EP0452401A1 - Dispositif de refrigeration a vide isolant commande par un sorbant - Google Patents

Dispositif de refrigeration a vide isolant commande par un sorbant

Info

Publication number
EP0452401A1
EP0452401A1 EP19900902055 EP90902055A EP0452401A1 EP 0452401 A1 EP0452401 A1 EP 0452401A1 EP 19900902055 EP19900902055 EP 19900902055 EP 90902055 A EP90902055 A EP 90902055A EP 0452401 A1 EP0452401 A1 EP 0452401A1
Authority
EP
European Patent Office
Prior art keywords
chamber
liquid
sorbent
vapor
heat
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.)
Withdrawn
Application number
EP19900902055
Other languages
German (de)
English (en)
Other versions
EP0452401A4 (en
Inventor
Cullen M. Sabin
Dennis A. Thomas
Gary V. Steidl
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
International Thermal Packaging Inc
Original Assignee
International Thermal Packaging Inc
Priority date (The priority date 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 date listed.)
Filing date
Publication date
Application filed by International Thermal Packaging Inc filed Critical International Thermal Packaging Inc
Publication of EP0452401A1 publication Critical patent/EP0452401A1/fr
Publication of EP0452401A4 publication Critical patent/EP0452401A4/en
Withdrawn legal-status Critical Current

Links

Classifications

    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F25—REFRIGERATION OR COOLING; COMBINED HEATING AND REFRIGERATION SYSTEMS; HEAT PUMP SYSTEMS; MANUFACTURE OR STORAGE OF ICE; LIQUEFACTION SOLIDIFICATION OF GASES
    • F25B—REFRIGERATION MACHINES, PLANTS OR SYSTEMS; COMBINED HEATING AND REFRIGERATION SYSTEMS; HEAT PUMP SYSTEMS
    • F25B39/00—Evaporators; Condensers
    • F25B39/02—Evaporators
    • F25B39/026—Evaporators specially adapted for sorption type systems
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F25—REFRIGERATION OR COOLING; COMBINED HEATING AND REFRIGERATION SYSTEMS; HEAT PUMP SYSTEMS; MANUFACTURE OR STORAGE OF ICE; LIQUEFACTION SOLIDIFICATION OF GASES
    • F25B—REFRIGERATION MACHINES, PLANTS OR SYSTEMS; COMBINED HEATING AND REFRIGERATION SYSTEMS; HEAT PUMP SYSTEMS
    • F25B17/00—Sorption machines, plants or systems, operating intermittently, e.g. absorption or adsorption type
    • F25B17/08—Sorption machines, plants or systems, operating intermittently, e.g. absorption or adsorption type the absorbent or adsorbent being a solid, e.g. salt
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F25—REFRIGERATION OR COOLING; COMBINED HEATING AND REFRIGERATION SYSTEMS; HEAT PUMP SYSTEMS; MANUFACTURE OR STORAGE OF ICE; LIQUEFACTION SOLIDIFICATION OF GASES
    • F25D—REFRIGERATORS; COLD ROOMS; ICE-BOXES; COOLING OR FREEZING APPARATUS NOT OTHERWISE PROVIDED FOR
    • F25D5/00—Devices using endothermic chemical reactions, e.g. using frigorific mixtures

