EP0057324A1 - Process of spraying emulsions and apparatus thereof - Google Patents
Process of spraying emulsions and apparatus thereof Download PDFInfo
- Publication number
- EP0057324A1 EP0057324A1 EP81306005A EP81306005A EP0057324A1 EP 0057324 A1 EP0057324 A1 EP 0057324A1 EP 81306005 A EP81306005 A EP 81306005A EP 81306005 A EP81306005 A EP 81306005A EP 0057324 A1 EP0057324 A1 EP 0057324A1
- Authority
- EP
- European Patent Office
- Prior art keywords
- liquid
- emulsion
- orifice
- charged
- potential
- Prior art date
- Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
- Granted
Links
Images
Classifications
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B05—SPRAYING OR ATOMISING IN GENERAL; APPLYING FLUENT MATERIALS TO SURFACES, IN GENERAL
- B05B—SPRAYING APPARATUS; ATOMISING APPARATUS; NOZZLES
- B05B5/00—Electrostatic spraying apparatus; Spraying apparatus with means for charging the spray electrically; Apparatus for spraying liquids or other fluent materials by other electric means
- B05B5/16—Arrangements for supplying liquids or other fluent material
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01F—MIXING, e.g. DISSOLVING, EMULSIFYING OR DISPERSING
- B01F23/00—Mixing according to the phases to be mixed, e.g. dispersing or emulsifying
- B01F23/40—Mixing liquids with liquids; Emulsifying
- B01F23/41—Emulsifying
- B01F23/411—Emulsifying using electrical or magnetic fields, heat or vibrations
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01F—MIXING, e.g. DISSOLVING, EMULSIFYING OR DISPERSING
- B01F33/00—Other mixers; Mixing plants; Combinations of mixers
- B01F33/05—Mixers using radiation, e.g. magnetic fields or microwaves to mix the material
Definitions
- This invention relates to spraying emulsions. More particularly, it relates to new processes for forming emulsions and spraying the emulsions so formed, and to apparatus therefor.
- An emulsion consists of small particles (generally of mean diameter in the range 0.1 to 10 microns) of a first liquid dispersed in a second liquid immiscible therewith.
- an emulsion may be formed of finely divided particles of oil in water; or conversely, of finely divided particles of water in oil, the latter being commonly referred to as an invert emulsion.
- An emulsion is a two- phase system; the particles constitute the disperse phase, while the medium in which they are suspended is the continuous phase. The propertiies of emulsions naturally depend on the properties of the two phases, their relative proportions and the particle size of the disperse phase.
- Dilute emulsions containing for example up to 10% or so of disperse phase, generally have, for example, a viscosity not dissimilar from that of the continuous phase; but increasing the proportion of the disperse phase leads to thickening, and the formation of immobile, scarcely pourable systems.
- the present invention is concerned with relatively dilute emulsions, not too thick to be able to flowlike liquids.
- Emulsions have a variety of uses; for example in the- food and pharmaceutical industries. Cosmetics may be formulated asemulsions, and so also may pesticides. The present invention relates to emulsions to be used as sprays.
- Emulsions are generally formed by thoroughly agitating the two phases together, for example in a high shear mixer. This is a relatively inefficient process, consuming unnecessary energy.
- emulsions so formed are not necessarily stable, and may break down into separate bulk phases on storage.
- the present invention provides a more efficient method of forming emulsions, not dependent on mechanical mixing, and which prevents emulsion break-down by reducing or eliminating storage time.
- a process for forming and spraying a dilute emulsion of a first liquid in a second liquid immiscible therewith which comprises passing small amounts of the first liquid into a body of the second liquid while electrically charging the first liquid relative to the second liquid to a potential sufficient to cause emulsification therein, and atomising the charged emulsion thereby formed.
- Such atomisation may be carried. out wholly or partly by mechanical means, but conveniently it may be effected by passing the charged emulsion into a region of high electrical field strength thereby causing it to atomise.
- the invention further comprises apparatus for forming and spraying an electrically charged emulsion of a first liquid in a second liquid immiscible therewith which comprises an orifice formed in an electrically conducting material communicating with a vessel for containing the second liquid, means for delivering the first liquid to and through the orifice, means for charging the orifice to a high potential, and a sprayhead for receiving the electrically charged emulsion formed at the orifice and for emitting the emulsion in the form of an electrically charged spray.
