US20100078382A1 - Continuous collection method of particle component in aqueous solution and apparatus therefor - Google Patents

Continuous collection method of particle component in aqueous solution and apparatus therefor Download PDF

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US20100078382A1
US20100078382A1 US12/570,470 US57047009A US2010078382A1 US 20100078382 A1 US20100078382 A1 US 20100078382A1 US 57047009 A US57047009 A US 57047009A US 2010078382 A1 US2010078382 A1 US 2010078382A1
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liquid
phase
emulsion flow
emulsion
phase separation
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Hirochika Naganawa
Nobuyuki Yanase
Tetsushi Nagano
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Japan Atomic Energy Agency
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Japan Atomic Energy Agency
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Priority claimed from JP2008253778A external-priority patent/JP5733691B2/ja
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Assigned to JAPAN ATOMIC ENERGY AGENCY reassignment JAPAN ATOMIC ENERGY AGENCY ASSIGNMENT OF ASSIGNORS INTEREST (SEE DOCUMENT FOR DETAILS). Assignors: NAGANAWA, HIROCHIKA, NAGANO, TETSUSHI, YANASE, NOBUYUKI
Publication of US20100078382A1 publication Critical patent/US20100078382A1/en
Priority to US13/527,013 priority Critical patent/US9108124B2/en
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    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D11/00—Solvent extraction
    • B01D11/04—Solvent extraction of solutions which are liquid
    • B01D11/0426—Counter-current multistage extraction towers in a vertical or sloping position
    • B01D11/0434—Counter-current multistage extraction towers in a vertical or sloping position comprising rotating mechanisms, e.g. mixers, rotational oscillating motion, mixing pumps
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D11/00—Solvent extraction
    • B01D11/04—Solvent extraction of solutions which are liquid
    • B01D11/0426—Counter-current multistage extraction towers in a vertical or sloping position
    • B01D11/0438—Counter-current multistage extraction towers in a vertical or sloping position comprising vibrating mechanisms, electromagnetic radiations
    • C—CHEMISTRY; METALLURGY
    • C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F1/00—Treatment of water, waste water, or sewage
    • C02F1/26—Treatment of water, waste water, or sewage by extraction
    • C—CHEMISTRY; METALLURGY
    • C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F1/00—Treatment of water, waste water, or sewage
    • C02F1/001—Processes for the treatment of water whereby the filtration technique is of importance
    • C—CHEMISTRY; METALLURGY
    • C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F1/00—Treatment of water, waste water, or sewage
    • C02F1/52—Treatment of water, waste water, or sewage by flocculation or precipitation of suspended impurities
    • C02F1/54—Treatment of water, waste water, or sewage by flocculation or precipitation of suspended impurities using organic material

Definitions

  • the present invention relates to a method for collecting continuously particle component in the aqueous solution without using filters and/or centrifuge separators.
  • the method utilizes a phenomenon that particle component in the aqueous solution aggregates at the liquid-to-liquid interface between the aqueous solution (aqueous phase) containing the particle component as the target component and the solvent (solvent phase) having hydrophobic nature and not mixing with water.
  • Liquid-liquid extraction method by which the target component included in the aqueous solution may be extracted into the solvent (such as organic solvent) that contains extraction agents (extractants) having hydrophobic nature and does not mix with water, is widely used in various industrial fields such as metal refinement, nuclear fuel reprocessing, removal of harmful ingredients in the waste water, recycling by separation and recovering of commercially valuable materials.
  • solvent such as organic solvent
  • extracts extracts having hydrophobic nature and does not mix with water
  • extracting the component in the aqueous solution other than liquid-liquid extraction method there is another method designed “liquid-to-solid extraction method” which uses solid materials such as resin to be filled into the column and the like structure.
  • Liquid-liquid extraction method which is often regarded as not so simple as the column-type liquid-to-solid extraction method, is better than the liquid-solid extraction method in terms of extraction capacity and speed of extraction process.
  • the material transport from one liquid to the other liquid is made reach an equilibrium state by keeping the emulsion state (the state in which the water and the organic solvent are well mixed and formed in emulsion) with continuous stirring and vibration (shaking) operations.
  • mixer-settler extractors using stirring machines come into wide use.
  • relatively newly developed continuous liquid-liquid extraction apparatus such pulsed column using vibration due to pulse generation in order to disperse liquid drops, and centrifugal extractor for phase separation by using centrifugal forces (refer to JP 09-085120 A) are used in nuclear industries.