Definitions

  • the invention relates to temperature changing devices and, in particular, to portable or disposable food or beverage coolers.
  • An alternate method for providing a cooled material on demand is to use portable insulated containers.
  • these containers function merely to maintain the previous temperature of the food or beverage placed inside them, or they require the use of ice cubes to provide the desired cooling effect.
  • insulated containers are much more bulky and heavy than the food or beverage.
  • ice may not be readily available when the cooling action is required.
  • Ice cubes have also been used independently to cool food or beverages rapidly. However, use of ice independently for cooling is often undesirable because ice may be stored only for limited periods above 0°C. Moreover, ice may not be available when the cooling action is desired.
  • a portable cooling device In addition to food and beverage cooling, there are a number of other applications for which a portable cooling device is extremely desirable. These include medical applications, including cooling of tissues or organs; preparation of cold compresses and cryogenic destruction of tissues as part of surgical procedures; industrial applications, including production of cold water or other liquids upon demand; preservation of biological specimens; cooling of protective clothing; and cosmetic applications.
  • medical applications including cooling of tissues or organs; preparation of cold compresses and cryogenic destruction of tissues as part of surgical procedures; industrial applications, including production of cold water or other liquids upon demand; preservation of biological specimens; cooling of protective clothing; and cosmetic applications.
  • a portable cooling apparatus could have widespread utility in all these areas.
  • An alternate procedure for providing a cooling effect in a portable device is to absorb or adsorb the refrigerant vapor in a chamber separate from the chamber in which the evaporation takes place.
  • the refrigerant liquid boils under reduced pressure in a sealed chamber and absorbs heat from its surroundings.
  • the vapor generated from the boiling liquid is continuously removed from the first chamber and discharged into a second chamber containing a desiccant or sorbent that absorbs the vapor.
  • one objective of the present invention is to provide a self-contained ⁇ orption cooling device with a means for handling heat produced in the sorbent so that the cooling effect in the evaporation chamber is not effectively diminished.
  • the present invention is a self-contained cooling apparatus comprising a first chamber containing a vaporizable liquid, an evacuated second chamber, and a third chamber containing a sorbent for the liquid, wherein the second chamber substantially surrounds the third chamber so that a vacuum surrounds the third chamber.
  • the second chamber is adapted to convey vaporized fluid between the first and the third chambers.
  • a valve prevents fluid communication between the first and the third chambers.
  • An actuator opens the valve to connect the first and third chambers, permitting the liquid to vaporize and permitting the vapor to pass through the second chamber into the sorbent. By opening the valve, a drop in pressure occurs in the first chamber because the second and third chambers are evacuated.
  • This drop in pressure causes the liquid in the first chamber to vaporize, and, because this liquid-to-gas phase change can occur only if the liquid removes heat equal to the latent heat of vaporization of the evaporated liquid from the first chamber, the first chamber cools.
  • the vapor passes through the second chamber into the third chamber where it is absorbed and adsorbed by the sorbent.
  • the sorbent also gains all of the heat contained in the absorbed or adsorbed vapor, and, if the absorbtion- adsorption process involves an exothermic chemical reaction, the sorbent must also absorb the reaction heat.
  • the heat contained within the sorbent is removed from the sorbent by a heat removing material.
  • that heat removing material is a phase change material which is thermally coupled to the sorbent. It has a thermal mass different from the material comprising the third chamber in contact with the sorbent and has a heat capacity greater than that of the sorbent.
  • the heat is also contained within the third chamber by a vacuum which insulates the third chamber.
  • the third chamber is mounted substantially concentrically within the second chamber, and in one embodiment the liquid vapor must flow substantially around the third chamber and into that third chamber.
  • the liquid is water.
  • a highly hydrophilic polymer lines the interior surface of the first chamber to maximize the surface area from which boiling may occur.
  • the liquid may be mixed with a nucleating agent that promotes ebullition of the liquid.
  • the present invention provides a self-contained rapid cooling device that cools a food, beverage or other material article from ambient temperature on demand in a timely manner, exhibits a useful change in temperature, retains the heat produced from the cooling process or retards the transfer of the heat from the sorbent back to the material being cooled, can be stored for unlimited periods without % losing its cooling potential, and is able to meet government standards for safety in human use.
