CA1185882A - Analytical means - Google Patents
Analytical meansInfo
- Publication number
- CA1185882A CA1185882A CA000390350A CA390350A CA1185882A CA 1185882 A CA1185882 A CA 1185882A CA 000390350 A CA000390350 A CA 000390350A CA 390350 A CA390350 A CA 390350A CA 1185882 A CA1185882 A CA 1185882A
- Authority
- CA
- Canada
- Prior art keywords
- fluid
- analytical means
- test
- fluid reservoir
- swellable polymer
- 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.)
- Expired
Links
Classifications
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01L—CHEMICAL OR PHYSICAL LABORATORY APPARATUS FOR GENERAL USE
- B01L3/00—Containers or dishes for laboratory use, e.g. laboratory glassware; Droppers
- B01L3/50—Containers for the purpose of retaining a material to be analysed, e.g. test tubes
- B01L3/508—Containers for the purpose of retaining a material to be analysed, e.g. test tubes rigid containers not provided for above
- B01L3/5082—Test tubes per se
-
- G—PHYSICS
- G01—MEASURING; TESTING
- G01N—INVESTIGATING OR ANALYSING MATERIALS BY DETERMINING THEIR CHEMICAL OR PHYSICAL PROPERTIES
- G01N31/00—Investigating or analysing non-biological materials by the use of the chemical methods specified in the subgroup; Apparatus specially adapted for such methods
- G01N31/22—Investigating or analysing non-biological materials by the use of the chemical methods specified in the subgroup; Apparatus specially adapted for such methods using chemical indicators
-
- G—PHYSICS
- G01—MEASURING; TESTING
- G01N—INVESTIGATING OR ANALYSING MATERIALS BY DETERMINING THEIR CHEMICAL OR PHYSICAL PROPERTIES
- G01N33/00—Investigating or analysing materials by specific methods not covered by groups G01N1/00 - G01N31/00
- G01N33/48—Biological material, e.g. blood, urine; Haemocytometers
- G01N33/50—Chemical analysis of biological material, e.g. blood, urine; Testing involving biospecific ligand binding methods; Immunological testing
- G01N33/52—Use of compounds or compositions for colorimetric, spectrophotometric or fluorometric investigation, e.g. use of reagent paper and including single- and multilayer analytical elements
- G01N33/525—Multi-layer analytical elements
Abstract
ABSTRACT OF THE DISCLOSURE
An analytical means for the detection of ingred-ients of aqueous or water-containing fluids is described, which means comprises two fluid-absorbing zones in mutual contact, one of which is composed of a chromatographically active material and the other serves as a fluid reservoir and is composed of a hydrophilic swellable polymer.
An analytical means for the detection of ingred-ients of aqueous or water-containing fluids is described, which means comprises two fluid-absorbing zones in mutual contact, one of which is composed of a chromatographically active material and the other serves as a fluid reservoir and is composed of a hydrophilic swellable polymer.
Description
so
- 2 The invention relates to an analytical means or the de section of ingredients ox aqueous or water-containing fluids .
In analytical screening methods, a pronounced 5 trend to the use of quick tests based on srr,al:L test rods, which are understood as esserltially two-dimensional struck lures, such as test strips, has been noticeable for a number of years . However, toes t strips enclosed by a film or structures in the shape ox small tubes are also 10 Icnown German AuslegeschriIt 1,498,875 and German O~fenlegungsschrift 1,940,964). These Buick tests are applied either by immersion OX an absorbent material, for example paper, which is impregnated with the chemicals necessary for the -test, into the sample to be examined 15 and observation of any color reaction which may occur, or by immersion OX a par-t OX the paper impregnated with . chemicals, chromatographic absorption ox the sample and observation of a color change in the non-~mmersed part OX the paper.
I Chromatographic quick tests of the last mentioned type are in general used. when before, during or after -the redaction of the chemicals necessary for the test with the substance to be detected it its intended to obtain a . separation of the substance to be detected from other sub-25 stances present in the sample, the reaction products of the chemicals necessary for the lo it, or various reagents from one another I'll essential precondition for fault-free, lopper-educible functioning of chronl.a~o~raph.ic quick tests is auniforin chromatographic saturation of that par, of -the absorbent material which has not been immersed, and to s in turn is achieved by making fluid available uniformly d reproducibly at a precisely defined starting line of the chromatographically active material.
