WO2014134666A1 - Procédé et dispositif de séparation de mélanges - Google Patents

Procédé et dispositif de séparation de mélanges Download PDF

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Publication number
WO2014134666A1
WO2014134666A1 PCT/AU2014/000202 AU2014000202W WO2014134666A1 WO 2014134666 A1 WO2014134666 A1 WO 2014134666A1 AU 2014000202 W AU2014000202 W AU 2014000202W WO 2014134666 A1 WO2014134666 A1 WO 2014134666A1
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Prior art keywords
separation
porous
mixture
medium
particles
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PCT/AU2014/000202
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English (en)
Inventor
Gang Zheng
William S. Price
Scott A WILLIS
Gary R. DENNIS
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University Of Western Sydney
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Priority claimed from AU2013900772A external-priority patent/AU2013900772A0/en
Application filed by University Of Western Sydney filed Critical University Of Western Sydney
Publication of WO2014134666A1 publication Critical patent/WO2014134666A1/fr

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    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D69/00—Semi-permeable membranes for separation processes or apparatus characterised by their form, structure or properties; Manufacturing processes specially adapted therefor
    • B01D69/02—Semi-permeable membranes for separation processes or apparatus characterised by their form, structure or properties; Manufacturing processes specially adapted therefor characterised by their properties
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D61/00—Processes of separation using semi-permeable membranes, e.g. dialysis, osmosis or ultrafiltration; Apparatus, accessories or auxiliary operations specially adapted therefor
    • B01D61/42—Electrodialysis; Electro-osmosis ; Electro-ultrafiltration; Membrane capacitive deionization
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D2323/00—Details relating to membrane preparation
    • B01D2323/30—Cross-linking
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D2325/00—Details relating to properties of membranes
    • B01D2325/06—Surface irregularities
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D2325/00—Details relating to properties of membranes
    • B01D2325/08—Patterned membranes

Definitions

  • the present invention relates to methods and apparatus for separation of molecules, ions, colloids and/or particles and in particular to methods and apparatus for separation of nano-scale molecules, ions, colloids and/or particles.
  • the invention has been developed primarily for use as method and apparatus for separation of nano-scale molecules, ions and/or particles for in-line particle separation applications and will be described hereinafter with reference to this application. However, it will be appreciated that the invention is not limited to this particular field of use (e.g., such a device could also be a method & apparatus for the concentration of nano-scale molecules, ions, colloids and/or particles).
  • FIGS 1A and 1B depict the typical prior art approaches to particle separation i.e., membrane separation/filtration ( Figure 1A) or column separation ( Figure 1B).
  • Membrane filtration/separation ( Figure 1A) uses a membrane 101 to selectively allow some of the molecules in the mixture 105 to pass through 104. Membranes can become clogged unless pre-filtration is used and the separation of small molecules requires high pressures/energy (e.g., as in desalination processes). This can be used for batch or continuous flow separations.
  • Ratchet-type separation methods are known and the general operation of a ratchet type continuous flow separation device is shown in Figure 1C.
  • Figure 1C (i) there is flow through a tube but no separation of components of the mixture, but in Figure 1C (ii), an array of obstacles 111 combined with diffusion or flow lanes may be used to separate molecules in a mixture 105 at an angle to the flow as they are forced through the obstacle array 111.
  • the obstacle array 111 there is separation of the constituents of the mixture at an angle to the flow.
  • This technique is continuous and typically requires less energy for the separation.
  • current ratchet-type devices are limited by lithography techniques which are prohibitively expensive and limited as to the obstacle size that can be fabricated. This means that with the obstacle dimensions available in current devices, ratchet-type separation methods are only suitable for large molecules (e.g. DNA) and suspensions.
  • ratchet type separation mechanism that is cheap, fast, easily implemented 'in-line' to existing production processes requiring particle separation and may be easily scalable to suit separations of components where the sizes may range from metal ions up to large particles.
  • nano-materials are used to achieve the new ratchet mechanism, removing the limitations of lithography (and similar methods) which are expensive and prevent current ratchet type devices separating small molecules/ions.
  • the separation medium of the ratchet separation apparatus disclosed herein is expected to be significantly cheaper and far easier to make compared to lithography methods.
  • the ratchet apparatus disclosed herein enables continuous flow separation of small molecules, ions or particles and has potential for applications such as speciation analysis or quality control monitoring where oxidation species are important (e.g., mining waste waters, electroplating industries, pharmaceutical industries, medical industries, and environmental analyses among many other applications).
  • a ratchet-type separation apparatus may comprise at least one inlet port.
  • the at least one input port may be adapted for receiving a mixture comprising at least two constituents of different sizes or having different diffusive properties.
  • the apparatus may further comprise a porous or phase-separated medium.
  • the porous or phase separated medium may be adapted for spatial separation of the at least two constituents.
  • the apparatus may further comprise at least two outlet ports. Each of the outlet ports may be adapted to output one of said spatially separated constituents. In particular arrangements, the outlet ports may output at least a portion of one or more of the constituents in the mixture.
  • Each of the constituents in the mixture may be output from the apparatus through one or more of the outlet ports.
  • the spatially separated constituents may be output from the apparatus through a plurality of the outlet ports, wherein each constituent is output according to a distribution across the plurality of outlet ports.
  • Each of the outlet ports may be adapted to output a portion of one or more of the mixture constituents.
  • the portion of each of the mixture constituents which is output from a selected outlet port may be determined by a distribution.
  • the distribution of the mixture constituents at the outlet ports may be determined by either or both of the size or the diffusive properties of the mixture constituents.
  • the porous or phase-separated medium may comprises a cross-linked polymerised liquid crystal material or liquid crystal templated material.
  • a ratchet-type separation apparatus comprising: at least one inlet port adapted for receiving a mixture comprising at least two constituents of different sizes; a porous or phase-separated medium adapted for spatial separation of the at least two constituents; and at least two outlet ports, each port adapted to output one of the at least two spatially separated constituents; wherein, the porous or phase-separated medium may comprises a cross-linked polymerised liquid crystal material or liquid crystal templated material.
  • the cross-linked polymerised liquid crystal material or liquid crystal templated material may be a cross-linked polymerised hexagonal phase material.
  • the separation apparatus may be a continuous flow separation apparatus.
  • the separation apparatus may be a continuous flow batch-process separation apparatus.
  • the separation apparatus may be a continuous flow particle concentrator (i.e. if the sample is added to the entire top of the array then the particles will be concentrated at one side of the apparatus).
  • the porous or phase-separated separation medium may be a bulk lyotropic liquid crystal medium.
