CA1285767C - Method of disinfecting petroleum and petroleum products - Google Patents
Method of disinfecting petroleum and petroleum productsInfo
- Publication number
- CA1285767C CA1285767C CA000497210A CA497210A CA1285767C CA 1285767 C CA1285767 C CA 1285767C CA 000497210 A CA000497210 A CA 000497210A CA 497210 A CA497210 A CA 497210A CA 1285767 C CA1285767 C CA 1285767C
- Authority
- CA
- Canada
- Prior art keywords
- petroleum
- propylene oxide
- inert carrier
- disinfecting
- concentration
- 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 - Fee Related
Links
Classifications
-
- A—HUMAN NECESSITIES
- A61—MEDICAL OR VETERINARY SCIENCE; HYGIENE
- A61L—METHODS OR APPARATUS FOR STERILISING MATERIALS OR OBJECTS IN GENERAL; DISINFECTION, STERILISATION OR DEODORISATION OF AIR; CHEMICAL ASPECTS OF BANDAGES, DRESSINGS, ABSORBENT PADS OR SURGICAL ARTICLES; MATERIALS FOR BANDAGES, DRESSINGS, ABSORBENT PADS OR SURGICAL ARTICLES
- A61L2/00—Methods or apparatus for disinfecting or sterilising materials or objects other than foodstuffs or contact lenses; Accessories therefor
- A61L2/16—Methods or apparatus for disinfecting or sterilising materials or objects other than foodstuffs or contact lenses; Accessories therefor using chemical substances
- A61L2/20—Gaseous substances, e.g. vapours
-
- A—HUMAN NECESSITIES
- A01—AGRICULTURE; FORESTRY; ANIMAL HUSBANDRY; HUNTING; TRAPPING; FISHING
- A01N—PRESERVATION OF BODIES OF HUMANS OR ANIMALS OR PLANTS OR PARTS THEREOF; BIOCIDES, e.g. AS DISINFECTANTS, AS PESTICIDES OR AS HERBICIDES; PEST REPELLANTS OR ATTRACTANTS; PLANT GROWTH REGULATORS
- A01N43/00—Biocides, pest repellants or attractants, or plant growth regulators containing heterocyclic compounds
- A01N43/02—Biocides, pest repellants or attractants, or plant growth regulators containing heterocyclic compounds having rings with one or more oxygen or sulfur atoms as the only ring hetero atoms
- A01N43/04—Biocides, pest repellants or attractants, or plant growth regulators containing heterocyclic compounds having rings with one or more oxygen or sulfur atoms as the only ring hetero atoms with one hetero atom
- A01N43/20—Biocides, pest repellants or attractants, or plant growth regulators containing heterocyclic compounds having rings with one or more oxygen or sulfur atoms as the only ring hetero atoms with one hetero atom three- or four-membered rings
-
- C—CHEMISTRY; METALLURGY
- C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
- C09K—MATERIALS FOR MISCELLANEOUS APPLICATIONS, NOT PROVIDED FOR ELSEWHERE
- C09K8/00—Compositions for drilling of boreholes or wells; Compositions for treating boreholes or wells, e.g. for completion or for remedial operations
- C09K8/02—Well-drilling compositions
- C09K8/03—Specific additives for general use in well-drilling compositions
- C09K8/035—Organic additives
-
- C—CHEMISTRY; METALLURGY
- C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
- C09K—MATERIALS FOR MISCELLANEOUS APPLICATIONS, NOT PROVIDED FOR ELSEWHERE
- C09K8/00—Compositions for drilling of boreholes or wells; Compositions for treating boreholes or wells, e.g. for completion or for remedial operations
- C09K8/60—Compositions for stimulating production by acting on the underground formation
- C09K8/605—Compositions for stimulating production by acting on the underground formation containing biocides
Abstract
ABSTRACT OF THE DISCLOSURE
The method uses propylene oxide as the active substance. It is particularly suitable for inhibiting undesirable growth of microorganisms in drilling for petroleum.
The method uses propylene oxide as the active substance. It is particularly suitable for inhibiting undesirable growth of microorganisms in drilling for petroleum.