- the sprayhead comprises an electrically conducting surface for receiving the electrically charged emulsion, and means for creating a field strength at the surface sufficient to atomise the emulsion therefrom in the form of a fine spray.
- the emulsions being electrostatically charged, are attracted to spray targets and coat them more evenly than uncharged sprays would do. Electrostatic force fields carry the charged particles behind the target, so as to coat all sides of it.
- the method and apparatus of the invention may be used for spraying paints and like coatings on to structures or articles of manufacture, and (with particular advantage) for spraying pesticides (eg, insecticides, herbicides, fungicides and the like) on to crops or weeds.
- pesticides eg, insecticides, herbicides, fungicides and the like
- Conveniently emulsions according to the invention comprise from about 1 to about 10% by weight disperse phase, though higher and lower amounts may be used where appropriate.
- a container 1 of insulating material (glass) is provided with an earthed jacket 13 of conductive material, and with a conduit 2 for delivering liquid.
- a metallic exit nozzle 3 In the base of the container 1 is a metallic exit nozzle 3, with a bore of capillary.size.
- a metal ring 4 connected (as shown in Figure 2) to earth 19.
- a second container 5 of insulating material (glass) fed by a liquid delivering conduit 6.
- a second metallic exit nozzle 7, of capillary dimensions is provided in the base of container 1 a second metallic exit nozzle 7, of capillary dimensions.
- Both nozzles 3 and 7 are connected (as shown in Figure 2) to a source of high potential 8 (0-20 kilovolts, 200 microamp module) via a switch 9.
- a source of high potential 8 (0-20 kilovolts, 200 microamp module)
- a switch 9 Below the container 5, within the container 1, and symmetrically disposed around the outlet of the nozzle 7, is a second earthed metal ring. 10.
- the nozzle 3 may be closed by an exterior cap or bung 12.
- a hydrocarbon oil 11 is passed into the container 1 from the conduit 2 until the level of oil 11 is above the base of container 5.
- An aqueous solution containing 7% by weight of para q uat dichloride is passed through conduit 6 into container 5.
- Capillary-sized droplets of the aqueous solution pass out through nozzle 7 and sink through the oil 11.
- the switch 9 is then closed, applying a voltage of the order of 15 kilovolts to the nozzles 7 and 3.
- the oil in the container 1 becomes turbulent, exhibiting negative surface tension due to the electrical charge it carries.
- the cap 12 is then removed, and the emulsion (containing about 4% weight disperse phase) issues from the nozzle 3.
- the electric field between the nozzle 3 and the earthed ring 4 causes the emulsion to atomise as fine particles, which pass outwards and are attracted to suitable targets, eg, weeds.
- suitable targets eg, weeds.
- the flows of oil 11 through conduit 2 and of aqueous solution through conduit 6 are adjusted to maintain the levels of liquid in containers 1 and 5 constant.
- the particle size of the disperse phase in the emulsion may be controlled by control of the field strength at the nozzle 7; eg, by varying the distance between the nozzle 7 and the ring 10, or, more conveniently, by varying the applied voltage. The stronger the field the smaller are the droplets.
- the particle size of droplets in the atomised emulsion may be controlled by control of the field strength at the nozzle 3. This may be done by varying the voltage on the nozzle 3, the position of the ring 4, or by applying a variable voltage (positive or negative with respect to the potential of the nozzle 3) to the ring 4 instead of earthing it.
- the same apparatus may be used, if desired, to form an emulsion in which water or an aqueous solution is the continuous phase and oil is the disperse phase, by feeding water to container 1 and oil to container 2.
- the nozzle 7 may be charged by induction, as shown in Figure 3. If the nozzle 7 is connected to the earth 19, and the source of potential 8 to ring 10, a strong charge of opposite sign will be induced on nozzle 7 and liquid passing through will be charged by contact in the same way as if the nozzle 7 were connected to source of potential 8, except that the charge will be of opposite sign.
- An emulsion will be formed in just the same way, with the charging current being taken from earth. This saves current at nozzle 7, but slightly more is used at nozzle3, because the emulsion has to be discharged and recharged in the opposite sense before atomisation.