US. Patent Specifications and 3,91~,647 have disclosed a quick-test device josh comprises a chromatographically active material and a sample vessel rigidly connected thereto, the sample vessel communicating lo with the absorbent material via fluid-permeable orifices.
The manufacture of this quick-test device is expensive, and the test strip must always be held Yen-tidally after immersion. Moreover, since fluid is sucked into the chroma-tographically active material, the fluid level in the reservoir falls and -the starting line ox the chroma-togram thus continuously changes during the test, and this leads to considerable fluctuations in the length of time taken for chromatography.
According to German Offenlegungsschrift 2,215,089, the chroma-togra.phically active rrlateriai it joined to a layer of a syllable gel former which serves as a fluid re~.crvoir, This process leads to a product winch, in the mois-tstate,i.s very unstable mechanically and readily becomes smear and, additionally, the gel itself strongly retains the moisture and -the swelling process is slow.
.. None ox these analytical wryness meet the demands which must be made on a chromato~raphi.c quickest device, namely simple handling, intensive mamlfac-ture without us problems and reproducible chromatographic proper-ties (sleight of development, time ox development due -to curl-slant availability of fluids It was therefore the object OX the invention to combine these demands in an improved cryptographic quickest device, comprising chromatographically acid material in the fluid reservoir, with reproducible Abe sorption ox` fluid.
Surprisingly, it has now been found that porous it hydrophilic, non~gel-forming syllable polymer are outstandingly suitable, even if the pore structure is non-uniform and coarse, as self~drawin~ fluid reservoirs with a very high and uniform absorption and release of fluid in a chromatographic quick-test device.
The preparation of porous hydroph~lic, syllable polymers is described, for example in German Offenlegungs-shrift 2,739,008 and 2,722,025, page 8 and 9.
Accordingly, examples of suitable polymeric sub-stances ox hydrophilic nature are regenerated and modified types of cellulose, which may be chemically cross linked, w~ter-insoluble graft polymers of cellulose and synthetic hydrophilic polymer--~ormers, such as polyacrylamides, polyacrylic acids, polyglycols and polyvinyl pyrrolidones, as well as these synthetic polymer-~ormers alone in a I cross linked form.
Regenerated, modified and/or crosslil~ed types cellulose are preferred.
The c~Jnsid~rable swelling capacity in aqueous media proves to be very advan-cageolls o'er purposes of the TV
inv~ntiorl, A dry sponge of these polymers con, for example, be compressed to 1/10 of its ret vole byway simple pressing step, and it retains this form until it is moistener. Not only -two dimensional, paper-like structures but also powders 9 flakes or other shaped structures can be used for this purpose. A dry-pressed two-dimensional material of the same dry strength as the chromatographically active material used can ad vantageously be employed for the preparation of test strips 9 since the least difficulties are then to be ox-pealed in production engineering.
Papers ox cellulose or cellulose derivatives as well as coated silica gels suitable for chromatography, and the like can be used as the chromatographically active material.
The examples which follow are intended to explain the invention:
to 1: Test s-trip for the de-termination of alpha aimless in urine A 10 mm long, 7 mm wide and 0.2 morn -thick piece ox dry-press~d artificial sponge ox regenerated cell-love is glued to one end of a plastic film ox 0.3 mm thickness, 7 mm width and 10 am length. Adjoining the wormer, a piece of filter paper of 40 mm length, 7 mm width and 0.2 mm thickness is glued on. One or several streaks of water-insoluble chromogenic starch compound ar~a~plied to the paper 5 transversely to the direction of the test strip.
To carry out the test, the lower third ox that erred of the test strip to which the artificial sponge is ' glued is immersed in urine ' '120 I of urine are sucked up by the artificial sponge, with e~pansicn to approximately ten times the thickness, and are trays-ported onwards to the joint edge with the filter paperweight this edge, the chromatography process s arts after about 2 seconds, and it is finished after about 5 minutes.
The aimless content can bread offsemi-cuantita-tivel~J from number of the starch streakswhicn have been detached' during these 5 minutes.