Description
~X~5767 METHOD OF DISINFECTING PETROLEUM AND PETROLEUM PRODUCTS
This invention relates to methods of disinfection, and more partic-ularly to a method of disinfecting petroleum and petroleum products, es-pecially for inhibiting the growth of microorganisms capable of living therein. The method is well suited for application in drilling for petroleum.
In exploring for petroleum, as well as in its processing, the indi-vidual operations may be disturbed by microbial contamination. The growth of microorganisms in oils requires the presence of water, a source of nitrogen, and necessary trace elements. These growth prerequisites 10 are met in most of the oil fields now being exploited. For example, in the case of offshore recovery, undesirable microorganisms are transferred to the oil well through drilling and also through the injection of large quantities of sea water. These microorganisms, or their metabolites, can lead to trouble in conveyance of the oil, e.g., plugging of pipelines, 15 gas formation, or corrosion of installations.
For inhibiting the growth of such microorganisms, biocides such as glutaraldehyde, acrolein, or quaternary ammonium compounds (quats) are used. However, these disinfectants exhibit certain drawbacks, such as substantivity to the surface or resinification. Suitable biocides for 20 use in oilwell drilling must be ecologically inoffensive, cover a broad microbial spectrum, be effective in low concentrations, not act selec-tively, and have adequate stability at the temperatures of use. Further-more, the biocides should not cause any corrosion, and they should be easy to handle and inexpensive. The prior art agents can lead to unde-25 sirable flow losses, to sedimentation, and even to blockages, constitut-ing serious disturbances of operations.
It is an object of this invention to provide an improved method of disinfecting petroleum and petroleum products whereby the microorganisms can be effectively combated without the aforementioned drawbacks.
3U To this end, in the method according to the present invention, a microbiocidal amount of propylene oxide is added to the crude oil or to the petroleum products.
35~67 In this method of disinfection, the propylene oxide is generallymixed with an inert carrier in a suitable concentration, so that safe handling of the agent is ensured~
Owing to their compatibility with the chemicals used in the petro-leum industry and with the petroleum itself, propylene oxide and the pre-ferred carrier materials can be quantitatively regulated and applied sat-isfactorily in all stages of processing.
The disinfecting method according to this invention can be applied not only in drilling for oil but also in further process stages and in 10 the storage of petroleum products. The presence of water, in particular, makes petroleum and petroleum products susceptible to microorganisms.
The method is therefore especially suitable for petroleum and petroleum products with which water is also present. Thus it is possible, for ex-ample, to convey the propylene oxide into the oil well by means of the 15 water at the time of completion. Microorganisms in the water are thereby already combated during such conveyance and cannot contaminate the oil if a minimum concentration of propylene oxide is maintained. Through the contact between the petroleum and the water containing the propylene ox-ide, part of the propylene oxide passes into the petroleum, where it can 20 likewise develop its biocidal activity.
The propylene oxide is preferably applied in a quantity such that the system to be disinfected exhibits a propylene oxide concentration of 15-20 ppm. Suitable carrier materials for such application are light kerosene, polyether compounds such as nonylphenol polyglycol ether having 25 10 units of ethylene oxide or fatty alcohol polyglycol ether having 12-16 carbons in the alcohol portion and 10-12 units of ethylene oxide, water, or mixtures thereof. In addition, anion-active, cation-active, and am-photeric emulsion systems are also suitable.
The following examples represent preferred embodiments of formula-30 tions of propylene oxide as may be utili~ed in the method of the presentinvention.
3 2857'1f.7 Example 1 A mixture of the following components is prepared:
15 parts by weight of propylene oxide, 50 parts by weight of light kerosene, and 35 parts by weight of nonylphenol polyglycol ether having 10 units of ethylene oxide.
This mixture is suitable for use in water-in-oil or oil-in-water systems. Effective disinfection of the systems is achieved when the propylene oxide concentration is 5-20 ppm.
Example 2 The following components are mixed:
20 parts by weight of propylene oxide, 40 parts by weight of white spirit, and 40 parts by weight of fatty alcohol polyglycol ether having 12-16 carbons in the alcohol portion and 10-12 units of ethylene oxide.
For disinfecting a mixture of oil and water, this formulation is 20 added in a concentration such that a propylene oxide concentration of 5-20 ppm results.