- the power consumption of the device is not high, and is readily adapted to use in portable devices powered by dry cells, or even solar cells. For agricultural spraying, however, it will often be convenient to mount the device on a vehicle (eg a tractor or aircraft) and power it from a power source carried on the vehicle (eg the tractor battery).
- the emulsion may be atomised wholly or partly mechanically, eg from a pressure nozzle or spinning cup or disc.
- electrostatic atomisation is preferred, with advantages which may include lower energy usage, apparatus with fewer or no moving parts, and spray droplets of very regular and controllable size.
Abstract
Description
- This invention relates to spraying emulsions. More particularly, it relates to new processes for forming emulsions and spraying the emulsions so formed, and to apparatus therefor.
- An emulsion consists of small particles (generally of mean diameter in the range 0.1 to 10 microns) of a first liquid dispersed in a second liquid immiscible therewith. For example, an emulsion may be formed of finely divided particles of oil in water; or conversely, of finely divided particles of water in oil, the latter being commonly referred to as an invert emulsion. An emulsion is a two- phase system; the particles constitute the disperse phase, while the medium in which they are suspended is the continuous phase. The propertiies of emulsions naturally depend on the properties of the two phases, their relative proportions and the particle size of the disperse phase. Dilute emulsions, containing for example up to 10% or so of disperse phase, generally have, for example, a viscosity not dissimilar from that of the continuous phase; but increasing the proportion of the disperse phase leads to thickening, and the formation of immobile, scarcely pourable systems. The present invention is concerned with relatively dilute emulsions, not too thick to be able to flowlike liquids.
- Emulsions have a variety of uses; for example in the- food and pharmaceutical industries. Cosmetics may be formulated asemulsions, and so also may pesticides. The present invention relates to emulsions to be used as sprays.
- Emulsions are generally formed by thoroughly agitating the two phases together, for example in a high shear mixer. This is a relatively inefficient process, consuming unnecessary energy.
- Moreover, emulsions so formed are not necessarily stable, and may break down into separate bulk phases on storage. The present invention provides a more efficient method of forming emulsions, not dependent on mechanical mixing, and which prevents emulsion break-down by reducing or eliminating storage time.
- According to the present invention we provide a process for forming and spraying a dilute emulsion of a first liquid in a second liquid immiscible therewith, which comprises passing small amounts of the first liquid into a body of the second liquid while electrically charging the first liquid relative to the second liquid to a potential sufficient to cause emulsification therein, and atomising the charged emulsion thereby formed. Such atomisation may be carried. out wholly or partly by mechanical means, but conveniently it may be effected by passing the charged emulsion into a region of high electrical field strength thereby causing it to atomise.
- The invention further comprises apparatus for forming and spraying an electrically charged emulsion of a first liquid in a second liquid immiscible therewith which comprises an orifice formed in an electrically conducting material communicating with a vessel for containing the second liquid, means for delivering the first liquid to and through the orifice, means for charging the orifice to a high potential, and a sprayhead for receiving the electrically charged emulsion formed at the orifice and for emitting the emulsion in the form of an electrically charged spray. Conveniently the sprayhead comprises an electrically conducting surface for receiving the electrically charged emulsion, and means for creating a field strength at the surface sufficient to atomise the emulsion therefrom in the form of a fine spray.
- The emulsions, being electrostatically charged, are attracted to spray targets and coat them more evenly than uncharged sprays would do. Electrostatic force fields carry the charged particles behind the target, so as to coat all sides of it. The method and apparatus of the invention may be used for spraying paints and like coatings on to structures or articles of manufacture, and (with particular advantage) for spraying pesticides (eg, insecticides, herbicides, fungicides and the like) on to crops or weeds. Conveniently emulsions according to the invention comprise from about 1 to about 10% by weight disperse phase, though higher and lower amounts may be used where appropriate.
- A specific embodiment of the invention will now be described with reference to the drawings, in which:
- Figure 1 is a vertical cross-section through a spraying device according to the invention adapted to spray an invert emulsion of aqueous herbicide in oil;
- Figure 2 is a circuit diagram for the device;
- Figure 3 is an alternative circuit diagram for the device.