  • the apparatus may further comprise means of providing a driving force to the mixture to generate movement of the mixture through the separation medium.
  • the apparatus may further comprise at least two electrodes adapted to provide a driving force in the form of an electrophoretic driving force to said mixture thereby to generate drift of the mixture through the separation medium.
  • the driving force may alternatively be hydrostatic pressure or gravity depending on the particular appraatus configuration.
  • the porous or phase-separated medium may be formed from a polymerisable surfactant/lyotropic liquid crystal (LLC) monomer.
  • LLC polymerisable surfactant/lyotropic liquid crystal
  • a method of separating at least two constituents from a mixture may comprise the step of providing an inlet port adapted to accept said mixture comprising said at least two constituents.
  • the method may comprise the further step of providing a porous or phase-separated separation medium located downstream from said inlet port.
  • the method may comprise the further step of providing a driving force to generate drift of the mixture, the mixture being received at the inlet port, through the porous or phase-separated separation medium.
  • the method may comprise the further step of providing at least two outlet ports located downstream of the porous separation medium. Each of the at least two outlet ports may be adapted to output at least a portion of the one or more of spatially separated constituents of the mixture.
  • the method may comprise the further step of inputting the mixture to the inlet port.
  • the method may comprise the further step of providing a downstream driving force to the mixture such that the mixture is propelled with the driving force through the porous or phase-separated separation medium.
  • Each of the constituents of the mixture may experience unique drift substantially perpendicular (or at some other angle between 0° and 90°) to the direction of flow of the mixture constituents through the separation medium such that on exiting the porous separation medium, the at least two constituents of different sizes are at least partially spatially separated.
  • the method may further comprise the step of outputting each of the at least partially spatially separated mixture constituents substantially through one or more of said at least two outlet ports.
  • a method of separating at least two constituents from a mixture comprising: providing an inlet port adapted to accept said mixture comprising said at least two constituents; providing a porous or phase- separated separation medium located downstream from said inlet port; providing a downstream driving force to the mixture such that the mixture is propelled with the driving force through the porous or phase-separated separation medium; providing at least two outlet ports located downstream of the porous separation medium, each of said at least two outlet ports being adapted to output at least a portion of the one or more of spatially separated constituent of the mixture; inputting the mixture to said inlet port; providing a downstream driving force to the mixture such that the mixture is propelled with the driving force through the porous or phase-separated separation medium; whereby said each constituent of different size and/or diffusive properties comprised in the mixture experiences unique drift perpendicular (or at
  • the porous or phase-separated separation medium may comprise a polymerised hexagonal phase material.
  • the at least partially separated constituents may exit through a plurality of the outlet ports. Each constituent may output according to a distribution across the plurality of outlet ports.
  • the porous separation medium may comprise hexagonally ordered, cylindrical nanopores/nanorods.
  • the porous separation medium may comprise a cross-linked polymerised hexagonal phase material.
  • the porous separation medium may be a bulk lyotropic liquid crystal medium.
  • the driving force may comprise an electrophoretic force provided by at least two electrodes respectively located upstream and downstream with respect to the porous separation medium.
  • the ratchet-type separation apparatus may be adapted for concentrating particles of one size, and accordingly would comprise one inlet and one outlet port designed to concentrate particles that enter the device less frequently (i.e. a low concentration suspension or simply a less frequent addition of particles to the entry - both are essentially just a lower entry frequency).
  • Figures 1A, 1 B & 1 C are schematic depictions of prior art separation methods
  • Figure 2 is a schematic of the operating methodology of a proposed ratchet- type separation apparatus based on a hexagonal phase as disclosed herein;
  • Figure 3A is a schematic depiction of a ratchet-type separation apparatus based on a hexagonal phase as dislcosed herein;
  • Figure 3B is a depiction of a porous or phase-separated separation medium of the ratchet-type separation apparatus based on a hexagonal phase of Figure 3A;
  • Figure 4 is an exploded schematic depiction of the ratchet-type separation apparatus of Figure 3A;
  • Figures 5A and 5B depict the operating principle of the ratchet-type separation apparatus of Figure 3A operating in separation mode;
  • Figure 6 is a depiction of the analytical solution from a simple approach of the dependence of the centre of the distribution, x c , and its width, w, at the exit of the array, on the flow angle, SFIOW, for a distance travelled in the flow direction, arrangement, flow rate and for two particle sizes, for the ratchet-type separation apparatus as disclosed herein;
  • Figure 7 is a depiction of the approximate analytical solution from a simple approach of the dependence of the optimum flow angle for maximum shift, 6>FI 0 W, on the ratio of the particle radius to the cylinder radius for the ratchet-type separation apparatus as disclosed herein;
  • Figure 8 is a depiction of the analytical solution from a simple approach of the dependence of the centre of the distribution, x c , and its width, w, at the exit of the array on the flow rate, v, for a distance travelled in the flow direction, arrangement and particle size, for the ratchet-type separation apparatus as disclosed herein;
  • Figure 9 is a depiction of the analytical solution from a simple approach of the dependence of the centre of the distribution, x c , and its width, w, at the exit of the array on the hexagonal lattice parameter, aHe*, for a distance travelled in the flow direction, arrangement, flow rate and particle size, for the ratchet-type separation apparatus as disclosed herein;
  • Figure 10 is a depiction of the analytical solution from a simple approach of the dependence of the centre of the distribution, x c , and its width, w, at the exit of the array on the cylinder radius, Rc y i, for a distance travelled in the flow direction, arrangement, flow rate and particle size, for the ratchet-type separation apparatus as disclosed herein;
  • Figure 13 is a prediction from the analytical solutions from a simple approach of the separation capability of Pb 2+ , Fe 2+ , Fe 3+ and Al 3+ ions for the ratchet-type apparatus disclosed herein;
  • Figure 14 show photographs of a 3D-printed scaled-up version of a ratchet- type separation apparatus depicting the operating principle as disclosed herein;
  • Figure 15 shows photographs of a 3D-printed scaled-up version of a ratchet- type separation apparatus as in Figure 14 but disassembled to show the components;
  • Figure 16 shows photographs of the technical aspects relating to a 3D-printed scaled-up version of a ratchet-type separation apparatus as in Figure 14 and Figure 15 and corresponding schematics highlighting parameters describing the array of cylinders (i.e., the cylinder radius, Rc y i, the hexagonal lattice parameter, aHex, and the array orientation, and the collection chamber (i.e., bin separation and number);
  • Figure 17 shows photographs of the size and shape of the two beads used to test the separation using the 3D-printed scaled-up version of a ratchet-type separation apparatus as in Figures 14, 15 and 16;
  • Figure 18 shows photographs of the entry chute diameters of the model of Figure 14 with and without an entry chute size modifier in place in the 3D-printed scaled-up version of a ratchet-type separation apparatus as in Figure 14;
  • Figure 19 shows a histogram of the results and fitted Gaussian curves for the separation of beads in Figure 17 when passed through a 3D-printed scaled-up version of a ratchet-type separation apparatus as in Figure 14 without the entry chute modifier in Figure 18;
  • Figure 20 shows a prediction of the results in Figure 19 with modified simple models (i.e., for bin number and position with respect to the entry point) showing the need for further modification of the simple models for the scaled-up version of the ratchet-type separation apparatus as disclosed herein;
  • Figure 21 shows a histogram of the results and fitted Gaussian curves for the separation of beads in Figure 17 when passed through a 3D-printed scaled-up version of a ratchet-type separation apparatus as in Figure 14 with and without the entry chute modifier in Figure 18 in place for the smaller of the two beads;
  • Figure 22 shows a prediction of the results in Figure 21 with modified simple models (i.e., for bin number and position with respect to the entry point) and correction to the injection width for particle size showing the need for further modification of the simple models or calibration using empirical parameters for the scaled-up version of the ratchet-type separation apparatus as disclosed herein; and
  • Figure 23 shows a histogram of the results and fitted Gaussian and reflected Gaussian curves for the 'reverse' entry chute showing no shift and no separation of beads in Figure 17 when passed through a 3D-printed scaled-up version of a ratchet- type separation apparatus as in Figure 14 with and without the entry chute modifier in Figure 18 in place for the smaller of the two beads.