The mixture ob-tained is put into a pressure-metering pump system in the pipe sys-tem to be treated. The rate of flow is adjusted so that the concentration of propylene oxide in the system to be disinfected is at 25 least 5-20 ppm. This results in excellen-t disinfection. ethylene oxide can likewise be used as the disinfectant in the same way and with the same effect. Owing to its physical properties, however, this substance has disadvantages in handling as compared with propylene oxide.
The following table illustrates the method of disinfection accord-ing to the invention as applied to an oil emulsion contaminated with mi-croorganisms. Similar contaminated oil emulsions treated with glutaral-dehyde, on the one hand, and untreated contaminated oil emulsions, on the other hand, are used for purposes of comparison.
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The biocide utilized in the present invention as compared with prior art biocides utilized in drilling for petroleum.
The following biocides are used for disinfecting water-circulation systems in drilling for petroleum (e.g., drilling fluids). At the pres-ent time, only a limited number of chemicals are employed in the field of petroleum recovery and processing.
The best known of these are:
Biocide Concentration in ppm 10 Isothiazoline 15- 30 Glutaraldehyde 25-100 Aliphatic amines 50-110 Quaternary ammonium compounds 50-100 Acrolein 5- 15 15 Dibromonitrilopropionamide30- 80 Propylene oxide (according to the 5- 10 present invention) In an article entitled, "Biocide testing against corrosion-causing oil-field bacteria helps control plugging," by I. Ruseska et al., pub-20 lished in the March 8, 1982, edition of Oil & Gas Journal, it was demon-strated -that suitable ac-tive biocides must be capable of penetrating bio-films in order -to destroy microorganisms. The pipes are generally cov-ered by the "glycocalyx," an anionic polysacccharide matrix, and the mi-croorganisms are embedded in this matrix. This means that the active bi-25 ocidal component must be soluble in polar and apolar systems. An activesubstance which is soluble only in water influences only the rate of growth of non-sessile bacteria but has no effect in combating sessile bacteria such as sulfate-reducing bacteria (SRB type).
The results of a screening test are listed in the following 30 Table II. The tests were carried out with a Robbins Device as de-scribed in an article entitled, "Observations on biofilm formation," by W. I. McCoy, et al., published in the Canadian Journal of Microbiology, Vol. 27, 1981, pp. 910-917.
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This invention relates to methods of disinfection, and more partic-ularly to a method of disinfecting petroleum and petroleum products, es-pecially for inhibiting the growth of microorganisms capable of living therein. The method is well suited for application in drilling for petroleum.
In exploring for petroleum, as well as in its processing, the indi-vidual operations may be disturbed by microbial contamination. The growth of microorganisms in oils requires the presence of water, a source of nitrogen, and necessary trace elements. These growth prerequisites 10 are met in most of the oil fields now being exploited. For example, in the case of offshore recovery, undesirable microorganisms are transferred to the oil well through drilling and also through the injection of large quantities of sea water. These microorganisms, or their metabolites, can lead to trouble in conveyance of the oil, e.g., plugging of pipelines, 15 gas formation, or corrosion of installations.
For inhibiting the growth of such microorganisms, biocides such as glutaraldehyde, acrolein, or quaternary ammonium compounds (quats) are used. However, these disinfectants exhibit certain drawbacks, such as substantivity to the surface or resinification. Suitable biocides for 20 use in oilwell drilling must be ecologically inoffensive, cover a broad microbial spectrum, be effective in low concentrations, not act selec-tively, and have adequate stability at the temperatures of use. Further-more, the biocides should not cause any corrosion, and they should be easy to handle and inexpensive. The prior art agents can lead to unde-25 sirable flow losses, to sedimentation, and even to blockages, constitut-ing serious disturbances of operations.
It is an object of this invention to provide an improved method of disinfecting petroleum and petroleum products whereby the microorganisms can be effectively combated without the aforementioned drawbacks.
3U To this end, in the method according to the present invention, a microbiocidal amount of propylene oxide is added to the crude oil or to the petroleum products.
35~67 In this method of disinfection, the propylene oxide is generallymixed with an inert carrier in a suitable concentration, so that safe handling of the agent is ensured~
Owing to their compatibility with the chemicals used in the petro-leum industry and with the petroleum itself, propylene oxide and the pre-ferred carrier materials can be quantitatively regulated and applied sat-isfactorily in all stages of processing.