  • Figure 1 is a schematic representation of a cooling device according to the present invention, wherein the second and third chambers are wholly within the first chamber.
  • Figure 2 is a schematic representation of a cooling device according to the present invention, wherein the second and third chambers are outside of the first chamber.
  • the cooling device 10 has a first chamber 12 containing a refrigerant liquid 18 and having its interior surface coated with a wicking material 16.
  • the cooling device 10 also includes a second chamber 20, which surrounds a third chamber 21.
  • the third chamber 21 is at least partially filled with a sorbent 24, which is optionally in contact with a heat-removing material 25.
  • the second chamber 20 and the third chamber 21 are in constant fluid communication. Initially, at least one of the two chambers is evacuated, thus creating a vacuum within the other.
  • a valve 30, Positioned between the first chamber 12 and the second chamber 20 is a valve 30, which allows fluid communication between the chambers 12 and 20 only when the valve 30 is open.
  • a conduit 28 is shown in Figure 2, a conduit 28.
  • the second chamber 20 and thus the third chamber 21 are wholly contained within the first chamber 12 so that no conduit is needed to connect the first chamber 12 and the second chamber 20.
  • the operation of the cooling device 10 is suspended (i.e., the system is static and no cooling occurs) until the valve 30 is opened, at which time the conduit 28 provides -fluid communication between the first, second, and third chambers, 12, 20 and 21 respectively. Opening the valve 30 between the first and second chambers 10 and 20 causes a drop in pressure in chamber 12 because the second chamber 20 is evacuated. The drop in pressure in the first chamber 12 upon opening of the valve 30 causes the liquid 18 to boil at ambient temperature into a liquid-vapor mixture 32. This liquid-to-gas phase change can occur only if the liquid 18 removes heat equal to the latent heat of vaporization of the evaporated liquid 18 from the first chamber 12. This causes the first chamber 12 to cool.
  • the cooled first chamber 12 removes heat from its surrounding material as indicated by the arrows 33.
  • the vapor is absorbed or adsorbed by the sorbent 24. This facilitates the maintenance of a reduced vapor pressure in the first chamber 12 and allows more of the liquid 18 to boil and become vapor, further reducing the temperature of chamber 12.
  • the continuous removal of the vapor maintains the pressure in the first chamber 12 below the vapor pressure of the liquid 18, so that the liquid 18 boils and produces vapor continuously until sorbent 24 is saturated, until the liquid 18 has boiled away or until the temperature of the liquid 18 has dropped below its boiling point.
  • the optional heat-removing material 25 which is thermally coupled to the sorbent 24 (and preferably is mixed with the sorbent 24) removes heat from the sorbent 24, preventing or slowing a rise in temperature in both the sorbent 24 and the third chamber 21, which rise in temperature might compromise the cooling effect produced by the first chamber 12.
  • the relationship of the three chambers performs another function which prevents any compromising of the cooling effect produced by the first chamber 12. Because the second chamber 20 is substantially evacuated and surrounds the third chamber 21, it forms an insulator so that the heat contained within the third chamber 21 remains within that chamber. The vacuum insulation about the third chamber 21 inhibits that chamber from warming the cooling first chamber 12.
  • the third chamber 21 is mounted substantially concentrically within the second chamber 20.
  • the entrance to the third chamber 21 is positioned so that the liquid vapor must flow substantially around the third chamber 21 until it enters the third chamber 21 and is sorbed by the sorbent 24.
  • the aforementioned configuration allows the construction of the cooling device 10 to be miniaturized and compact. Its size can be greatly reduced by placing the second and third chambers 20 and 21 within the first chamber 12. Nevertheless, it is understood that the second and third chambers 20 and 21 can be situated alongside of the first chamber 12 as is depicted in Figure 2 as long as the second chamber 20 insulates the third chamber 21 to prevent heat from compromising the cooling effect.
  • the device ensures that a vacuum will remain in the second chamber 20 at the most critical time to ensure insulation about the third chamber 21 - after the sorption process is complete. It is also preferable that, while there may not be a complete vacuum in the second chamber 20, it is at a pressure substantially lower than atmospheric during and after evaporation so that a substantial vacuum exists to insulate about the third chamber 21.
  • the liquid and the sorbent must be complimentary (i.e., the sorbent must be capable of absorbing or adsorbing the vapor produced by the liquid) , and suitable choices for these components would be any combination able to make a useful change in temperature in a short time, meet government standards for safety and be compact.