  • centrifugal extractors are expected to be applied to the reprocessing technology of spent nuclear fuels because they are excellent in the efficiency of the phase contact and the phase separation of the two liquid phases, and are compact in size.
  • the above mentioned apparatuses have the common principle for mixing two liquid phases by applying mechanical external forces (such as stirring and vibrating) continuously or intermittently, which may lead to such disadvantageous aspects as being not easy to handle, increased running cost, increased maintenance cost, increased apparatus manufacturing cost (initial cost), uncertain safety features. More specifically, they include: 1) large energy load required to generate mechanical external forces; 2) load and stress at the driving parts for generating mechanical external forces; 3) long adjusting work required to prepare and setup the operation of apparatus; 4) risk of ignition due to friction or static electricity at the driving parts; 5) high strength and high price materials required to manufacture the driving parts; 6) ambient noises in connection with stirring, vibrating and high-speed rotating operations; and 7) uncertainty in ensuring safety during earthquake.
  • mechanical external forces such as stirring and vibrating
  • uncertain safety features More specifically, they include: 1) large energy load required to generate mechanical external forces; 2) load and stress at the driving parts for generating mechanical external forces; 3) long adjusting work required to prepare and setup the operation of apparatus; 4) risk of ignition due to friction or static electricity
  • Emersion flow technology is such an innovative method that enables liquid-liquid extraction (solvent extraction) in a simplified manner similar to column-type liquid-to-solid extraction method which uses solid materials such as resin to be filled into the column.
  • the extraction apparatus using emulsion flow has also advantageous features in the column-type liquid-solid extraction apparatus (being easy to handle and low running cost) in addition to the advantageous features in the conventional solvent extraction apparatus, such as mixer-settler extractor (large extraction volume and rapid extraction process).
  • the column-type liquid-solid extraction apparatus As large extraction capacity and rapid extraction process cannot be realized by the column-type liquid-solid extraction apparatus, and easiness to handle and low running cost cannot be realized by the conventional solvent extraction apparatus, it is very significant to enable to establish the co-existence of those advantageous features.
  • emulsion flow technology is an innovative method as described above, it has some unresolved problems.
  • it is difficult to generate fine-grained and high quality emulsion flow, and it is not easy to obtain the extraction rate (extractability) over 90% because some amount of non-uniformity occurs.
  • extractability extraction rate
  • the single current method as it is difficult to maintain stable emulsion flow in the wide region, there is a problem in scale-up of the apparatus.
  • the holes at the head part from which the aqueous solution is spouted out are often plugged due to the particle component, which is a critical weak point.
  • An object of the present invention is to provide a method for collecting particle component in the aqueous solution without using filters and/or centrifuge separators.
  • the method utilizes a phenomenon that particle component in the aqueous solution aggregates at the liquid-to-liquid interface.
  • Another object of the present invention is to provide a method for collecting the particle component suspended in the aqueous solution as well as for extracting and collecting the dissolved component (for example, metallic ions) by solvent (liquid-liquid extraction).
  • a further object of the present invention is to provide a counter-current type emulsion flow continuous liquid-liquid extraction apparatus allowing to: 1) obtain the extraction rate (extractability) over 90% by generating high quality emulsion flow; 2) facilitate scale-up of the apparatus by maintaining stable emulsion flow in the wide region; 3) prevent the particle component in the aqueous solution from plugging holes in the head part.
  • One aspect of the continuous collection method for the particle component in the aqueous solution according to the present invention is to collect continuously the particle component in the aqueous solution without using filters but with utilizing a phenomenon that the particle component aggregates at the liquid-to-liquid interface between the aqueous solution (aqueous phase) containing the target suspended particle component and the solvent (solvent phase) having hydrophobic nature and not mixing with water.
  • Another aspect of the continuous collection method for the particle component in the aqueous solution according to the present invention is to collect both the particle component and the dissolved component in the aqueous phase at the same time by using both an aggregation phenomenon that the particle component in the aqueous phase aggregates at the liquid-to-liquid interface and a liquid-liquid extraction phenomenon that the dissolved component in the aqueous phase is extracted into the solvent phase through the liquid-to-liquid interface.
  • an organic ligand designated as an “extraction agent (extractant)” may be added to the solvent.