  • real-time for example “displaying real-time data,” refers to the display of the data without intentional delay, given the processing limitations of the system and the time required to accurately measure the data.
  • a new ratchet type separation mechanism has been developed as presently disclosed herein with the use of nano-materials (in a particular example arrangement, lyotropic liquid crystal polymers/templated materials using lyotropic liquid crystals are described or other suitable 'bottom-up' approach) to employ this new ratchet separation mechanism for the separation of small molecules/ions which has significant implications for the industrial separation procedures & applications.
  • Current types of ratchets e.g., geometric (2D) Brownian ratchets and Deterministic (microfluidic) ratchets
  • the area of lyotropic liquid crystals membranes is also a very active research area.
  • the new ratchet mechanism disclosed herein seems to fall in between geometric (2D) Brownian ratchets and Deterministic (microfluidic) ratchets and allows the proposed materials to be used for this purpose.
  • the aligned hexagonal phase which ideally consists of a hexagonal lattice of circular cylinders is employed.
  • such systems typically comprise features that are roughly circular, however hexagonal phases are commonly described as comprising a hexagonal lattice of circular cylinders.
  • the flow of the mixture containing disparate constituents (i.e. molecules/particles/etc) to be separated is set at an angle to the cylinder alignment of the apparatus which results in the molecule/ions being shifted by the cylinder tilt and hence separated from the mixture.
  • the separation technique disclosed herein can be used to separate: very small ions such as, for example, hydrated metal ions; and different oxidation states of the same ion (i.e. speciation).
  • very small ions such as, for example, hydrated metal ions
  • different oxidation states of the same ion i.e. speciation
  • the main advantage of this method over others is the simplicity and continuous flow nature while other small ion separation techniques are batch processes.
  • This has applications as a continuous flow separation/monitoring device suitable for use in industries such as mining, electroplating, environmental monitoring (e.g., waste water), pharmaceutical etc.
  • the separation mechanism employed in the currently disclosed ratchet apparatus is readily scalable to be applicable for separation of larger (e.g.
  • the feature size and spacing of the cylinders can typically be manipulated during fabrication of the separation medium by use of different lyotropic liquid crystal constituent molecules or mixtures of different constituent molecules.
  • the dimensions of the features within the separation medium are dependent on the surfactant type and hydrophilic/solvophilic and hydrophobic/solvophobic lengths of the constituent molecules.
  • surfactants for example that vary from one to the next by increasing the length of the hydrophobic/solvophobic and/or hydrophilic/solvophilic region which would increase the size of the cylinders and/or change the cylinder spacing.
  • different surfactants may require different amounts of solvent to make the phase structure which would change the dimensions in the phase.
  • the size of the bulk separation material may be scaled depending on the sample alignment technique used for fabrication of the material. For example, if the constituent molecules and phase are readily alignable with magnetic fields then it could be that the array size is easily made to be large (i.e., the cylinder radius and spacings are still the same but the size of the final bulk material is large and contains more cylinders).
  • the size of the individual features (e.g. cylinders) in the separation medium may also be scaled depending upon the available surfactants, polymers etc that have suitable characteristics for formation of the requisite liquid crystal phases/phase separated regions in the material and it can be appreciated that other phases with anisotropy but not necessarily consisting of cylinders may also be utilised (e.g. lamellar phases).
  • lithographic techniques e.g., using a top-down approach
  • ratchet type continuous flow separation devices e.g., geometric (2D) Brownian ratchets and Deterministic (microfluidic) ratchets
  • the feature size and depth expected from current micro- fabrication techniques is typically ⁇ >50 - 100 nm (smaller feature sizes may be achieved for example, with soft lithography techniques or more specialised techniques) but the results suffer from deformation problems and the fabrication techniques are typically either slow, or are surface-only methods or are capable of only producing shallow obstacle arrays.
  • ratchet-type separation devices to the separation of large particles/molecules such as, for example, DNA, polymer spheres, suspensions etc, where the constituents to be separated are typically in the sub-micron to micron size range.
  • An additional problem for these type of analysis/separation devices is the depth of the obstacles because, for shallow arrays, there are sample concentration limitations (i.e.
  • Geometric Brownian ratchets require a mechanism comprising ideal obstacle shapes, sizes or orientations. Also, Deterministic (microfluidic) ratchet separation devices in bulk material require specific lattice orientations.
  • Previous LLC membranes have been based on the hexagonal phase (inverse - where the cylinders are pores and so the separation occurs because the pores limit which molecules in the mixture can go through) and also on a bicontinuous cubic phase which is isotropic and so the pores are channels in a specific path for the bicontinuous cubic structure.
  • the main difference here is that the membranes use the size exclusion based on the pore size to effect separation.
  • the NanoRatchet apparatus as disclosed herein differs in two aspects here: it is typically going to be bulk materials not thin membranes and it is the anisotropy of the hexagonal (or other) phase which is utilised to effect separation.