  • the refrigerant liquids used in the present invention preferably have a high vapor pressure at ambient temperature, so that a reduction of pressure will produce a high vapor production rate.
  • the vapor pressure of the liquid at 20°C is preferably at least about 9 mm Hg, and more preferably is at least about 15 or 20 mm Hg.
  • Liquids with suitable characteristics for various uses of the invention include: various alcohols, such as methyl alcohol and ethyl alcohol; ketones or aldehydes, such as acetone and acetaldehyde; water; and freons, such as freon C318, 114, 21, 11, 114B2, 113 and 112.
  • the preferred liquid is water.
  • the refrigerant liquid may be mixed with an effective quantity of a miscible nucleating agent having a greater vapor pressure than the liquid to promote ebullition so that the liquid evaporates even more quickly and smoothly, and so that supercooling of the liquid does not occur.
  • Suitable nucleating agents include ethyl alcohol, acetone, methyl alcohol, propyl alcohol and isobutyl alcohol, all of which are miscible with water.
  • a combination of a nucleating agent with a compatible liquid might be a combination of 5% ethyl alcohol in water or 5% acetone in methyl alcohol.
  • the nucleating agent preferably has a vapor pressure at 25°C of at least about 25 mm Hg and, more preferably, at least about 35 mm Hg.
  • solid nucleating agents may be used, such as the conventional boiling stones used in chemical laboratory applications.
  • the sorbent material used in the third chamber 21 is preferably capable of absorbing and adsorbing all the vapor produced by the liquid, and also preferably will meet government safety standards for use in an environment where contact with food may occur.
  • Suitable sorbent ⁇ for various applications may include barium oxide, magnesium perchlorate, calcium ⁇ ulfate, calcium oxide, activated carbon, calcium chloride, glycerine, silica gel, alumina gel, calcium hydride, phosphoric anhydride, phosphoric acid, potassium hydroxide, sulphuric acid, lithium chloride, ethylene glycol and sodium sulfate.
  • the heat-removing material may be one of three types: (1) a material that undergoes a change of phase when heat is applied; (2) a material that has a heat capacity greater than the sorbent; or (3) a material that undergoes an endothermic reaction when brought in contact with the liquid refrigerant.
  • Suitable phase change materials for particular applications may be selected from paraffin, naphthalene, sulphur, hydrated calcium chloride, bro ocamphor, cetyl alcohol, cyanimide, eleudic acid, lauric acid, hydrated sodium silicate, sodium thiosulfate pentahydrate, disodium phosphate, hydrated sodium carbonate, hydrated calcium nitrate, Glauber's salt, potassium, sodium and magnesium acetate.
  • the phase change materials remove some of the heat from the sorbent material simply through storage of sensible heat. In other words, they heat up as the sorbent heats up, removing heat from the sorbent. However, the most effective function of the phase change material is in the phase change itself.
  • phase change material in connection with the phase change (i.e., change from a solid phase to a liquid phase, or change from a liquid phase to a vapor phase) .
  • phase change material which change from a solid phase to a liquid, absorbing from the sorbent their latent heat of fusion, are the most practical in a .closed system.
  • a phase change material changing from a liquid to a vapor is also feasible.
  • an environmentally-safe liquid could be provided in a separate container (not shown) in contact with the sorbent material (to absorb heat therefrom) but vented in such a way that the boiling phase change material carries heat away from the sorbent material and entirely out of the system.
  • phase change materials change phase at a temperature greater than the expected ambient temperature of the material to be cooled, but less than the temperature achieved by the sorbent material upon absorption of a substantial fraction (i.e., one-third or one-quarter) of the refrigerant liquid.
  • the phase change material could change phase at a temperature above about 30 °C, preferably above about 35°C but preferably below about 70°C, and most preferably below about 60°C.
  • substantially higher or lower phase change temperatures may be desirable.
  • phase change materials with phase change temperatures as high as 90°C, 100°C or 110°C may be appropriate in certain systems.
  • Various materials which have a high specific heat include cyanimide, ethyl alcohol, ethyl ether, glycerol, isoamyl alcohol, isobutyl alcohol, lithium hydride, methyl alcohol, sodium acetate, water, ethylene glycol and paraffin wax.
  • the heat-absorbing material for example, is a liquid, it may be necessary to package that liquid or otherwise prevent physical contact between the heat- absorbing material and the sorbent. Small individual containers of heat-absorbing material scattered throughout the sorbent may be utilized when the sorbent and the heat- absorbing material cannot contact one another. Alternatively, the heat-absorbing material may be placed in a single package having a relatively high surface area in contact with the sorbent to facilitate heat transfer from the sorbent into the heat-absorbing material.