  • One aspect of the counter-current type emulsion flow continuous liquid-liquid extraction apparatus comprises the first head part for spouting the aqueous phase, the second head part for spouting the extracting solvent phase, said the second head part arranged in the opposite position to the first head part, the column part where the emulsion flow generates, the upper phase separation part installed at the upper side of the column part and the lower phase separation part installed at the lower side of the column part, and further comprises the fluid supply pump.
  • the apparatus can be operated in stably without any effect by the particle component. This is realized by using such a characteristic that the particle component in the aqueous solution is never distributed into the extracting solvent. Thus, upon making the extracting solvent phase fine-grained, there is no need for paying attention to the plugging problem in the head part (the second head part).
  • the structure of the second head part influences the quality of emulsion flow, and that the structure of the first head part spouting the aqueous phase is not dominant. This means that, even if the first head part may not have a structure in which the particle component cannot pass sufficiently through the head part (the structure in which the aqueous phase may not be fine-grained), there is no significant effect on the extractability.
  • the invention of the emulsion flow has been completed according to those new findings.
  • the apparatus according to the present invention in comparison with the conventional apparatus based on the continuous centrifugal separation method, may provide larger processing capacity and reduced levels of running cost, initial cost and maintenance cost as well as the size of the apparatus itself is compact.
  • the apparatus according to the present invention is expected to be used in plants in various industrial fields.
  • the method according to the present invention may provide such a significant effect not found in the conventional methods that the dissolved component as well as the particle component can be simultaneously collected, as necessary, being combined with the liquid-liquid extraction method.
  • the target component can be extracted with higher extractability, and also that the scale-up of the apparatus can be facilitated, all of which cannot be attained by the emulsion flow apparatus based on the single current method.
  • the plugging problem in the head part due to the particle component such as suspension materials which is recognized as the critical weak point of the emulsion flow apparatus based on the single current method, is solved.
  • FIG. 1A , FIG. 1B and FIG. 1C are illustrations representing the phenomenon that aluminum oxide Al 2 O 3 particles aggregate at the liquid-to-liquid interface.
  • FIG. 2A and FIG. 2B are schematic diagrams illustrating an example of the emulsion flow apparatus implementing the continuous collection method for the particle component in the solution according to the present invention.
  • FIG. 3A is an overall configuration showing a small-sized experimental setup for the emulsion flow apparatus shown in FIG. 2
  • FIG. 3B is an enlarged view of a part of the apparatus.
  • FIG. 4A is an overall configuration showing an intermediate-sized experimental setup for the emulsion flow apparatus shown in FIG. 2
  • FIG. 4B is an enlarged view of a part of the apparatus.
  • FIG. 5 is a photo picture showing the state of aluminum oxide Al 2 O 3 particles deposited at the column part in the experimental setup for the emulsion flow apparatus shown in FIG. 2 .
  • FIG. 6 is a graph showing the result of continuous extraction of ytterbium Yb (III) from the aqueous nitric acid solution.
  • FIG. 7 is a graph showing the result of continuous extraction of ytterbium Yb (III) in the coexistence of the particle component (Al 2 O 3 ).
  • FIG. 8 is a graph showing the result of extracting uranium U from the waste solution simulating the decontamination waste solution in highly selective manner by the counter-current type emulsion flow apparatus.
  • FIG. 1 illustrates an example of the phenomenon that the particle component aggregates at the liquid-to-liquid interface to be interpreted as the basic principle of the present invention.
  • FIG. 2 illustrates an example of the embodiment apparatus for implementing the continuous collection method of the particle component in the aqueous solution according to the present invention.
  • FIG. 1A , FIG. 1B and FIG. 1C Suspended aqueous solution including large amount of iron oxide Fe 2 O 3 was prepared as the particle component in the test tube (refer to FIG. 1A ), and then isooctane was added gently into the test tube (refer to FIG. 1B ), and then the test tube was shaken by hand for ten seconds, and then the test tube was allowed to stand for 1 minute (refer to FIG. 1C ).
  • iron oxide Fe 2 O 3 aggregated at the liquid-to-liquid interface and the suspended aqueous solution was purified.
  • the aggregation of the particle component at the liquid-to-liquid interface may be promoted by generating the emulsion state by mixing the aqueous phase and the solvent phase.
  • the emulsion flow apparatus 10 illustrated in FIG. 2A is composed of the apparatus body, being composed of the first head part 11 for spouting the aqueous phase, the second head part 12 for spouting the solvent phase, the column part 13 in which emulsion flow is formed, and the phase separation parts placed at the upper and lower sides of the column part (upper phase separation part 14 and lower phase separation part 15 ), and the liquid supply pump 16 (a single duplex pump or a couple of simple pumps).