  • Drug delivery with LLC phases typically the interest is in the phases for slow drug release.
  • NanoRatchet apparatus exploits the anisotropy to effect separation using bulk macroscopically aligned LLC phase materials and the separation mechanism using the anisotropy is something different.
  • an especially preferred poiymerisable molecule may comprise a lyotropic liquid crystal (LLC) monomer.
  • Lyotropic liquid crystal (LLC) monomers are amphiphilic molecules containing one or more hydrophobic/solvophobic regions/tails and one or more hydrophilic/solvophilic regions/headgroups. The amphiphilic character of these molecules encourages them to self-organize into aggregate structures, with the boundary of the hydrophobic/solvophobic regions and the hydrophilic/solvophilic regions defining the interface of phase-separated domains.
  • These aggregates may be relatively simple individual structures such as micelles and vesicles or highly ordered yet fluid condensed assemblies with specific nanometer-scale geometries known collectively as LLC phases.
  • LLC phases are well-suited for the production of nanostructured organic materials. Their architectures may incorporate hydrophobic/solvophobic and hydrophilic/solvophilic (or charged) compounds in separate domains with well-defined nano-scale geometries, and may be especially attractive for the production of nanostructured materials, with only the caveat that LLC phases are inherently fluid and therefore lack the robustness required for most materials applications.
  • the present invention may use polymerisable LLC surfactants to form nanoporous polymers.
  • Polymerisable surfactants may comprise molecules having a pair of hydrophobic/solvophobic and hydrophilic/solvophilic components together with one or more polymerisable groups in their structure. These polymerisable surfactants may be used to form surfactant phases to produce useful materials with highly regular nano- scale architectural features (i.e. pores, cylinders etc.).
  • the surfactant molecules can be single molecular weight molecules, distributions of molecular weights, or mixtures comprising members of the general families of surfactants (anionic, cationic, no-ionic, and zwitterionic).
  • An example could be non- ionic surfactants like polyethylene glycol monoalkyl ethers but including a polymerisable group such as a diene moiety.
  • ratchet-type continuous flow separation devices If these nano-structured materials are to be used as ratchet-type continuous flow separation devices a new type of ratchet mechanism has to be developed.
  • Known geometric Brownian ratchets use an array of obstacles with asymmetry with respect to the flow direction, and the molecules are separated through different shifting probabilities. This is related to the diffusion coefficient of the particles, where those with a higher diffusion coefficient (small particles) are shifted more than those with lower diffusion coefficients (large particles).
  • known Deterministic ratchets use an array of obstacles of specific arrangement and the molecules are separated into different flow lanes by being 'bumped' from one flow lane to the next by the obstacle.
  • the two types of known ratchet mechanisms mentioned above are concerned with a 2D arrangement, whereas the NanoRatchet disclosed herein is concerned with a 3D arrangement; the NanoRatchet disclosed herein has obstacles arranged so there is some asymmetry with respect to at least one axis or the flow direction but could be symmetric from with respect to other axes; simulations of the separation medium of the Nanoratchet disclosed herein suggest that particles of different sizes are separated with the larger particles shifting the most because of the greater anisotropy experienced by those larger particles.
  • phase structure which would be suitable for separation purposes would be the lamellar phase.
  • the lamellar could be tilted with respect to the flow direction so that the highest diffusion direction is at an angle to the flow.
  • the transport in the direction of the flow would be enabled through defects present in the phase structure (i.e., porous lamellar sheets) or via the presence of micro-domain boundaries.
  • a mesh phase (perforated lamellar phase) liquid crystal material could also be useful (but this is an intermediate phase so it may be hard to find a surfactant that displays a large region of mesh phase).
  • Another alternative is an inverted hexagonal phase whereby the mixture flows down the inside of the cylinders instead of around them and where the defects (such as bridges between the cylinders) and micro-domain/crystallite sizes could allow transport along the flow direction.
  • FIG. 2 A schematic of the operating methodology of a proposed ratchet-type separation apparatus (an example arrangement of which is as seen in Figure 3A) referred to herein as the NanoRatchet, is shown in Figure 2.
  • the particular arrangement of the NanoRatchet device disclosed herein takes advantage of the anisotropic properties of aligned hexagonal phases in lyotropic liquid crystals, however it will be appreciated that suitable polymerisable surfactant could be used as discussed above.
  • the hexagonal lattice arrangement of the present porous (or phase-separated) material used for the NanoRatchet device comprises a lattice of cylinders 201 aligned along the z axis 206 with flow v at an angle to the cylinder axes (i.e. 203 is defined as the angle the flow makes with the y axis 204 in the -z plane).
  • the hexagonal lattice is characterised by the hexagonal lattice parameter, aHox 205.
  • the cylinders are circular with radius Rc y i 207.
  • the spacing between the cylinders limits the particle radius (actually in some of the example simulations the particle radius, Rpsmae 209, was approximately 1/3 of the cylinder radius, 3 ⁇ 4 y i 207, but this depended on the cylinder spacing).
  • the cylinders could be small and comparable to the particle radii and so the anisotropy might not be as great but still large enough over a large array size to still provide sufficient separation ability for the device to be useful. So, in general the particle radius, Rps Me 209, is limited to less than a maximum of (aHex -
  • Point 214 is the reference position if no shift at an angle FIOW to the flow occurs during the flow time and 216 is the shifted position.
  • the shift relative to the flow line, ds m 215, is positive if z > z and > yena.
  • the x-y plane is perpendicular to the cylinder axes.
  • the lines, L 217 and L> 218 are perpendicular to the flow direction, and cross the start and end points, respectively; and the line L OW 204 denotes the direction along which flow occurs.
  • the array orientation ( ⁇ TM ⁇ 221) is the angle of rotation of the hexagonal lattice 202 in the x plane and is between 0° and 30° for the simulations because of symmetry.
  • the hexagonal lattice has symmetry that means the only angles that are important for purposes of simulation of the flow characteristics of the NanoRatchet device are those between 0 and 30 degrees. In practise, the actual rotation angle of the hexagonal lattice 202 (i.e.
  • the lattice of this kind of separation device might not necessarily be required to be hexagonal and other lattice types might also be used, for example square, rectangular lattice types may be developed with suitable surfactants or for scaled up devices.
  • aligned hexagonal phase materials shows promise for continuous flow separation/concentration of small molecules because of their nm characteristic dimensions (i.e. cyl inder radius and hexagonal lattice parameter) and essentially unlimited bulk dimensions (i.e. the alignment can readily be made to occur over macroscopic dimension materials and exhibits anisotropy despite any microscopic crystal sizes/defects that make up the bul k material).