' In other embodiments, the sponge itself can '- already contain cherrlicals or other substances (for example enzymes) necessary for the test, the fluid absorption ''''capacity decreasing slightly. '' '"''-' Another technically utilizable property of the artificial sponge results from the fact that the pressed sponge is only syllable with water and can thus also be sod in an optimum manner in effluents which are severely contaminated with organic matter, without the fluid Abe -.0 sorption capacity already being saturated by non-aqueous solvents.
Exarn~le 2: Test for iron content in effluent (see drawing) ,, _ ' A small plastic tube (1) (Makrolon(R)) having an internal diameter of 6 mm is closed at one end lath a ~ater-permeable perforated plate (2j, and it is then filled with about 1 ml of a loose bed of a powder I of venerated cellulose of a particle size of about 1 2 mm d~alne~er, and the bed is compacted to 1 ml (= 3 CDI lent ox Thea small tube with the rid of a paper stopper (4) _ 7 _ inserted afterwards. above the latter, a paper sleeve (5) having an external dimwit of 6 mm and impregnated with potassium hexacyanoferrate-~I)is arranged and this is pressed against the paper stopper (4) with the aid of a closure plug (6).
. To carry out the test, the small tube Ruth the water permeable perforated plate is immersed for about 6 seconds into the effluent sample. The defined qua-lily of fluid absorbed within this period migrates into the paper sleeve (5) where sparingly soluble Prussian Blue is formed WriteNow Fe-tLII)salts, When chromatography is complete, the concentration of Fissility in the effluent sample can be read off from the height of the Prussian Blue zone in the paper sleeve (5) by reference Lo to the calibration curve.
,. ' , ' .
,
In analytical screening methods, a pronounced 5 trend to the use of quick tests based on srr,al:L test rods, which are understood as esserltially two-dimensional struck lures, such as test strips, has been noticeable for a number of years . However, toes t strips enclosed by a film or structures in the shape ox small tubes are also 10 Icnown German AuslegeschriIt 1,498,875 and German O~fenlegungsschrift 1,940,964). These Buick tests are applied either by immersion OX an absorbent material, for example paper, which is impregnated with the chemicals necessary for the -test, into the sample to be examined 15 and observation of any color reaction which may occur, or by immersion OX a par-t OX the paper impregnated with . chemicals, chromatographic absorption ox the sample and observation of a color change in the non-~mmersed part OX the paper.
I Chromatographic quick tests of the last mentioned type are in general used. when before, during or after -the redaction of the chemicals necessary for the test with the substance to be detected it its intended to obtain a . separation of the substance to be detected from other sub-25 stances present in the sample, the reaction products of the chemicals necessary for the lo it, or various reagents from one another I'll essential precondition for fault-free, lopper-educible functioning of chronl.a~o~raph.ic quick tests is auniforin chromatographic saturation of that par, of -the absorbent material which has not been immersed, and to s in turn is achieved by making fluid available uniformly d reproducibly at a precisely defined starting line of the chromatographically active material.
US. Patent Specifications and 3,91~,647 have disclosed a quick-test device josh comprises a chromatographically active material and a sample vessel rigidly connected thereto, the sample vessel communicating lo with the absorbent material via fluid-permeable orifices.
The manufacture of this quick-test device is expensive, and the test strip must always be held Yen-tidally after immersion. Moreover, since fluid is sucked into the chroma-tographically active material, the fluid level in the reservoir falls and -the starting line ox the chroma-togram thus continuously changes during the test, and this leads to considerable fluctuations in the length of time taken for chromatography.
According to German Offenlegungsschrift 2,215,089, the chroma-togra.phically active rrlateriai it joined to a layer of a syllable gel former which serves as a fluid re~.crvoir, This process leads to a product winch, in the mois-tstate,i.s very unstable mechanically and readily becomes smear and, additionally, the gel itself strongly retains the moisture and -the swelling process is slow.
.. None ox these analytical wryness meet the demands which must be made on a chromato~raphi.c quickest device, namely simple handling, intensive mamlfac-ture without us problems and reproducible chromatographic proper-ties (sleight of development, time ox development due -to curl-slant availability of fluids It was therefore the object OX the invention to combine these demands in an improved cryptographic quickest device, comprising chromatographically acid material in the fluid reservoir, with reproducible Abe sorption ox` fluid.