  • the head parts are not necessarily required to contact the liquid phase (aqueous phase, solvent phase or emulsion mixed phase).
  • the water sample in the reservoir 20 is supplied through the conduit tube 21 to the emulsion flow apparatus 10 .
  • the first head part 11 has either one of the following structures;
  • the operation of the apparatus in FIG. 2A will be described below.
  • the liquid supply pump 16 placed at the conduit tube 21 connecting the emulsion flow apparatus 10 to the reservoir 20 for the water sample containing the particle component and, the aqueous solution supplied from the reservoir 20 is made spouted into the organic solvent through the tube provided as the first head part 11 of the emulsion flow apparatus 10 .
  • the liquid droplets so formed by fine-graining the solvent phase are made spouted through the pipe provided as the second head part 12 of the apparatus from the opposite direction to the flow direction of the aqueous solution.
  • emulsion flow a flow composed of the aqueous phase and the solvent phase formed as emulsion mixed phase
  • emulsion flow a flow composed of the aqueous phase and the solvent phase formed as emulsion mixed phase.
  • emulsion flow a flow composed of the aqueous phase and the solvent phase formed as emulsion mixed phase
  • the emulsion mixed phase reaches the phase separation parts 14 and 15 of the emulsion flow apparatus 10 , the state of emulsion disappears and then the aqueous phase and the solvent phase are separated from each other.
  • the solvent phase is localized at the upper phase separation part 14
  • the aqueous phase is localized at the lower phase separation part 15 .
  • the clean solvent phase in the upper phase separation part 14 is circulated through the second head part 12 .
  • the clean aqueous phase in the lower phase separation part 15 is drained as drainage water after processing.
  • head parts 11 and 12 may not be necessarily shaped in a circular cylinder, but may be shaped in a square cylinder.
  • the column part 13 and the phase separation parts 14 and 15 may not be necessarily shaped in a circular columned form, but may be shaped, for example, in a square columned form.
  • the particle component 31 in the aqueous solution (refer to FIG. 2B ) will be deposited on the inner wall of the column part 13 in connection to the emulsion flow generation at the column part 13 .
  • the particle component 31 deposited on the inner wall of the column part can be collected, for example, by using a piston 30 as shown in FIG. 2B .
  • the small-sized and intermediate-sized emulsion flow apparatuses (both having the height of 70 cm) as shown in FIG. 3 and FIG. 4 , respectively, were fabricated, and the experiments were carried out for collecting only a particle component and for collecting simultaneously both a particle component and a dissolved component, and then the performance of the apparatus was evaluated.
  • the experimental results were compared with those in the conventional method (continuous centrifugal separation method).
  • Aluminum oxide Al 2 O 3 particles classified in the range from 20 ⁇ m to 25 ⁇ m in particle diameter are used as the particle component and ytterbium Yb (trivalent ion) was used as the dissolved component. Note that the present invention is not limited to those specific embodiments.
  • the aluminum oxide Al 2 O 3 particles provided with a uniform diameter by classification were used, and the ratio of the weight of collected particles to the weight of initially added particles (collection ratio) was estimated by collecting the residual particles in the aqueous solution after processing and measuring their weight.
  • classification ratio the ratio of the weight of collected particles to the weight of initially added particles
  • Aluminum oxide Al 2 O 3 particles that were not collected by the apparatus but remained in the aqueous solution were measured by filter method.
  • Polycarbonate filter (with 0.2 ⁇ m mesh), which does not change in weight even in contacting to water, was used.
  • FIG. 3A shows a photo picture of the small-sized emulsion flow apparatus used in the experiment.
  • the first head part 11 used in the apparatus has such a structure that the side wall of the hollow cylinder with its one end being closed, being made of polypropylene, is and being provided with 10 holes having 1 mm diameter.
  • the second head part 12 has such a structure that a sintered glass plate having pores with 40 ⁇ m diameter bonded onto the end of the hollow cylinder as described above.
  • the upper phase separation part 14 has such a structure that a vessel having a narrow mouth inserted at the upper side of the column part 13 (refer to FIG. 3B )).
  • the lower phase separation part 15 connected to the lower part of the column part 13 has such a structure that a vessel with a diameter larger than the diameter of the column part 13 .
  • the overall processing time was 60 minutes (with processing capacity of 20 litters per hour) to collect almost 100% (99.5% or higher: note that the digits after the decimal point were not reliable due to the measurement error) of aluminum oxide Al 2 O 3 particles.