  • FIG. 2 there is depicted a stylised conceptual model of the separation method according to the present disclosure where the porous or phase- separated medium is made using polymerised lyotropic liquid crystal hexagonal phases (or polymers/silicon arrays in gels/gels templated using them).
  • the hexagonal lattice 202 is characterised by the hexagonal lattice parameter, 205.
  • the cylinders 201 are circular with radius Rc ⁇ 207.
  • the particle radius, RpartMe, 209 is simply added to the cylinder radius 207 for the simulation calculations discussed below.
  • the distance travelled in the flow direction 211 from the start point 213 zstan) is dv.
  • Reference co-ordinate zi3 ⁇ 4f) is the reference position if no shift at an angle to the flow occurs during the flow time and is the shifted position.
  • the shift relative to the flow line 204 is cfshm 215 and is positive if and
  • the xy plane is perpendicular to the cylinder axes which is aligned along the z-axis 206.
  • the lines, L ⁇ 217 and Li 218, are perpendicular to the flow direction 211 and cross the start and end points, respectively; and the line 204 is the line along which flow occurs.
  • the array orientation 221 is the angle of rotation of the lattice 223 in the x-y plane with respect to the 0° array 202.
  • 221 is maintained between 0° and 30° for the numerical simulations because of symmetry.
  • 221 may range between 0° and 360° however, due to symmetry of the hexagonal lattice, all algles can be simulated simply by considering angle between 0° and 30°.
  • NanoRatchet device 300 util ising the separation method described in Figure 2 is depicted in Figures 3A and 3B.
  • the device arrangement 300 shown in Figure 3A is particularly suited to be used as a continuous-flow-device for continuous quality control/monitoring, speciation analysis, pre-concentration, etc, or other molecular or particulate separation application.
  • the NanoRatchet device may vary slightly as would be appreciated by the skilled addressee e.g. for the pre-concentration mode, the device would have a modified input channel so that the sample covers the entire top of the array.
  • Figure 3B depicts the main component of the separation apparatus 300, the separation region 350 formed by a porous or phase-separated medium.
  • the limitations on the dimensions of the separation medium which may be used in the NanoRatchet device will typically be dependent on factors such as, for example, the specific particles the device is designed to separate and the flow rate of the particles through the separation medium are required to be known in order to select the width and height of the array (i.e., to be able to achieve sufficient separation in accordance with requirements).
  • the depth of the array is an important consideration: i.e. the larger the array depth, the more sample that can be added to the top of the device.
  • the porous/phase-separated separation medium is shown in the present example (as seen in Figure 3) as an aligned polymerised lyotropic bulk liquid crystal material 350 with hexagonal phases or, alternately, templated polymers/gels/silicon arrays of cyl inders 351 embedded in gels using them (where the slanted cylinders 351 - i.e. cylinders 201 of Figure 2 - are the ratchet obstacles).
  • the alignment of the slanted cylinders 351 is oriented so that cylinders 351 are at an angle to the flow of mixture through the separation medium 350 (the optimal angle for separation is easily found using the theories developed below complemented with random walk simulation results).
  • a key feature of separation medium 350 is the size of the obstacles i.e. cylinders 351 , their spacing and final array dimensions compared to what is currently available with micro-fabrication/lithography techniques.
  • the obstacles and the spacings of separation medium 350 are in the low nm range and the width, depth and height of the final array is easily made to any size within practical fabrication constraints, for example, the array dimensions (length, width and depth) can be made quite large with a magnetic field alignment procedure for aligning the phase structure of the medium during fabrication - but note that while the cyl inder alignment, for example, over the entire array is along one axis, the bulk material still has numerous micro-domains (crystallites) that have individual hexagonal lattice orientations and defects are likely present across the final material too (but all of these are only likely to average or have l imited effect on the results or aid the results for other phase structures). Other alignment methods could be useful as well as would be appreciated by the ski lled addressee.
  • Figure 5A depicts one possible implementation 300 of the NanoRatchet using a polymerised lyotropic liquid crystal material separation medium 350 utilising electrophoresis as a driving force to push an input mixture 360 admitted through an inlet port (i.e. inlet ports 301a or 301 b) of device 300 and through the separation medium 350 to one of a plurality of outlet ports 305 in a 'lab-on-a-chip' format.
  • an inlet port i.e. inlet ports 301a or 301 b
  • NanoRatchet device 300 is readily scalable for separation of molecular or particulate mixtures comprising constituents of varied size then it is foreseeable that flow in an array on a larger scale (i.e., not using lyotropic liquid crystal materials) with greater permeability could be generated via hydraulic or hydrostatic pressure or gravity as an alternate driving mechanism for the device 300.
  • Figure 4 depicts an exploded view of the concept model of the NanoRatchet separation device 300 of Figure 3A and using a polymerised lyotropic liquid crystal material with hexagonal phases (or polymers/silicon arrays in gels/gels templated using them) as the separation medium 350.
  • the most likely method for flow generation is electrophoretic based on the permeability of membranes made from lyotropic liquid crystal materials but for scaled up forms of this type of ratchet and further developed materials the flow could be generated via a hydraul ic or hydrostatic pressure or gravity as well as would be appreciated by the skilled addressee.
  • NanoRatchet arrangement 300 including multiple inlet channels 301a and 301 b; and a plurality of possible outlet ports 305; separation medium / obstacle array 350; electrodes 307a and 307b to provide the electrophoretic drivi ng force; optional porous supports 311a and 311 , optional inlet 309a and outlet 309b ports for an optional buffer chamber located underneath the buffer ports ; and a microfabricated channel system portion 315 with barriers 313a and 313b between the slots for the electrodes and the rest of the channel system.
  • the purpose of the sample input channel having an inlet 301a and an outlet 301 b is so that the device can be used in 'continuous flow' monitoring applications where only a small amount of sample is required so the device 300 can be placed 'inline' with a process.
  • the purpose of the buffer chamber is to allow the electric field (in this particular arrangement where electrophoresis is used as the driving force) to be across the entire separation channel where the sample inlet is only on the top corner of the obstacle array for separation mode.
  • the buffer chamber has an inlet 309a and outlet 309b so that the buffer can be refreshed easily if required while retaining the conti nuous operation.
  • the multiple outlet channels 305 are a requirement due to the continuous flow separation operation because they allow for the different sample fractions, separated laterally, to be collected or taken to the next process or detector individually and free from the other fractions.