The disinfecting method according to this invention can be applied not only in drilling for oil but also in further process stages and in 10 the storage of petroleum products. The presence of water, in particular, makes petroleum and petroleum products susceptible to microorganisms.
The method is therefore especially suitable for petroleum and petroleum products with which water is also present. Thus it is possible, for ex-ample, to convey the propylene oxide into the oil well by means of the 15 water at the time of completion. Microorganisms in the water are thereby already combated during such conveyance and cannot contaminate the oil if a minimum concentration of propylene oxide is maintained. Through the contact between the petroleum and the water containing the propylene ox-ide, part of the propylene oxide passes into the petroleum, where it can 20 likewise develop its biocidal activity.
The propylene oxide is preferably applied in a quantity such that the system to be disinfected exhibits a propylene oxide concentration of 15-20 ppm. Suitable carrier materials for such application are light kerosene, polyether compounds such as nonylphenol polyglycol ether having 25 10 units of ethylene oxide or fatty alcohol polyglycol ether having 12-16 carbons in the alcohol portion and 10-12 units of ethylene oxide, water, or mixtures thereof. In addition, anion-active, cation-active, and am-photeric emulsion systems are also suitable.
The following examples represent preferred embodiments of formula-30 tions of propylene oxide as may be utili~ed in the method of the presentinvention.
3 2857'1f.7 Example 1 A mixture of the following components is prepared:
15 parts by weight of propylene oxide, 50 parts by weight of light kerosene, and 35 parts by weight of nonylphenol polyglycol ether having 10 units of ethylene oxide.
This mixture is suitable for use in water-in-oil or oil-in-water systems. Effective disinfection of the systems is achieved when the propylene oxide concentration is 5-20 ppm.
Example 2 The following components are mixed:
20 parts by weight of propylene oxide, 40 parts by weight of white spirit, and 40 parts by weight of fatty alcohol polyglycol ether having 12-16 carbons in the alcohol portion and 10-12 units of ethylene oxide.
For disinfecting a mixture of oil and water, this formulation is 20 added in a concentration such that a propylene oxide concentration of 5-20 ppm results.
The mixture ob-tained is put into a pressure-metering pump system in the pipe sys-tem to be treated. The rate of flow is adjusted so that the concentration of propylene oxide in the system to be disinfected is at 25 least 5-20 ppm. This results in excellen-t disinfection. ethylene oxide can likewise be used as the disinfectant in the same way and with the same effect. Owing to its physical properties, however, this substance has disadvantages in handling as compared with propylene oxide.
The following table illustrates the method of disinfection accord-ing to the invention as applied to an oil emulsion contaminated with mi-croorganisms. Similar contaminated oil emulsions treated with glutaral-dehyde, on the one hand, and untreated contaminated oil emulsions, on the other hand, are used for purposes of comparison.
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_, E 3 .~ 111111111111 +' S i -~ +++++i U~3 S ++ +
+ +
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The biocide utilized in the present invention as compared with prior art biocides utilized in drilling for petroleum.
The following biocides are used for disinfecting water-circulation systems in drilling for petroleum (e.g., drilling fluids). At the pres-ent time, only a limited number of chemicals are employed in the field of petroleum recovery and processing.
The best known of these are:
Biocide Concentration in ppm 10 Isothiazoline 15- 30 Glutaraldehyde 25-100 Aliphatic amines 50-110 Quaternary ammonium compounds 50-100 Acrolein 5- 15 15 Dibromonitrilopropionamide30- 80 Propylene oxide (according to the 5- 10 present invention) In an article entitled, "Biocide testing against corrosion-causing oil-field bacteria helps control plugging," by I. Ruseska et al., pub-20 lished in the March 8, 1982, edition of Oil & Gas Journal, it was demon-strated -that suitable ac-tive biocides must be capable of penetrating bio-films in order -to destroy microorganisms. The pipes are generally cov-ered by the "glycocalyx," an anionic polysacccharide matrix, and the mi-croorganisms are embedded in this matrix. This means that the active bi-25 ocidal component must be soluble in polar and apolar systems. An activesubstance which is soluble only in water influences only the rate of growth of non-sessile bacteria but has no effect in combating sessile bacteria such as sulfate-reducing bacteria (SRB type).