  • FIG. 4A shows an intermediate-sized emulsion flow apparatus.
  • the term of “Intermediate-sized” apparatus means an apparatus having an apparatus volume three times larger than the apparatus volume used in Embodiment 1.
  • the first head part 11 used in the apparatus has such a structure that the side wall of the hollow cylinder with its one end being closed, being made of polypropylene, and being provided with 6 holes having 4.8 mm diameter.
  • the second head part 12 has such a structure that a sintered glass plate having pores with 40 ⁇ m diameter bonded onto the end of the hollow cylinder as described above.
  • the upper phase separation part 14 has such a structure that a vessel having a narrow mouth inserted at the upper side of the column part 13 (refer to FIG. 4B ).
  • the lower phase separation part 15 connected to the lower part of the column part 13 has such a structure that a vessel with a diameter larger than the diameter of the column part 13 . It should be noted that this apparatus has a processing capacity about 10 times larger than the processing capacity of the apparatus used in Embodiment 1.
  • Embodiment 1 the increased processing capacity for the aqueous solution from 20 litters per hour (in Embodiment 1) to 228 litters per hour (in Embodiment 2) gives little effect to the collection ratio of aluminum oxide Al 2 O 3 particles. From the experimental findings as described above, it is proved that the emulsion flow apparatus can be scaled-up while its processing capacity is maintained.
  • the size of holes formed at the head part from which the aqueous phase is spouted out (the first head part 11 ) is not dominant. That is, it is proved that larger sized holes formed at the first head part 11 could be applicable for processing the aqueous solution including the particle component having a larger size without plugging in the holes. It should also be noted that there is no concern of plugging problem at the second head part 12 because the particle component in the aqueous phase is not transported into the solvent phase.
  • H-660-type Continuous Centrifuge Separator manufactured by KOKUSAN Co. Ltd. in Japan
  • an experiment was carried out for collecting aluminum oxide Al 2 O 3 particles classified, which were the same as those used in Embodiment 1, from the aqueous solution.
  • the dimensions of H-660-type Continuous Centrifuge Separator are 650 mm in width, 650 mm in depth and 870 mm in height, its apparatus volume is 368 litters and its apparatus weight is 160 kg.
  • Dissolved metallic ion and suspended particle component can be selectively and simultaneously collected by adding an extraction agent relevant to the metal ion to such a solvent phase as isooctane; while, in Embodiment 1 and Embodiment 2, pure isooctane is used.
  • Embodiment 3 an experiment was carried out by using the above described intermediate-sized emulsion flow apparatus provided with 2 litters of isooctane including bis(2-ethylhexyl) phosphoric acid (DEHPA) as the extraction agent by 1 ⁇ 10 ⁇ 3 M and with 200 litters of aqueous nitric acid solution (pH 2) including aluminum oxide Al 2 O 3 particles as the particle component by 0.02 M and ytterbium Yb (trivalent ion) as the dissolved component by 6 ⁇ 10 ⁇ 6 M.
  • DEHPA bis(2-ethylhexyl) phosphoric acid
  • pH 2 aqueous nitric acid solution
  • Al 2 O 3 particles aluminum oxide Al 2 O 3 particles
  • ytterbium Yb trivalent ion
  • FIG. 4 ( a ) The intermediate-sized apparatus shown in FIG. 4 ( a ) was also used in this experiment, and under the condition that the flow rate of the aqueous phase to be supplied was set to be 231 litters per hour and the flow rate of the solvent phase to be circulated was set to be 30 litters per hour, the overall processing time for 200 litters of the aqueous solution was 52 minutes (with processing capacity of 231 litters per hour).
  • FIG. 5 shows a photo picture of large amount of aluminum oxide Al 2 O 3 particles deposited at the column part after completing the collecting operation in this embodiment.
  • the particle collection performance, defined in terms of the collection ratio, of the emulsion flow apparatus of the present invention is little different from that in of the continuous centrifuge separator.
  • the emulsion flow apparatus does not have a power output section that requires a number of heavy metallic parts, this apparatus is light and has no limitation in handling solutions containing acids.
  • a solvent as alkane for example, kerosene
  • a component dissolved in an aqueous solution can also be simultaneously collected and removed by liquid-liquid extraction.
  • the extraction agent may be added to an alkane as the solvent, in which this method can be fit to provide low environmental impact by using an extraction agent that has low solubility in water and has a tendency to be decomposed easily in environment.
