A).
    [0003]
    3) Device (1) according to claims 1 or 2, wherein said singularity (31, 32, 33, 34, 35, 36) is a bend formed in each micro-outlet channel (25, 26) of said microsystem (2 ).
    [0004]
    4) Device (1) according to claim 3, comprising two to six elbows (31, 32, 33, 34, 35, 36) formed in each micro-channel (26, 27) output of said microsystem (2).
    [0005]
    5) Device (1) according to claims 1 or 2, wherein said singularity (31, 32, 33, 34, 35, 36) is a sudden enlargement or narrowing formed in each output micro-channel (25, 26) of said microsystem (2).
    [0006]
    6) Device (1) according to claims 1 or 2, further comprising a second microsystem in series or in parallel comprising: o at least two micro-channels for admission into said device of each fluid, facing each other along the a central inlet axis, o at least two micro-channels for the emulsion outlet formed from said device (1).
    [0007]
    7) Device (1) according to claim 6, wherein said second microsystem is identical to said first microsystem (3).
    [0008]
    8) Device (1) according to any one of the preceding claims, wherein the intake micro-channel (23, 24) and outlet (26, 27) has a section S1, S2 square or rectangular.
    [0009]
    9) Process for producing a continuous emulsion of two immiscible liquids implementing the device (1) as defined in any one of claims 1 to 8, said method comprising the following steps: 1) the arrival of each fluid in the intake microchannels (23, 24) of said microsystem (2), - 2) the frontal collision of said fluids at the intersection (27) of the inlet (23, 24) and outlet micro-channels (25). , 26), so as to generate an interface between the two liquids constituting a pre-emulsion, - 3) the admission of the pre-emulsion in said outlet channels (25, 26), - 4) the output of the microsystem ( 2) by said outlet channels (25, 26) of the finalized emulsion comprising a continuous phase and a dispersed phase, said method being characterized in that the flow rate of the fluid of the continuous phase is between 8.3.10-7 m3 / s at 20.10-7 m3 / s, and the fluid of the dispersed phase represents between 3 and 20% volu of the continuous phase, and in that it further comprises between a step of fractionating the pre-emulsion between steps 3 and 4, to obtain an emulsion with an average diameter of the drops of the dispersed phase of between and 20 microns.
    [10" id="c-fr-0010]
    The method of claim 9, wherein the fluid of the dispersed phase is between 5 and 10% by volume of the continuous phase.
    [11" id="c-fr-0011]
    The process according to claims 9 or 10, wherein the flow rate of continuous phase fluid is from 8.3 × 10 -7 m 3 / s to 12 × 10 -7 m 3 / s (i.e. 120 ml / min).
    [12" id="c-fr-0012]
    12. Process according to any one of claims 9 to 11, in which the fluids to be emulsified comprise: a hydrophilic fluid, preferably an aqueous phase, and a hydrophobic fluid, preferably a lipid or hydrocarbon fluid.
    [13" id="c-fr-0013]
    The method of claim 12, wherein the hydrophilic fluid is a salt-free aqueous phase and the lipid or hydrocarbon fluid is free of surfactant.
    [14" id="c-fr-0014]
    14. Use of the emulsion obtainable by the process as defined in claim 13, as a fuel for internal combustion engines, turbines, furnaces and boilers.
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    同族专利:
    公开号 | 公开日
    US20180369767A1|2018-12-27|
    CN108472604A|2018-08-31|
    JP2019506286A|2019-03-07|
    WO2017103498A1|2017-06-22|
    FR3045404B1|2021-06-11|
    EP3389837A1|2018-10-24|
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    法律状态:
    2016-12-16| PLFP| Fee payment|Year of fee payment: 2 |
    2017-06-23| PLSC| Publication of the preliminary search report|Effective date: 20170623 |
    2017-12-14| PLFP| Fee payment|Year of fee payment: 3 |
    2019-12-30| PLFP| Fee payment|Year of fee payment: 5 |
    2020-12-28| PLFP| Fee payment|Year of fee payment: 6 |
    2021-12-30| PLFP| Fee payment|Year of fee payment: 7 |
    优先权:
    申请号 | 申请日 | 专利标题
    FR1562682A|FR3045404B1|2015-12-17|2015-12-17|DEVICE AND METHOD FOR CARRYING OUT A CONTINUOUS EMULSION OF TWO IMMISCIBLE LIQUIDS|FR1562682A| FR3045404B1|2015-12-17|2015-12-17|DEVICE AND METHOD FOR CARRYING OUT A CONTINUOUS EMULSION OF TWO IMMISCIBLE LIQUIDS|
    PCT/FR2016/053458| WO2017103498A1|2015-12-17|2016-12-15|Device and method for carrying out continuous emulsion of two immiscible liquids|
    JP2018525604A| JP2019506286A|2015-12-17|2016-12-15|Device and method for the continuous emulsion of two immiscible liquids|
    EP16825521.4A| EP3389837A1|2015-12-17|2016-12-15|Device and method for carrying out continuous emulsion of two immiscible liquids|
    CN201680074422.0A| CN108472604A|2015-12-17|2016-12-15|Device and method for the continuous emulsification liquid for implementing two kinds of immiscible liquids|
    US16/063,463| US20180369767A1|2015-12-17|2016-12-15|Device and method for carrying out a continuous emulsion of two immiscible liquids|
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