Surprisingly, it has now been found that porous it hydrophilic, non~gel-forming syllable polymer are outstandingly suitable, even if the pore structure is non-uniform and coarse, as self~drawin~ fluid reservoirs with a very high and uniform absorption and release of fluid in a chromatographic quick-test device.
The preparation of porous hydroph~lic, syllable polymers is described, for example in German Offenlegungs-shrift 2,739,008 and 2,722,025, page 8 and 9.
Accordingly, examples of suitable polymeric sub-stances ox hydrophilic nature are regenerated and modified types of cellulose, which may be chemically cross linked, w~ter-insoluble graft polymers of cellulose and synthetic hydrophilic polymer--~ormers, such as polyacrylamides, polyacrylic acids, polyglycols and polyvinyl pyrrolidones, as well as these synthetic polymer-~ormers alone in a I cross linked form.
Regenerated, modified and/or crosslil~ed types cellulose are preferred.
The c~Jnsid~rable swelling capacity in aqueous media proves to be very advan-cageolls o'er purposes of the TV
inv~ntiorl, A dry sponge of these polymers con, for example, be compressed to 1/10 of its ret vole byway simple pressing step, and it retains this form until it is moistener. Not only -two dimensional, paper-like structures but also powders 9 flakes or other shaped structures can be used for this purpose. A dry-pressed two-dimensional material of the same dry strength as the chromatographically active material used can ad vantageously be employed for the preparation of test strips 9 since the least difficulties are then to be ox-pealed in production engineering.
Papers ox cellulose or cellulose derivatives as well as coated silica gels suitable for chromatography, and the like can be used as the chromatographically active material.
The examples which follow are intended to explain the invention:
to 1: Test s-trip for the de-termination of alpha aimless in urine A 10 mm long, 7 mm wide and 0.2 morn -thick piece ox dry-press~d artificial sponge ox regenerated cell-love is glued to one end of a plastic film ox 0.3 mm thickness, 7 mm width and 10 am length. Adjoining the wormer, a piece of filter paper of 40 mm length, 7 mm width and 0.2 mm thickness is glued on. One or several streaks of water-insoluble chromogenic starch compound ar~a~plied to the paper 5 transversely to the direction of the test strip.
To carry out the test, the lower third ox that erred of the test strip to which the artificial sponge is ' glued is immersed in urine ' '120 I of urine are sucked up by the artificial sponge, with e~pansicn to approximately ten times the thickness, and are trays-ported onwards to the joint edge with the filter paperweight this edge, the chromatography process s arts after about 2 seconds, and it is finished after about 5 minutes.
The aimless content can bread offsemi-cuantita-tivel~J from number of the starch streakswhicn have been detached' during these 5 minutes.
' In other embodiments, the sponge itself can '- already contain cherrlicals or other substances (for example enzymes) necessary for the test, the fluid absorption ''''capacity decreasing slightly. '' '"''-' Another technically utilizable property of the artificial sponge results from the fact that the pressed sponge is only syllable with water and can thus also be sod in an optimum manner in effluents which are severely contaminated with organic matter, without the fluid Abe -.0 sorption capacity already being saturated by non-aqueous solvents.
Exarn~le 2: Test for iron content in effluent (see drawing) ,, _ ' A small plastic tube (1) (Makrolon(R)) having an internal diameter of 6 mm is closed at one end lath a ~ater-permeable perforated plate (2j, and it is then filled with about 1 ml of a loose bed of a powder I of venerated cellulose of a particle size of about 1 2 mm d~alne~er, and the bed is compacted to 1 ml (= 3 CDI lent ox Thea small tube with the rid of a paper stopper (4) _ 7 _ inserted afterwards. above the latter, a paper sleeve (5) having an external dimwit of 6 mm and impregnated with potassium hexacyanoferrate-~I)is arranged and this is pressed against the paper stopper (4) with the aid of a closure plug (6).
. To carry out the test, the small tube Ruth the water permeable perforated plate is immersed for about 6 seconds into the effluent sample. The defined qua-lily of fluid absorbed within this period migrates into the paper sleeve (5) where sparingly soluble Prussian Blue is formed WriteNow Fe-tLII)salts, When chromatography is complete, the concentration of Fissility in the effluent sample can be read off from the height of the Prussian Blue zone in the paper sleeve (5) by reference Lo to the calibration curve.