  • the third category of heat-removing material (material that undergoes an endothermic reaction) has the advantage of completely removing heat from the system and storing it in the form of a chemical change.
  • the endothermic material may advantageously be a material that undergoes an endothermic reaction when it comes in contact with the refrigerant liquid (or vapor) .
  • the valve 30 in the conduit 28 is opened, permitting vapor to flow through the conduit 28 into the third chamber 21,. -the vapor comes in contact with some of the endothermic material, which then undergoes an endothermic reaction, removing heat from the sorbent 24.
  • Such endothermic materials have the advantage that the heat is more or less permanently removed from the sorbent, and little, if any, of that heat can be retransferred to the material being cooled. This is in contrast to phase change materials and materials having a heat capacity greater than the sorbent material, both of which may eventually give up their stored heat to the surrounding materials, although such heat exchange (because of design factors that retard heat transfer, such as poor thermal conductivity of the sorbent 24) generally does not occur with sufficient rapidity to reheat the cooled material prior to use of that material.
  • Heat-absorbing materials which undergo an endothermic reaction may variously be selected from such compounds as H 2 B0 3 , PbBr 2 , Br0 3 , KC10 3 , K 2 Cr 2 0 7 , KC10 , K 2 S, Snl 2 , NH4CI, KMn ⁇ 4 and CSCIO4.
  • the heat-removing material may be advantageously in contact with the sorbent.
  • the sorbent and heat-removing material could be blended, the heat-removing material could be in discrete pieces mixed with the sorbent, or the material could be a mass in contact with, but not mixed into, the sorbent.
  • any of a number of materials may be chosen, depending upon the requirements of the system and the particular refrigerant liquid 18 being used.
  • the wicking material may be something as simple as cloth or fabric having an affinity for the refrigerant liquid 18 and a substantial wicking ability.
  • the wicking material may be cloth, sheets, felt or flocking material which may be comprised of cotton, filter material, natural cellulose, regenerated cellulose, cellulose derivatives, blotting paper or any other suitable material.
  • the most preferred wicking material would be highly hydrophilie, such as gel-forming polymers which would be capable of coating the interior surface of the evaporation 0/07684 _ __ 3 _ P
  • Such materials preferably consist of alkyl, aryl and amino derivative polymers of vinylchloride acetate, vinylidene chloride, tetrafluoroethylene , methyl methacrylate, hexanedoic acid, dihydro-2,5-furandione, propenoic acid, 1, 3-isobenzofurandione, 1 h-pyrrole-2, 5- dione or hexahydro-2 h-azepin-2-one.
  • the wicking material may be sprayed, flocked, or otherwise coated or applied onto the interior surface of the first chamber 12.
  • the wicking material is electrostatically deposited onto that
  • the wicking material is mixed with a suitable solvent, such as a non-aqueous solvent, and then the solution is applied to the interior surface of the first chamber 12.
  • a suitable solvent such as a non-aqueous solvent
  • the wicking material is able to control any violent boiling of the evaporator and thus reduces any liquid entrainment in the vapor phase.
  • the wicking material is a polymer forming a porous space-filling or sponge-like structure, and it may fill all or part of the first chamber 12.
  • the valve 30 may be selected from any of the various types shown in the prior art.
  • the valve 30 may be located at any location between the first chamber 14 and the third chamber 21 so long as it prevents vapor from being sorbed by the sorbent 24.
  • a pressure responsive valve can be used which can actuate the cooling device upon the release of the pressure within the container.
  • the invention also includes a method of using the cooling device described herein.
  • This method includes the step of providing a cooling device of the type set forth herein; opening the valve between the first chamber 12 and the second chamber 20, whereby the pressure in the first chamber is reduced, causing the liquid to boil, forming a vapor, which vapor is collected by the sorbent material; removing vapor from the second chamber by collecting the same in the sorbent until an equilibrium condition is reached wherein the sorbent is substantially saturated or substantially all of the liquid originally in the first chamber has been collected in the sorbent; and simultaneously removing heat from the sorbent by means of the heat-removing material described above.
  • the process is preferably a one-shot process; thus, opening of the valve 30 in the conduit 28 connecting the first chamber 12 and the second chamber 20 is preferably irreversible.
  • the system is a closed system; in other words, the refrigerant liquid does not escape the system, and there is no means whereby the refrigerant liquid or the sorbent may escape either the first chamber 12 or the second chamber 20.