The results of a screening test are listed in the following 30 Table II. The tests were carried out with a Robbins Device as de-scribed in an article entitled, "Observations on biofilm formation," by W. I. McCoy, et al., published in the Canadian Journal of Microbiology, Vol. 27, 1981, pp. 910-917.
~285767 l,q ~I N
____________________________ x ~¦ ¦ ~ I l I
ta 01 1~ 1 1 C~ O--~--------------------------------_____________ 0 L, N _________ _________ ___________ O 0 ~1 ID ~1 ,~N N N
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~ ~ ~ S llD ~D ~ 00t:O t)l) ~ ~1 E
V~ ~ ~ N O O O O O v O V V
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I,q ~1 3 ~ 0 (D ~ ~0 1-) N Ll~ O G) ~: .,~ S ~ 0 ~ 0 ~ O O
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,~~ 01` ~0 1~ ~O (~) ~ ~0 oD (~
~ ~ 0 bO 0~ ~0 ~0 O _O
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~ ~ ~U N ~I N _________ ___________ O
C O ~ ~ S 0 0 ~ 0 ~ ~ 1~ ~ 0 11 ,-13 D ~D O O O O O O O O O
C C U~ o ~1 ~ ~1 ~ ~1 _1 ~1 ~ ~1 E
~ '' C>*. ___ _________ _________ ___________ D E . N N N
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,1 r,q ol H 0H O ~1 ~) I o 0 o 0 o 0 I h X S h X S h X sl ~ =~ ~~ ~ I C a~ C a) ~ I ~ 0 3 ~ 0 3 ~ 0 31 _9_
Claims (7)
1. In a method of disinfecting crude petro-leum in drilling for petroleum, particularly for inhibiting the growth of microorganisms capable of living therein to avoid disturbing exploration due -to microbial contamination, the improvement comprising the step of adding to the petroleum a microbiocidal amount of propylene oxide, by injecting water comprising propylene oxide in an amount which is sufficient to produce a concentration of 5 to 20 ppm of propylene oxide when coming into contact with petroleum in the region of application.
2. The method of Claim 1, wherein the water comprises additionally an inert carrier.
3. The method of Claim 2, wherein the inert carrier contains a mixture of light kerosene and nonylphenol polyglycol ether having 10 units of ethylene oxide.
4. The method of claim 2, wherein the inert carrier contains a mixture of white spirit and C12-16-fatty alcohol polyglycol ether having 10-12 units of ethylene oxide.
5. The method of Claim 2, wherein the inert carrier is an anion-active, cation-active, or amphoteric emulsion system.
6. The method of Claim 1, wherein the water comprises propylene oxide in such an amount that its concentration in the petroleum is about 15 to 20 ppm.
7. The method of Claim 1, wherein the petroleum is disinfected in offshore drilling.
Applications Claiming Priority (2)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CH5852/84 | 1984-12-10 | ||
| CH585284 | 1984-12-10 |
Publications (1)
| Publication Number | Publication Date |
|---|---|
| CA1285767C true CA1285767C (en) | 1991-07-09 |
Family
ID=4300382
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| CA000497210A Expired - Fee Related CA1285767C (en) | 1984-12-10 | 1985-12-09 | Method of disinfecting petroleum and petroleum products |
Country Status (8)
| Country | Link |
|---|---|
| US (1) | US5000918A (en) |
| EP (1) | EP0185612A1 (en) |
| JP (1) | JPS61140503A (en) |
| CA (1) | CA1285767C (en) |
| DK (1) | DK165186B (en) |
| ES (1) | ES8800326A1 (en) |
| FI (1) | FI854772A (en) |
| NO (1) | NO163437C (en) |
Families Citing this family (9)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US5171454A (en) * | 1991-08-19 | 1992-12-15 | Betz Laboratories, Inc. | Methods for inhibiting the production of acid in acid mine waters |
| US5128051A (en) * | 1991-09-30 | 1992-07-07 | Union Carbide Chemicals & Plastics Technology Corporation | Method for the control of biofouling |