  • a continuous extraction experiment for ytterbium Yb (III) from aqueous nitric acid solution was carried out by using a counter-current type emulsion flow extraction apparatus 10 , having the height of 70 cm, as shown in FIG. 4A and FIG. 4B .
  • the first head part 11 has such a structure that the side wall of the hollow cylinder with its one end being closed, being made of polypropylene and having 1.5 cm diameter and 5 cm in height, is provided with 38 holes (2 mm in diameter), and that TeflonTM sheet having mesh with 70 ⁇ m pitch covers over the side wall of the hollow cylinder.
  • the second head part has such a structure that a sintered glass plate having holes with 40 ⁇ m diameter is bonded onto one end of the hollow cylinder as described above.
  • the upper phase separation part 14 has such a structure that a vessel with a narrow mouth is inserted at the upper side of the column part 13 .
  • the lower phase separation part 15 has such a structure that a vessel having a diameter larger than the diameter of the column part 13 is coupled to the lower side of the column part 13 .
  • ytterbium Yb (III) and the liquid supply volume were measured: ytterbium Yb (III) and bis(2-ethylhexyl) phosphoric acid (DEHPA) are employed as a metal ion and an extraction agent (extractant), respectively.
  • the volume of the sample aqueous solution (aqueous phase) was 200 litters, the volume of the organic phase, in which isooctane was used as the solvent, was 2 litters.
  • Hydrogen ion exponent, pH, of the aqueous phase was adjusted to be 2.0 by adding nitric acid, and the concentration of ytterbium Yb (III) in the aqueous phase was set to be 6 ⁇ 10 ⁇ 4 M.
  • concentration of the extraction agent (DEHPA) in the organic phase was set to be 6 ⁇ 10 ⁇ 2 M.
  • the first head part 11 used in this experiment has such a structure that the hollow cylinder with its one end being closed, being made of polypropylene and having 1.5 cm diameter and 5 cm in height, is provided with only 6 holes having 4.8 mm diameter on the side wall of the cylinder (and without a mesh sheet).
  • the second head part 12 has the similar structure as Embodiment 1 in which a sintered glass plate having holes with 40 ⁇ m pore diameter is bonded onto the side wall of the hollow cylinder as described above.
  • the aqueous phase was sampled every 25 litters processed as drainage water, and then the concentration of ytterbium Yb (III) was measured by ICP-MS.
  • FIG. 7 shows the result of the measurement.
  • the extraction rate of ytterbium Yb (III) was about 97%, which was independent of the supply liquid volume. It is proved that a satisfactory level of extraction rate can be achieved although this result may be slightly smaller than the result of Embodiment 1 in which the extraction rate was 99%.
  • There was no plugging at the first head part 11 and the second head part 12 respectively. Note that the broken line in FIG. 7 plots the data from FIG. 6 .
  • Embodiment 2 Using the same counter-current type emulsion flow extraction apparatus as used in Embodiment 2 (with the same structures of the first head part 11 and the second head part 12 ), the time required for restarting the apparatus after stopping the apparatus was measured. After stopping completely the apparatus normally operated, the time from restarting the liquid supply pump to generation of stable emulsion flow was measured.
  • the liquid supply pump was made stop suddenly in operating the apparatus under the condition that the flow rate in the liquid supply of the aqueous phase is 205 litters/hour and the flow rate in circulating the organic phase is 30 litters/hour. It was found that the state of stable emulsion flow was established after about 5 seconds after restarting the liquid supply pump at 2 minutes passed after stopping suddenly the apparatus. Thus, it was proved that the operation of the apparatus can be restarted promptly without any adjusting work even if liquid supply process completely stops.
  • sulfuric acid aqueous solution including Al (8.4 ⁇ 10 ⁇ 4 M), Ti(4.6 ⁇ 10 ⁇ 4 M), Cr (1.1 ⁇ 10 ⁇ 4 M), Fe (4.2 ⁇ 10 ⁇ 2 M), Co (4.3 ⁇ 10 ⁇ 3 M), Ni (6.1 ⁇ 10 ⁇ 3 M), Cu (2.1 ⁇ 10 ⁇ 4 M), Mo (3.8 ⁇ 10 ⁇ 4 M) and U (5.0 ⁇ 10 ⁇ 7 M) was prepared, and the selective extraction of Uranium U was attempted by using the same counter-current type emulsion flow extraction apparatus as used in Embodiment 2.