  • the purpose of the multiple outlet channels 305 having an inlet 305a and outlet 305b is so the sample can be removed from the outlet chambers with buffer flushes and so that the device can be used in 'pre-concentration' type applications (or if the sample needs to be concentrated before analysis) where the sample is not removed from the outlet channel until a sufficient amount is collected.
  • porous supports 311a and 311 b at the top and the bottom of the separation medium 350, and barriers 313a and 313b between the electrodes 307a and 307b and the buffer/sample solutions to prevent electrolysis.
  • the microfabricated channel system 315 could have small or large inputs with numerous or few outputs depending on requirements, and that the chamber for the separation medium/obstacle matrix 350 could have any dimensions depending on the requirements of particular applications.
  • the separation medium 350 could be made of several blocks of arrays of different characteristic sizes stacked i n the flow direction to modify the separation characteristics as the molecules/ions/particles are forced through the arrays (this is similar to particular applications of geometric (2D) Brownian ratchets and Determi nistic (microfluidic) ratchets), however, the smallest characteristic gap size cannot be smaller than the largest molecule/ion/particle.
  • Figures 5A and 5B depict the operating principle of the NanoRatchet device 300 (of Figures 3 and 4) operating in separation mode (although the separation mode operates similarly to other operating modes including pre-concentration or continuous monitoring etc).
  • a mixture 360 comprising two molecular or particulate constituents 361 and 363 of different size, enters the device 300 at inlet port 301a where it is forced through the separation medium 350 such that the constituents 361 and 363 are separated based on anisotropic diffusion and array dimensions of the separation medium 350, and two separate (or at least partially separate) particle distributions exit the array through exit ports 365 and 366 for collection, analysis or transport for use in a downstream process.
  • Figure 5B depicts a schematic of the nature of the continuous flow separation in the NanoRatchet device 300.
  • a narrow particle/molecule distribution 371 of the input mixture 360 is forced through the array of the separation medium 350 where the obstruction and anisotropy of the medium 350 result in the particles/molecules of different sizes shifting off the flow/drift line to different extents resulting in separation at the exit of the array between the differently sized molecular components 361 and 363 of the input mixture 360.
  • the NanoRatchet device 300 can operate in different modes, much the same as other types of ratchets, for example, geometric (2D) Brownian ratchets and Deterministic (microfluidic) ratchets. Two common modes are 'separation' and 'concentration'. [ 0088 ] In 'separation mode' there is continuous flow separation of molecular or particulate constituents of a mixture whereby the mixture is injected into the array at one of the top corners, and the molecules/particles/ions are separated as they flow through the array of the separation medium and exit at different locations on the bottom edge or side of the array.
  • the 'separation mode' requires a small injection width, as with most separation technologies, to ensure the best resolution.
  • Small structures/channels with dimensions of the ⁇ range can be made using currently known methods.
  • an input channel for a NanoRatchet separation device such as device 300 discussed above made using polymerised lyotropic liquid crystal hexagonal phases (or polymers/silicon arrays in gels/gels templated using them) can easily be made to have a small width (e.g., it is not unreasonable to assume an initial width of ⁇ 100 ⁇ , even ⁇ 50 ⁇ ) minimising the effect of the initial distribution width.
  • the width, w, of the particle distribution at the bottom edge/exit of the array can be described by: w(D d v , v, a 0 , e FLow ,
  • D ⁇ is the diffusion (in units of m 2 s -1 ) parallel to the cylinder axes (and already including the reduction due to the matrix);
  • dv is the distance (in units of m) travelled i n the flow direction if there is no shift and depends on the flow rate, v (m s ') and the time taken, t (in units of s);
  • ⁇ is the standard deviation due to the injection port width corrected for the particle radius (in units of m)
  • ⁇ , ⁇ is the standard deviation from the injection port (may be taken as 1/2 the injection port width in the direction of the separation)
  • ⁇ is the angle of the flow in the y-z plane with respect to the y-axis (rad)
  • frtex which is the obstruction factor describing the obstruction to diffusion by the cylinders and depends on the hexagonal lattice parameter, an (in units of m); the particle radius, (in units of m), and the cylinder radius, Rc ⁇ (in units of m).
  • the width could be reduced to lots of SHH by dividing the result by 3 ⁇ « ⁇ .
  • the above equation can also be written in terms of the diffusion coefficient of the solute at infinite dilution, Do (in units of m 2 s -1 ), provided a model for the obstruction factor from the matrix surrounding the cylinders, f atrix, e. ., the polymer chains (for a separating medium made from polymerised lyotropic liquid crystal phases or for cylinders templated into polymer gels) which may also include a correction that represents additional averaging due to binding events, is known.
  • This equation could be improved and scaled up versions of the apparatus and method may requi re modifications to this equation to account for other effects (such as for example bouncing, no diffusion etc) which are observed at larger scales.
  • the predicted output for the simulations and analytical models can be visualised using a normalised Gaussian function (i.e., normalised to the number of particles) and could be normalised to an ⁇ .
  • Figure 11 depicts the results of random walk simulations for a NanoRatchet device 300 compared to the analytically derived expressions for the centre of the distribution, c in lots of aHex (i.e., normalised to the hexagonal lattice parameter, anex), and the width of the distribution, w in lots of anex.
  • aHex i.e., normalised to the hexagonal lattice parameter, anex
  • Line 1102 (with square points 1101) and line 1104 (with circular points 1103) are the predictions from the analytically derived equations for Xc in lots of anex and w in lots of anex , respectively, where the solid l ines represent the predictions from numerical modelling and the points are simulation results.
  • Figure 12 depicts the results of random walk simulations for a NanoRatchet device 300 compared to the analytically derived expressions for the centre of the distribution, x c in lots of anex (i.e., normalised to the hexagonal lattice parameter, aHex), and the width of the distribution, w in lots of 3 ⁇ 4.
  • #/ ⁇ / ⁇ / € are the results of random walk simulations for x c in lots of aHex and w in lots of respectively and the different symbols represent different step sizes used.
  • Line 1202 (with square points 1201) and l ine 1204 (with circular points 1203) are the predictions from the analytically derived equations for c in lots of aHe and w in lots of ate, respectively, where the solid lines represent the predictions from numerical modelling and the points are simulation results.
  • 401 is the predicted result for the Pb 2+ alone
  • 402 is the predicted result for the Fe 2i alone
  • 403 is the predicted result for the Fe 3+ alone
  • 404 is the predicted result for the Al 3+ alone and is the combined result as would be expected for the separation from the Nanoratchet device 300. Note that these model predictions still include several assumptions and the appearance could improve with better models.