Landscapes

  • Engineering & Computer Science (AREA)
  • Physics & Mathematics (AREA)
  • Mechanical Engineering (AREA)
  • Thermal Sciences (AREA)
  • General Engineering & Computer Science (AREA)
  • Chemical & Material Sciences (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Combustion & Propulsion (AREA)
  • Sorption Type Refrigeration Machines (AREA)

Abstract

Dispositif autonome à refroidissement rapide qui garde la chaleur produite lors du refroidissement et qui peut être stocké pour des périodes illimitées sans perdre son potentiel de refroidissement. Un liquide (18) dans une première chambre (12) subit un changement de phase, de la phase liquide vers la phase vapeur, qui refroidit la première chambre (12). Une deuxième chambre forme un vide isolant autour d'une troisième chambre (21) contenant un sorbant. Le sorbant (24) dans la troisième chambre (21) permet une communication fluide avec la vapeur et évacue la vapeur à partir de la première chambre (12). Le dispositif est autonome puisque un matériau (25) en contact avec le sorbant (24) absorbe la chaleur du sorbant (24) afin d'empêcher une réduction dans l'effet de refroidissement produit par la première chambre. De plus, un vide isolant autour d'une troisième chambre (21) empêche le sorbant de chaleur (24) de diminuer l'effet de refroidissement.
EP19900902055 1989-01-05 1990-01-02 Vacuum insulated sorbent-driven refrigeration device Withdrawn EP0452401A4 (en)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
US29381289A 1989-01-05 1989-01-05
US293812 1989-01-05

Publications (2)

Publication Number Publication Date
EP0452401A1 true EP0452401A1 (fr) 1991-10-23
EP0452401A4 EP0452401A4 (en) 1992-01-02

Family

ID=23130686

Family Applications (1)

Application Number Title Priority Date Filing Date
EP19900902055 Withdrawn EP0452401A4 (en) 1989-01-05 1990-01-02 Vacuum insulated sorbent-driven refrigeration device

Country Status (4)

Country Link
EP (1) EP0452401A4 (fr)
JP (1) JPH04502665A (fr)
AU (1) AU623220B2 (fr)
WO (1) WO1990007684A1 (fr)

Families Citing this family (6)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
AU8712591A (en) * 1990-08-01 1992-03-02 International Thermal Packaging, Inc. Vacuum insulated sorbent-driven refrigeration device
CA2362571C (fr) * 1999-02-26 2007-11-27 Tempra Technology, Inc. Preparation de materiaux de refroidissement
CN1188643C (zh) * 1999-02-26 2005-02-09 坦普拉技术公司 相变热沉物料的制备方法
WO2007121480A2 (fr) * 2006-04-18 2007-10-25 Medivance Incorporated Appareil et methode permettant de refroidir un liquide dans un système de refroidissement intravasculaire
WO2011007165A2 (fr) * 2009-07-13 2011-01-20 Specmat Limited Appareil permettant de refroidir un objet
JP6899748B2 (ja) * 2017-09-25 2021-07-07 株式会社前川製作所 移動体の冷却システム

Family Cites Families (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US2871674A (en) * 1956-12-12 1959-02-03 Sulo C Koivisto Portable refrigeration unit
US3642059A (en) * 1969-06-30 1972-02-15 Leonard Greiner Heating and cooling unit
SE7706357A0 (sv) * 1977-05-31 1978-12-01 Ray Olsson Sätt vid kylning av ett utrymme samt anordning för genomförande av sättet
US4250720A (en) * 1979-03-12 1981-02-17 Israel Siegel Disposable non-cyclic sorption temperature-changers
US4759191A (en) * 1987-07-07 1988-07-26 Liquid Co2 Engineering, Inc. Miniaturized cooling device and method of use

Also Published As

Publication number Publication date
EP0452401A4 (en) 1992-01-02
WO1990007684A1 (fr) 1990-07-12
AU4941390A (en) 1990-08-01
JPH04502665A (ja) 1992-05-14
AU623220B2 (en) 1992-05-07

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