- In figure 1, a container 1 of insulating material (glass) is provided with an
earthed jacket 13 of conductive material, and with a conduit 2 for delivering liquid. In the base of the container 1 is ametallic exit nozzle 3, with a bore of capillary.size. Below the container 1, and disposed symmetrically around the outlet ofnozzle 3, is a metal ring 4 connected (as shown in Figure 2) toearth 19. Centrally within the upper part of the container 1 is a second container 5 of insulating material (glass) fed by aliquid delivering conduit 6. In the base of container 5 is a second metallic exit nozzle 7, of capillary dimensions. Bothnozzles 3 and 7 are connected (as shown in Figure 2) to a source of high potential 8 (0-20 kilovolts, 200 microamp module) via a switch 9. Below the container 5, within the container 1, and symmetrically disposed around the outlet of the nozzle 7, is a second earthed metal ring. 10. Thenozzle 3 may be closed by an exterior cap orbung 12. - In operation, a
hydrocarbon oil 11 is passed into the container 1 from the conduit 2 until the level ofoil 11 is above the base of container 5. An aqueous solution containing 7% by weight of paraquat dichloride is passed throughconduit 6 into container 5. Capillary-sized droplets of the aqueous solution pass out through nozzle 7 and sink through theoil 11. The switch 9 is then closed, applying a voltage of the order of 15 kilovolts to thenozzles 7 and 3. At once the passage of capillary-sized droplets into theoil 11 ceases, and the oil becomes cloudy, indicating the formation of an emulsion. The liquid in the container 1 becomes turbulent, exhibiting negative surface tension due to the electrical charge it carries. Thecap 12 is then removed, and the emulsion (containing about 4% weight disperse phase) issues from thenozzle 3. The electric field between thenozzle 3 and the earthed ring 4 causes the emulsion to atomise as fine particles, which pass outwards and are attracted to suitable targets, eg, weeds. Meanwhile the flows ofoil 11 through conduit 2 and of aqueous solution throughconduit 6 are adjusted to maintain the levels of liquid in containers 1 and 5 constant. - The particle size of the disperse phase in the emulsion may be controlled by control of the field strength at the nozzle 7; eg, by varying the distance between the nozzle 7 and the
ring 10, or, more conveniently, by varying the applied voltage. The stronger the field the smaller are the droplets. Similarly, the particle size of droplets in the atomised emulsion may be controlled by control of the field strength at thenozzle 3. This may be done by varying the voltage on thenozzle 3, the position of the ring 4, or by applying a variable voltage (positive or negative with respect to the potential of the nozzle 3) to the ring 4 instead of earthing it. - The same apparatus may be used, if desired, to form an emulsion in which water or an aqueous solution is the continuous phase and oil is the disperse phase, by feeding water to container 1 and oil to container 2.
- If desired, the nozzle 7 may be charged by induction, as shown in Figure 3. If the nozzle 7 is connected to the
earth 19, and the source of potential 8 to ring 10, a strong charge of opposite sign will be induced on nozzle 7 and liquid passing through will be charged by contact in the same way as if the nozzle 7 were connected to source of potential 8, except that the charge will be of opposite sign. An emulsion will be formed in just the same way, with the charging current being taken from earth. This saves current at nozzle 7, but slightly more is used at nozzle3, because the emulsion has to be discharged and recharged in the opposite sense before atomisation. In any case the power consumption of the device is not high, and is readily adapted to use in portable devices powered by dry cells, or even solar cells. For agricultural spraying, however, it will often be convenient to mount the device on a vehicle (eg a tractor or aircraft) and power it from a power source carried on the vehicle (eg the tractor battery). - If desired, (eg to obtain a greater throughput rate than is normally conveniently available through electrostatic atomisation) the emulsion may be atomised wholly or partly mechanically, eg from a pressure nozzle or spinning cup or disc. Generally, however, electrostatic atomisation is preferred, with advantages which may include lower energy usage, apparatus with fewer or no moving parts, and spray droplets of very regular and controllable size.