  • a 3D printer (Model: uPrint SE Plus, Stratasys Inc.) was used to produce a working model made from acrylonitrile butadiene styrene (ABS) plastic and is shown in Figures 14 to 16.
  • the stereolithography (.stl) file was generated from 3D models drawn in Google Sketchup 8 (free version; Trimble Sketchup v. 8.0.15158), and were converted to the toolpath (printer head path) file using CatalystEX v. 4.3 (Dimension, Stratasys Inc.).
  • the stated layer resolution was 0.254 mm.
  • the total print time was on the order about 50 h, and the time for the solvent wash bath (to remove the support material) was simi lar to this.
  • the separation chamber (i.e., the cylinder array) was 14.4 * 3.5 ⁇ 15 cm (i.e., dv - 15 cm) and the arrangement of the cylinders was such that when upright it had a (9 - 50°, 6 ray - 20° (i.e., when measured from the cylinder i n the centre of a hexagon and in the xy plane, there is a cylinder 10° from the y axis and 20° from the x axis; see Figure 16), Rc was 2.5 mm and was 1 1 mm. This means that the maximum radius of particles that could be separated was 3 mm.
  • Figure 14 depicts a photograph of a 3D-printed scaled-up NanoRatchet 1400 (i.e., a MacroRatchet).
  • Vertical arrow 1401 in Figure 14A indicates the direction of the flow (i.e., the particles fall through the device under gravitational force).
  • Vertical arrow 1401 as shown is pointing down the 'normal' entry chute that is at the top corner of the cyl inders in the separation chamber whereby the cylinders are tilted from top left to bottom right in the images.
  • Horizontal red arrow 1403 in Figure 14(A) and 14(B) indicate the direction of separation (for this arrangement, and with the bins in the collection chamber ( Figure14(B)(i)) horizontal).
  • FIG 14(B) Also shown in Figure 14(B) is an example of the output for 40 particles (beads) with 1.97 mm average radius, after falling down the 'normal' entry chute marked in (A) with the vertical arrow 1401 into the collection chamber ( Figure 14(B)(i)).
  • Line 1405 in Figure14(B) is a depiction of a Gaussian curve that is used to describe the output particle distribution.
  • the second entry point (i.e., the 'reverse' entry chute) on the top right corner in Figure 14 was 3D printed for a test to confirm that there was no shift if the particles are input via this entry. Note that this 3D printed scaled up Nano atchet is only one possible arrangement and size.
  • Figures 15(A) to (F) show a series of photographs of this example MacroRatchet device 1400 of Figure 14 depicting details of the components of the 3D printed scaled NanoRatchet 1400.
  • Figure 15(A) shows the assembled NanoRatchet example device 1400 with the chute lids 1409 taken off.
  • Figure 15(B)(i) shows a view into device 1400 from the base of the separation chamber. Collection bin dividers are visible in the collection chamber ( Figure 15(B)(ii)), and in the base of the separation chamber casing at the bottom of the cylinders ( Figure 15(B)(i)).
  • the separation chamber containing the tilted cylinders can be removed from the separation chamber casing ( Figure 15(C)).
  • Figures 15(D) to 15(F) show the removed separation chamber (i.e., the array of tilted cylinders 1411 in a hexagonal lattice, for this example). Locator mark 1501 marks the same corner of the separation chamber.
  • FIG. 16B Details of the collection bins are shown in Figure 16B. There was a distance of 7 mm between the centre of the bin dividers (or the centre of the bins) and the bin dividers were 2 mm thick, giving a collection bin width of 5 mm for the particles to enter a bin. That is, the bins integrate regions of 7 mm at a time. It should be noted that the last bin only had a 4 mm width for the particles to enter this bin because of the dimensions to the device (i.e., this is the left over space available for the length of the array printed - so from the centre of the last bin divider to the wall is 5 mm).
  • Figure 16(A)(i) is a photograph of the 3D printed separation chamber (i.e., the array of tilted cylinders 1411 in a hexagonal lattice, for this example) viewed from the bottom and down the cylinder axes. Note that in the photo the cylinders 1411 appear to shift slightly off the hexagon and their diameter seems to change but this is due to perspective.
  • the 3D printed separation chamber i.e., the array of tilted cylinders 1411 in a hexagonal lattice, for this example
  • Figure 16 (A)(ii) A schematic showing the values for some parameters
  • the y-axis shown matches the y-axis in Figure 2 and that if the x-axis was reversed in the schematic, the same goes for the x-axis in the Figure 2, the resulting would still be 20° (i.e., not 40°) since ranges from 0° to 30° because of symmetry.
  • Figure 16 (B) depicts the collection chamber 1407 with bins 1408 suited to hold particles up to 5 mm diameter - except the last bin (shaded) which is only suitable for 4 mm particles.
  • the bin dividers (the vertical lines within the large rectangle shown in Figure 16(B)(ii) and as also seen in the separation chamber in Figure 15(B)(i)) are 2 mm thick, the vertical lines at the end of the rectangle shown in Figure 16 ⁇ B)(ii) can also be considered as 2 mm thick, with the vertical lines in Figure 16(B)(ii) representing the centre of the bin dividers. Note that the entry point is approximately above the bin divider for the end of bin 1 and corresponds to ⁇ 0 cm shift. Bin 21 is shaded grey to highlight that this bin is 1 mm smaller than the others due to the number of bins and the width of the array 3D printed (which was limited by the 3D print envelope volume).
  • the particle radii used for the predictions were the average radii based on the particle/bead shape as they were not spherical (see Figure 17(B)).
  • the reasoning for this was as follows: the variation of the particle radius due to the shape of the particles/beads (i.e., a spherical segment; capped spheres; spheres with a flat top and bottom) may have resulted in an averaged shift (e.g., c. Fit) other than predicted using the average radius and the simple theory, but because of the tumbling of the particle it may be represented adequately by the average radius from consideration of the shape.
  • an averaged shift e.g., c. Fit
  • the average radius was calculated by using the average radius for the spherical section (i.e., average of the value found for a few beads) and the angular dependence of the average distance from the centre of the capped sphere to the plane at the top or bottom (i.e., angular average of the particle radius).
  • the average radius for the large particles was 1.97 mm and for the small particles this was 0.92 mm.
  • the height of the modified entry chute was 9 mm (with a 1 mm lip at the top) and the outer diameter of the insert was about 5.5 mm (to ensure that it fitted in the larger entry port easily) and the outer diameter of the lip at the top of the cylinder was about 6.5 mm.
  • This entry chute modifier was used to measure the results for 800 of the smaller particles input via the 'normal' entry chute and 40 smaller particles input via the 'reverse' entry chute for comparison to the results obtained for the larger entry chute.