,. ' , ' .
,
Claims (3)
OR PRIVILEGE IS CLAIMED ARE DEFINED AS FOLLOWS:
1. An analytical means for the detection of ingredients of aqueous or water-containing fluids, comprising at least two fluid-absorbing zones which are in mutual contact, at least one of said zones being composed of a chromatographically active material and another serving as a fluid reservoir, and a carrier which is two-dimensional or has the form of a hollow body and stabilizes the arrangement of the zones, wherein the zone serving as a fluid reservoir is composed of a hydrophilic swellable polymer.
2. An analytical means as claimed in claim 1, wherein the fluid reservoir is a plastic sponge of a hydrophilic swellable polymer.
3. An analytical means as claimed in claim 1, wherein the hydrophilic swellable polymer is composed of regenerated cellu-lose or a cellulose derivative.
Applications Claiming Priority (2)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| DE19803043608 DE3043608A1 (en) | 1980-11-19 | 1980-11-19 | ANALYTICAL AGENT |
| DEP3043608.9 | 1980-11-19 |
Publications (1)
| Publication Number | Publication Date |
|---|---|
| CA1185882A true CA1185882A (en) | 1985-04-23 |
Family
ID=6117127
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| CA000390350A Expired CA1185882A (en) | 1980-11-19 | 1981-11-18 | Analytical means |
Country Status (6)
| Country | Link |
|---|---|
| EP (1) | EP0052328B1 (en) |
| JP (1) | JPS57113363A (en) |
| AT (1) | ATE11342T1 (en) |
| AU (1) | AU551024B2 (en) |
| CA (1) | CA1185882A (en) |
| DE (2) | DE3043608A1 (en) |
Cited By (6)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US5135873A (en) * | 1989-11-27 | 1992-08-04 | Syntex (U.S.A.) Inc. | Device and method for completing a fluidic circuit which employs a liquid expandable piece of bibulous material |
| US5602040A (en) * | 1987-04-27 | 1997-02-11 | Unilever Patent Holdings B.V. | Assays |
| US5620657A (en) * | 1989-11-27 | 1997-04-15 | Behringwerke Ag | Device and method for completing a fluidic circuit |
| US5622871A (en) | 1987-04-27 | 1997-04-22 | Unilever Patent Holdings B.V. | Capillary immunoassay and device therefor comprising mobilizable particulate labelled reagents |
| USRE37437E1 (en) | 1984-12-15 | 2001-11-06 | Dade Behring Marburg, Gmbh | Sheet-like diagnostic device |
| US6352862B1 (en) | 1989-02-17 | 2002-03-05 | Unilever Patent Holdings B.V. | Analytical test device for imuno assays and methods of using same |
Families Citing this family (5)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| DD278482A3 (en) * | 1988-06-22 | 1990-05-09 | Univ Berlin Humboldt | DEVICE AND METHOD FOR CHROMATOGRAPHIC SEPARATION |
| DE3842702A1 (en) * | 1988-12-19 | 1990-06-21 | Boehringer Mannheim Gmbh | TEST CARRIER FOR ANALYTICAL EXAMINATION OF A SAMPLING LIQUID WITH THE AID OF A SPECIFIC BINDING REACTION OF TWO BIOAFFIN BINDING PARTNERS AND A CORRESPONDING TEST PROCEDURE |
| AU634814B2 (en) * | 1989-09-14 | 1993-03-04 | Terumo Kabushiki Kaisha | Method for determination of ion concentration, specific gravity, or osmotic pressure of solution and apparatus therefor |
| US6979576B1 (en) | 1997-07-25 | 2005-12-27 | Shu-Ching Cheng | Methods of use of one step immunochromatographic device for Streptococcus A antigen |
| US6699722B2 (en) | 2000-04-14 | 2004-03-02 | A-Fem Medical Corporation | Positive detection lateral-flow apparatus and method for small and large analytes |
Family Cites Families (6)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| DE1598224A1 (en) * | 1964-10-12 | 1970-07-30 | Heinrich Dipl Chem Gerhard Her | Process and tubes for carrying out clinical-chemical analyzes |