Claims (10)
Priority Applications (1)
Application Number | Priority Date | Filing Date | Title |
---|---|---|---|
AT81306005T ATE19597T1 (en) | 1981-01-30 | 1981-12-21 | METHOD AND DEVICE FOR SPRAYING EMULSIONS. |
Applications Claiming Priority (2)
Application Number | Priority Date | Filing Date | Title |
---|---|---|---|
GB8102823 | 1981-01-30 | ||
GB8102823 | 1981-01-31 |
Publications (2)
Publication Number | Publication Date |
---|---|
EP0057324A1 true EP0057324A1 (en) | 1982-08-11 |
EP0057324B1 EP0057324B1 (en) | 1986-05-07 |
Family
ID=10519331
Family Applications (1)
Application Number | Title | Priority Date | Filing Date |
---|---|---|---|
EP81306005A Expired EP0057324B1 (en) | 1981-01-30 | 1981-12-21 | Process of spraying emulsions and apparatus thereof |
Country Status (7)
Country | Link |
---|---|
EP (1) | EP0057324B1 (en) |
JP (1) | JPS57159564A (en) |
AT (1) | ATE19597T1 (en) |
AU (1) | AU7917082A (en) |
CA (1) | CA1176508A (en) |
DE (1) | DE3174591D1 (en) |
NZ (1) | NZ199410A (en) |
Cited By (8)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
EP0356030A2 (en) * | 1988-08-15 | 1990-02-28 | United Kingdom Atomic Energy Authority | A method of enhanced solvent Extraction and apparatus therefor |
WO2002055211A1 (en) * | 2001-01-12 | 2002-07-18 | The Procter & Gamble Company | Electrostatic spray device |
US6682004B2 (en) | 1999-08-18 | 2004-01-27 | The Procter & Gamble Company | Electrostatic spray device |
US6814318B2 (en) | 1999-08-18 | 2004-11-09 | The Procter & Gamble Company | Disposable cartridge for electrostatic spray device |
US6860439B2 (en) | 2002-03-01 | 2005-03-01 | Unilever Home & Personal Care Usa, Division Of Conopco, Inc. | Electrostatic spraying of a cosmetic composition |
WO2007131917A1 (en) * | 2006-05-15 | 2007-11-22 | Unilever Plc | Process for preparing an emulsion |
US7712687B2 (en) | 1999-08-18 | 2010-05-11 | The Procter & Gamble Company | Electrostatic spray device |
CN110935338A (en) * | 2019-09-24 | 2020-03-31 | 福建爱溥环保设备有限公司 | Device and method for mixing oil and water into floccule |
Families Citing this family (1)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
JP4877173B2 (en) * | 2007-09-21 | 2012-02-15 | パナソニック電工株式会社 | Electrostatic atomizer and heated air blower equipped with the same |
Citations (10)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
FR639245A (en) * | 1927-08-09 | 1928-06-16 | Process for preparing emulsions by means of an electric charge | |
GB320919A (en) * | 1928-06-19 | 1929-10-21 | Provia Soc | Improved process of and apparatus for making bituminous emulsions and distributing same on road surfaces |
FR1017481A (en) * | 1950-02-07 | 1952-12-11 | Onera (Off Nat Aerospatiale) | Improvements in means for the production of electrified particles, in particular electrified droplets |
FR1087802A (en) * | 1952-04-18 | 1955-03-01 | Harper J Ransburg Company | Process for coating objects by spraying and equipment for its implementation |
FR1122243A (en) * | 1955-01-07 | 1956-09-04 | Bonnet Reymond Sa | Advanced atomizer |
FR1182266A (en) * | 1957-04-15 | 1959-06-24 | Automatic valve with emulsion pump | |
US3131131A (en) * | 1962-04-03 | 1964-04-28 | Socony Mobil Oil Co Inc | Electrostatic mixing in microbial conversions |
US3873023A (en) * | 1972-09-18 | 1975-03-25 | Ransburg Corp | Apparatus for and method of spraying plural component materials |
GB1564973A (en) * | 1976-12-30 | 1980-04-16 | Research Corp | Electrostatic spray nozzle system |
GB1569707A (en) * | 1976-07-15 | 1980-06-18 | Ici Ltd | Atomisation of liquids |
-
1981
- 1981-12-21 EP EP81306005A patent/EP0057324B1/en not_active Expired