  • Trioctyl amine (TOA) was used as an extraction agent, and isooctane including n-octanol with 2.5 vol % (volume percentage) was used as a solvent. Note that the concentration of TOA was 0.3 M.
  • An experiment was carried out under the condition that the flow rate in the liquid supply of the aqueous phase is 225 litters/hour and the flow rate in circulating the organic phase is 30 litters/hour. From the experimental result, it was proved that only Uranium U of low concentration can be extracted with its extractability of 97% in highly selective manner from the solution including various metal ions coexisting in high concentrations.
  • FIG. 8 shows the experimental result. Note that molybdenum Mo was extracted in some quantity, which may lead to an advantageous result because the removal of molybdenum Mo by precipitation is difficult intrinsically, and molybdenum Mo may be extracted as it happens.
  • the counter-current type emulsion flow continuous liquid-liquid extraction apparatus has a number of advantageous features in comparison with the conventional continuous liquid-liquid extraction apparatus (such as mixer-settler extractor, pulsed column and centrifugal extractor). For example, from the view point of cost-effectiveness, low running and maintenance costs are important features. Differently from the conventional continuous liquid-liquid extraction apparatus, the emulsion flow apparatus is not required to apply continuously the mechanical external forces (such as stirring and vibrating), the electric power consumption for the operation may be saved. The energy required to be used for driving the liquid supply may be free from electric power by applying the potential energy or the drainage water flow energy. In addition, handiness is one of the significant factors.
  • the emulsion flow continuous liquid-liquid extraction apparatus requires short adjusting work and little experienced skill for operating the apparatus because the apparatus is stable against the changes in the liquid supply volume and can be operated stably so as to restore the steady state within about 5 seconds even if the apparatus might shut down suddenly. Those features may lead to large reduction in the labor cost.
  • the apparatus is compact in its structure, it may be fabricated easily and with low cost, and the initial cost for installation may be low, and furthermore, as the apparatus does not require a large installation space due to its compact size, it may be advantageous to integrate the plant with the apparatus.
  • the apparatus according to the present invention advantageously provides higher safety features in comparison with the conventional apparatuses.
  • the following characteristics may contribute to higher safety features; insusceptibility of vibration (with high earthquake-resisting capacity) in the similar way to the column-type liquid-to-solid extractor, the reduced amount of organic solvent because of the compactness of the apparatus itself, and no existence of frictional heat generated due to the repetitive and continuous application of mechanical external forces (such as stirring and vibrating).
  • the reduced amount of waste solution in associate with adjusting work and the reduced level of ambient noises may provide valuable advantageous features in terms of environmental impact.
  • the above mentioned advantageous features come from the nature of the emulsion flow apparatus without using mechanical external forces, which enables to establish the efficient liquid-liquid extraction in a similar level of handiness to the column-type liquid-solid extraction.
  • the counter-current type emulsion flow continuous liquid-liquid extraction apparatus is expected to be widely put to practical use in various industrial fields related to liquid-liquid extraction technologies (such as metal refinement technology and rare metal recycling technology).
  • liquid-liquid extraction technologies such as metal refinement technology and rare metal recycling technology.
  • a new market development for liquid-liquid extraction may be expected.
  • next-generation continuous liquid-liquid extraction apparatus to be applied in wet reprocessing for spent nuclear fuels, and facilities for purifying the large amount of low-level radioactive liquid waste with lower cost and with high processing performance may be expected due to the nature of the emulsion flow apparatus such as higher safety features, easiness in handling, low cost and compactness of the apparatus itself (refer to Embodiment 4).