  • Figure 18 shows a series of photographs of the entry chute width modifier 1801 (shown in Figure 18(C)) to test the effect on the width of the resulting distribution at the exit for the smaller particles in the 3D printed scaled NanoRatchet or 'MacroRatchet' (the chute modifier was also 3D printed and fits inside the entry chutes to reduce the entry point diameter.
  • Figure 18(A) shows the entry chute that is suitable for both large and small particles tested (having a radius of about 3 mm) and
  • Figure 18(B) shows the entry chute reduced to a radius of about 1.05 mm to reduce the standard deviation of the entry point for the small particles.
  • Figure 19 shows experimental results for the separation of two particles (beads) of different sizes and Gaussian curves fitted to the results.
  • the result for the large particles are given by point 1905 and the corresponding curve-fit 1907, and the results for the small particles are given by points 1901 and curve-fit 1903.
  • the data points i.e., points 1901 and 1905) are experimental data points in this figure.
  • a full Gaussian curve, (N pit /(w Fit [n/2 ) exp (— 2(x - x c ,Fit ⁇ / w t ) > w 'th Npamaes 800 (i.e., peak area; total number of particles) was fitted to each distribution where Xc.
  • the entry chute radius was 3 mm and was the same for both particles.
  • the vertical grid lines in the figure represent the centres of the bin dividers.
  • Figure 20 shows the expected outcome for a total of 800 of each size particle (bead) predicted using slightly modified equations from the simple analytical models derived.
  • the predicted results shown are the expected Gaussian distribution and corresponding discrete distribution (i.e., histogram) results.
  • the result for the large particles are given by points 2005 (histogram format via integration for each bin of the predicted Gaussian curve) and curve-fit 2007 (predicted Gaussian curve); and the results for the small particles are given by points 2001 and curve-fit 2003.
  • the entry chute radius was 3 mm (i.e., this was taken to be ⁇ and was the same for both particles - but consideration for this showed this is not the correct ao and needed modification).
  • the vertical grid lines in the figure represent the centres of the bin dividers.
  • Figure 21 shows the experimental results highlighting the influence of the particle size on the width of the output distri butions for the separation of two particles (beads) of different sizes and Gaussian curve s fitted to the results.
  • the result for the large particles with entry chute radius of 3 mm are given by points 2101 and the corresponding curve-fit 2103; and the results for the small particles with entry chute radius of 3 mm are given by 2105 and curve-fit 2107 (note that the data points 2105 and 2101 and respective curve-fits 2103 and 2107 are the same as in Figure 19).
  • the results for the smaller particles with the entry chute modifier so that the entry chute radius is 1.05 mm are given by points 2109 and corresponding curve-fit 2111.
  • the vertical grid l ines in the figure represent the centres of the bin dividers.
  • the predicted results shown are the expected Gaussian distribution and the expected discrete (i.e., histogram) results.
  • the result for the large particles are given by points 2201 (histogram format via integration for each bin of the predicted Gaussian curve) and line 2203 (the predicted Gaussian curve) with
  • the separation chamber was turned around in the casing (i.e., so as to align the opposite entry chute with the bin labelled as bin 1 in the collection chamber for comparison to the results with the 'normal' entry chute (i.e., see Figure 19 and Figure 21), and 40 beads of each particle size were put through the device (note that the smaller particles were done twice - once for each size of entry chute).
  • a full Gaussian curve was also fitted for comparison and is shown in Figure 23(B) and the corresponding equation is given by exp[-2(x - 1 ) 2 /w
  • the vertical grid lines in the figure represent the centres of the bin dividers.

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Abstract

La présente invention concerne un dispositif de séparation à cliquet comprenant : au moins un orifice d'entrée conçu pour recevoir un mélange comprenant au moins deux constituants de tailles différentes ; un milieu poreux ou à phases séparées ou des obstacles conçus pour la séparation spatiale des au moins deux constituants ; et au moins deux orifices de sortie (pour la séparation et au moins un orifice de sortie pour des applications de concentration, le(s) constituant(s) à concentrer pénétrant dans le dispositif à travers le ou les orifices d'entrée moins fréquemment et étant concentrés au niveau du ou des orifices de sortie), chaque orifice étant conçu pour produire au moins une partie de l'un desdits au moins deux constituants spatialement séparés du mélange ; ledit milieu poreux ou à phases séparées pouvant comprendre un matériau à base de cristal liquide polymérisé fortement réticulé.
PCT/AU2014/000202 2013-03-06 2014-03-05 Procédé et dispositif de séparation de mélanges WO2014134666A1 (fr)

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Citations (6)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
WO2006087556A1 (fr) * 2005-02-17 2006-08-24 Membrane Extraction Technology Ltd Procédé de séparation
US20060204400A1 (en) * 2004-11-24 2006-09-14 Christoph Blattert Process for separation of dispersions and an apparatus
US20080076143A1 (en) * 2001-10-19 2008-03-27 Protea Biosciences, Inc. Microfluidic system for proteome analysis
AU2007223448B2 (en) * 2006-03-02 2011-10-20 Sei-Ichi Manabe Pore diffusion type flat membrane separating apparatus, flat membrane concentrating apparatus, regenerated cellulose porous membrane for pore diffusion, and method of non-destructive inspection of flat membrane
US20120031833A1 (en) * 2010-07-15 2012-02-09 The Ohio State University Research Foundation Systems, compositions, and methods for fluid purification
AU2011235954B2 (en) * 2006-03-02 2013-06-13 Sei-Ichi Manabe Regenerated cellulose porous membrane

Patent Citations (6)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US20080076143A1 (en) * 2001-10-19 2008-03-27 Protea Biosciences, Inc. Microfluidic system for proteome analysis
US20060204400A1 (en) * 2004-11-24 2006-09-14 Christoph Blattert Process for separation of dispersions and an apparatus
WO2006087556A1 (fr) * 2005-02-17 2006-08-24 Membrane Extraction Technology Ltd Procédé de séparation
AU2007223448B2 (en) * 2006-03-02 2011-10-20 Sei-Ichi Manabe Pore diffusion type flat membrane separating apparatus, flat membrane concentrating apparatus, regenerated cellulose porous membrane for pore diffusion, and method of non-destructive inspection of flat membrane
AU2011235954B2 (en) * 2006-03-02 2013-06-13 Sei-Ichi Manabe Regenerated cellulose porous membrane
US20120031833A1 (en) * 2010-07-15 2012-02-09 The Ohio State University Research Foundation Systems, compositions, and methods for fluid purification

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