| US3595754A (en) * | 1969-02-12 | 1971-07-27 | Baxter Laboratories Inc | Fabric for testing amylase activity |
| US3811840A (en) * | 1969-04-01 | 1974-05-21 | Miles Lab | Test device for detecting low concentrations of substances in fluids |
| JPS5844208B2 (en) * | 1976-08-31 | 1983-10-01 | 東洋濾紙株式会社 | Test piece |
| DE2711201C3 (en) * | 1977-03-15 | 1980-06-12 | 7800 Freiburg | Method of checking the levels of urea in the human body |
| DE2739008A1 (en) * | 1977-08-30 | 1979-03-15 | Behringwerke Ag | Indicator sheet for use with liquids, esp. blood and urine - having coating of hydrophilic swellable polymer particles, preventing indicator running |
-
1980
- 1980-11-19 DE DE19803043608 patent/DE3043608A1/en not_active Withdrawn
-
1981
- 1981-11-10 DE DE8181109588T patent/DE3168396D1/en not_active Expired
- 1981-11-10 AT AT81109588T patent/ATE11342T1/en not_active IP Right Cessation
- 1981-11-10 EP EP81109588A patent/EP0052328B1/en not_active Expired
- 1981-11-18 AU AU77601/81A patent/AU551024B2/en not_active Expired
- 1981-11-18 CA CA000390350A patent/CA1185882A/en not_active Expired
- 1981-11-18 JP JP56183910A patent/JPS57113363A/en active Pending
Cited By (12)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US6228660B1 (en) | 1908-04-27 | 2001-05-08 | Conopco Inc. | Capillary immunoassay and device therefor comprising mobilizable particulate labelled reagents |
| USRE37437E1 (en) | 1984-12-15 | 2001-11-06 | Dade Behring Marburg, Gmbh | Sheet-like diagnostic device |
| USRE38688E1 (en) | 1984-12-15 | 2005-01-18 | Dade Behring Marburg Gmbh | Sheet-like diagnostic device |
| US5602040A (en) * | 1987-04-27 | 1997-02-11 | Unilever Patent Holdings B.V. | Assays |
| US5622871A (en) | 1987-04-27 | 1997-04-22 | Unilever Patent Holdings B.V. | Capillary immunoassay and device therefor comprising mobilizable particulate labelled reagents |
| US5656503A (en) | 1987-04-27 | 1997-08-12 | Unilever Patent Holdings B.V. | Test device for detecting analytes in biological samples |
| US6187598B1 (en) | 1987-04-27 | 2001-02-13 | Conopco Inc. | Capillary immunoassay and device therefor comprising mobilizable particulate labelled reagents |
| US6818455B2 (en) | 1987-04-27 | 2004-11-16 | Inverness Medical Switzerland Gmbh | Capillary immunoassay and device therefor comprising mobilizable particulate labelled reagents |
| US6352862B1 (en) | 1989-02-17 | 2002-03-05 | Unilever Patent Holdings B.V. | Analytical test device for imuno assays and methods of using same |
| US5135873A (en) * | 1989-11-27 | 1992-08-04 | Syntex (U.S.A.) Inc. | Device and method for completing a fluidic circuit which employs a liquid expandable piece of bibulous material |
| US5620657A (en) * | 1989-11-27 | 1997-04-15 | Behringwerke Ag | Device and method for completing a fluidic circuit |
| US5622870A (en) * | 1989-11-27 | 1997-04-22 | Behringwerke Ag | Device and method for completing a fluidic circuit |
Also Published As
| Publication number | Publication date |
|---|---|
| EP0052328B1 (en) | 1985-01-16 |
| DE3168396D1 (en) | 1985-02-28 |
| AU7760181A (en) | 1982-05-27 |
| EP0052328A3 (en) | 1982-06-23 |
| JPS57113363A (en) | 1982-07-14 |
| AU551024B2 (en) | 1986-04-17 |
| ATE11342T1 (en) | 1985-02-15 |
| EP0052328A2 (en) | 1982-05-26 |
| DE3043608A1 (en) | 1982-06-24 |
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Legal Events
| Date | Code | Title | Description |
|---|---|---|---|
| MKEX | Expiry |