- 1981-12-21 AT AT81306005T patent/ATE19597T1/en active
- 1981-12-21 DE DE8181306005T patent/DE3174591D1/en not_active Expired
-
1982
- 1982-01-04 AU AU79170/82A patent/AU7917082A/en not_active Abandoned
- 1982-01-06 NZ NZ199410A patent/NZ199410A/en unknown
- 1982-01-29 CA CA000395245A patent/CA1176508A/en not_active Expired
- 1982-01-29 JP JP57013213A patent/JPS57159564A/en active Pending
Patent Citations (10)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
FR639245A (en) * | 1927-08-09 | 1928-06-16 | Process for preparing emulsions by means of an electric charge | |
GB320919A (en) * | 1928-06-19 | 1929-10-21 | Provia Soc | Improved process of and apparatus for making bituminous emulsions and distributing same on road surfaces |
FR1017481A (en) * | 1950-02-07 | 1952-12-11 | Onera (Off Nat Aerospatiale) | Improvements in means for the production of electrified particles, in particular electrified droplets |
FR1087802A (en) * | 1952-04-18 | 1955-03-01 | Harper J Ransburg Company | Process for coating objects by spraying and equipment for its implementation |
FR1122243A (en) * | 1955-01-07 | 1956-09-04 | Bonnet Reymond Sa | Advanced atomizer |
FR1182266A (en) * | 1957-04-15 | 1959-06-24 | Automatic valve with emulsion pump | |
US3131131A (en) * | 1962-04-03 | 1964-04-28 | Socony Mobil Oil Co Inc | Electrostatic mixing in microbial conversions |
US3873023A (en) * | 1972-09-18 | 1975-03-25 | Ransburg Corp | Apparatus for and method of spraying plural component materials |
GB1569707A (en) * | 1976-07-15 | 1980-06-18 | Ici Ltd | Atomisation of liquids |
GB1564973A (en) * | 1976-12-30 | 1980-04-16 | Research Corp | Electrostatic spray nozzle system |
Cited By (12)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
EP0356030A2 (en) * | 1988-08-15 | 1990-02-28 | United Kingdom Atomic Energy Authority | A method of enhanced solvent Extraction and apparatus therefor |
EP0356030A3 (en) * | 1988-08-15 | 1990-09-05 | United Kingdom Atomic Energy Authority | A method of enhanced solvent extraction and apparatus therefor |
US5022973A (en) * | 1988-08-15 | 1991-06-11 | United Kingdom Atomic Energy Authority | Method of electrostatically enhanced solvent extraction and apparatus therefor |
US6682004B2 (en) | 1999-08-18 | 2004-01-27 | The Procter & Gamble Company | Electrostatic spray device |
US6814318B2 (en) | 1999-08-18 | 2004-11-09 | The Procter & Gamble Company | Disposable cartridge for electrostatic spray device |
US7152817B2 (en) | 1999-08-18 | 2006-12-26 | The Procter & Gamble Company | Electrostatic spray device |
US7712687B2 (en) | 1999-08-18 | 2010-05-11 | The Procter & Gamble Company | Electrostatic spray device |
WO2002055211A1 (en) * | 2001-01-12 | 2002-07-18 | The Procter & Gamble Company | Electrostatic spray device |
CN1292840C (en) * | 2001-01-12 | 2007-01-03 | 宝洁公司 | Electrostatic spray device |
US6860439B2 (en) | 2002-03-01 | 2005-03-01 | Unilever Home & Personal Care Usa, Division Of Conopco, Inc. | Electrostatic spraying of a cosmetic composition |
WO2007131917A1 (en) * | 2006-05-15 | 2007-11-22 | Unilever Plc | Process for preparing an emulsion |
CN110935338A (en) * | 2019-09-24 | 2020-03-31 | 福建爱溥环保设备有限公司 | Device and method for mixing oil and water into floccule |
Also Published As
Publication number | Publication date |
---|---|
JPS57159564A (en) | 1982-10-01 |
EP0057324B1 (en) | 1986-05-07 |
NZ199410A (en) | 1985-08-16 |
AU7917082A (en) | 1982-08-12 |
ATE19597T1 (en) | 1986-05-15 |
CA1176508A (en) | 1984-10-23 |
DE3174591D1 (en) | 1986-06-12 |
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