| DE4340665A1 (en) * | 1993-11-30 | 1995-06-01 | Stockhausen Chem Fab Gmbh | Oil-in-water emulsions to replace microbicides (biocides) in water-bearing systems |
| US5749203A (en) * | 1994-09-23 | 1998-05-12 | Kimberly-Clark Corporation | Method of packaging a medical article |
| US6461563B1 (en) * | 2000-12-11 | 2002-10-08 | Advanced Materials Technologies Pte. Ltd. | Method to form multi-material components |
| US6800101B2 (en) * | 2001-10-18 | 2004-10-05 | Chevron U.S.A. Inc. | Deactivatable biocides for hydrocarbonaceous products |
| CN1297626C (en) * | 2003-12-22 | 2007-01-31 | 吐哈石油勘探开发指挥部技术监测中心 | Anticorrosion preservative agent special for sleeve for oilfield well drilling and well cementing |
| US20100242341A1 (en) * | 2007-12-20 | 2010-09-30 | Tinetti Sheila M | Corrosion and microbial control in hydrocarbonaceous compositions |
| KR20110013398A (en) * | 2008-05-15 | 2011-02-09 | 엥거스 케미칼 캄파니 | Improved corrosion and microbial control in hydrocarbonaceous compositions |
Family Cites Families (10)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US2680058A (en) * | 1948-04-27 | 1954-06-01 | Texaco Development Corp | Preservation of petroleum in storage |
| US3256143A (en) * | 1961-11-06 | 1966-06-14 | M & T Chemicals Inc | Controlling gram negative bacteria with n-propyl ten halides and oxides |
| US3169906A (en) * | 1961-11-16 | 1965-02-16 | Norwich Pharma Co | Method of sterilizing with alkylene oxide |
| US3624213A (en) * | 1963-10-30 | 1971-11-30 | Merck & Co Inc | Method of sterilizing aqueous pharmaceutical solutions employing propylene oxide and entrained air |
| US4200634A (en) * | 1978-03-13 | 1980-04-29 | Petrolite Corporation | Sulfone containing quaternary ammonium derivatives of 1,4-thiazines as microbiocides |
| US4200633A (en) * | 1978-03-13 | 1980-04-29 | Petrolite Corporation | Thioether containing quaternary ammonium derivatives of 1,4-thiazines as microbiocides |
| ZA802875B (en) * | 1979-05-17 | 1981-12-30 | Unilever Ltd | Process for making detergent compositions |
| JPS5799507A (en) * | 1980-12-13 | 1982-06-21 | Katayama Chem Works Co Ltd | Industrial bactericidal and bacteriostatic composition |
| DE3266571D1 (en) * | 1981-11-06 | 1985-10-31 | Ciba Geigy Ag | Use of mono- and dibromodicyanomethane as a pesticide, and pesticides containing these compounds |
| US4552752A (en) * | 1983-01-31 | 1985-11-12 | Rohm And Haas Company | Microbiocidal article for aqueous systems |
-
1985
- 1985-11-11 EP EP85810525A patent/EP0185612A1/en not_active Withdrawn
- 1985-12-02 FI FI854772A patent/FI854772A/en not_active Application Discontinuation
- 1985-12-06 JP JP60273537A patent/JPS61140503A/en active Pending
- 1985-12-09 CA CA000497210A patent/CA1285767C/en not_active Expired - Fee Related
- 1985-12-09 ES ES549736A patent/ES8800326A1/en not_active Expired
- 1985-12-09 NO NO854945A patent/NO163437C/en unknown
- 1985-12-09 DK DK569585A patent/DK165186B/en not_active Application Discontinuation
-
1987
- 1987-08-28 US US07/090,460 patent/US5000918A/en not_active Expired - Fee Related
Also Published As
| Publication number | Publication date |
|---|---|
| ES549736A0 (en) | 1987-10-16 |
| FI854772A (en) | 1986-06-11 |
| NO163437C (en) | 1990-05-30 |
| DK569585D0 (en) | 1985-12-09 |
| NO163437B (en) | 1990-02-19 |
| ES8800326A1 (en) | 1987-10-16 |
| NO854945L (en) | 1986-06-11 |
| FI854772A0 (en) | 1985-12-02 |
| DK569585A (en) | 1986-06-11 |
| JPS61140503A (en) | 1986-06-27 |
| EP0185612A1 (en) | 1986-06-25 |
| US5000918A (en) | 1991-03-19 |
| DK165186B (en) | 1992-10-19 |
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