  • the conventional liquid-liquid extraction methods to the purifying processes for environmental water and the water treatment processes for a large amount of waste water

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CN102091436A (zh) * 2011-01-19 2011-06-15 中国科学院过程工程研究所 一种液-液-液三相连续逆流萃取装置及其使用方法
US8337789B2 (en) 2007-05-21 2012-12-25 Orsite Aluminae Inc. Processes for extracting aluminum from aluminous ores
US9023301B2 (en) 2012-01-10 2015-05-05 Orbite Aluminae Inc. Processes for treating red mud
CN104784967A (zh) * 2015-03-25 2015-07-22 合肥通用机械研究院 一种在线可调本级回流型离心萃取机及其调节方法
US9150428B2 (en) 2011-06-03 2015-10-06 Orbite Aluminae Inc. Methods for separating iron ions from aluminum ions
US9181603B2 (en) 2012-03-29 2015-11-10 Orbite Technologies Inc. Processes for treating fly ashes
US9260767B2 (en) 2011-03-18 2016-02-16 Orbite Technologies Inc. Processes for recovering rare earth elements from aluminum-bearing materials
US9290828B2 (en) 2012-07-12 2016-03-22 Orbite Technologies Inc. Processes for preparing titanium oxide and various other products
US9353425B2 (en) 2012-09-26 2016-05-31 Orbite Technologies Inc. Processes for preparing alumina and magnesium chloride by HCl leaching of various materials
US9382600B2 (en) 2011-09-16 2016-07-05 Orbite Technologies Inc. Processes for preparing alumina and various other products
US9410227B2 (en) 2011-05-04 2016-08-09 Orbite Technologies Inc. Processes for recovering rare earth elements from various ores
US9534274B2 (en) 2012-11-14 2017-01-03 Orbite Technologies Inc. Methods for purifying aluminium ions
RU2609112C2 (ru) * 2011-09-05 2017-01-30 Сайтек Текнолоджи Корп. Способы извлечения органического экстрагирующего растворителя из эмульсий, стабилизированных твердыми частицами, образующихся в контурах гидрометаллургической экстракции растворителем
CN118359289A (zh) * 2024-06-20 2024-07-19 合肥莱瑞科技有限公司 一种锂电池浆料废水处理装置

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CN102728099B (zh) * 2012-06-26 2014-09-24 中国科学院过程工程研究所 一种大相比体系梯度分级分离的填料萃取塔及萃取方法
JP6551550B2 (ja) * 2018-01-09 2019-07-31 信越化学工業株式会社 めっき液中の希土類金属イオン抽出除去方法

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Cited By (18)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US8337789B2 (en) 2007-05-21 2012-12-25 Orsite Aluminae Inc. Processes for extracting aluminum from aluminous ores
US8597600B2 (en) 2007-05-21 2013-12-03 Orbite Aluminae Inc. Processes for extracting aluminum from aluminous ores
CN102091436A (zh) * 2011-01-19 2011-06-15 中国科学院过程工程研究所 一种液-液-液三相连续逆流萃取装置及其使用方法
US9945009B2 (en) 2011-03-18 2018-04-17 Orbite Technologies Inc. Processes for recovering rare earth elements from aluminum-bearing materials
US9260767B2 (en) 2011-03-18 2016-02-16 Orbite Technologies Inc. Processes for recovering rare earth elements from aluminum-bearing materials
US9410227B2 (en) 2011-05-04 2016-08-09 Orbite Technologies Inc. Processes for recovering rare earth elements from various ores
US9150428B2 (en) 2011-06-03 2015-10-06 Orbite Aluminae Inc. Methods for separating iron ions from aluminum ions
RU2609112C2 (ru) * 2011-09-05 2017-01-30 Сайтек Текнолоджи Корп. Способы извлечения органического экстрагирующего растворителя из эмульсий, стабилизированных твердыми частицами, образующихся в контурах гидрометаллургической экстракции растворителем
US10174402B2 (en) 2011-09-16 2019-01-08 Orbite Technologies Inc. Processes for preparing alumina and various other products
US9382600B2 (en) 2011-09-16 2016-07-05 Orbite Technologies Inc. Processes for preparing alumina and various other products
US9023301B2 (en) 2012-01-10 2015-05-05 Orbite Aluminae Inc. Processes for treating red mud
US9556500B2 (en) 2012-01-10 2017-01-31 Orbite Technologies Inc. Processes for treating red mud
US9181603B2 (en) 2012-03-29 2015-11-10 Orbite Technologies Inc. Processes for treating fly ashes
US9290828B2 (en) 2012-07-12 2016-03-22 Orbite Technologies Inc. Processes for preparing titanium oxide and various other products
US9353425B2 (en) 2012-09-26 2016-05-31 Orbite Technologies Inc. Processes for preparing alumina and magnesium chloride by HCl leaching of various materials
US9534274B2 (en) 2012-11-14 2017-01-03 Orbite Technologies Inc. Methods for purifying aluminium ions
CN104784967A (zh) * 2015-03-25 2015-07-22 合肥通用机械研究院 一种在线可调本级回流型离心萃取机及其调节方法
CN118359289A (zh) * 2024-06-20 2024-07-19 合肥莱瑞科技有限公司 一种锂电池浆料废水处理装置

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US9108124B2 (en) 2015-08-18

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