WO1996017888A1 - Bioabbaubare thermoplastisch verformbare materialien und verpackungen daraus - Google Patents
Bioabbaubare thermoplastisch verformbare materialien und verpackungen daraus Download PDFInfo
- Publication number
- WO1996017888A1 WO1996017888A1 PCT/DE1995/001732 DE9501732W WO9617888A1 WO 1996017888 A1 WO1996017888 A1 WO 1996017888A1 DE 9501732 W DE9501732 W DE 9501732W WO 9617888 A1 WO9617888 A1 WO 9617888A1
- Authority
- WO
- WIPO (PCT)
- Prior art keywords
- packaging
- biodegradable
- materials according
- biodegradable thermoplastic
- thermoplastic materials
- Prior art date
Links
Classifications
-
- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08L—COMPOSITIONS OF MACROMOLECULAR COMPOUNDS
- C08L3/00—Compositions of starch, amylose or amylopectin or of their derivatives or degradation products
- C08L3/04—Starch derivatives, e.g. crosslinked derivatives
- C08L3/06—Esters
-
- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08L—COMPOSITIONS OF MACROMOLECULAR COMPOUNDS
- C08L69/00—Compositions of polycarbonates; Compositions of derivatives of polycarbonates
-
- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08L—COMPOSITIONS OF MACROMOLECULAR COMPOUNDS
- C08L71/00—Compositions of polyethers obtained by reactions forming an ether link in the main chain; Compositions of derivatives of such polymers
- C08L71/02—Polyalkylene oxides
-
- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08L—COMPOSITIONS OF MACROMOLECULAR COMPOUNDS
- C08L2201/00—Properties
- C08L2201/06—Biodegradable
Definitions
- the invention relates to thermoplastically deformable materials made from biodegradable polymer blends in the form of granules. Moldings, extrudates. Foils etc. based on a blend consisting of starch esters, polyalkylene glycols and other biologically compatible additives, its use, as well as packaging made from the biodegradable thermoplastic materials.
- this embrittlement can be prevented by modifying starch esters with a degree of substitution ⁇ 3, preferably 1.8 to 2.6, using polyethylene glycol (PEG).
- PEG polyethylene glycol
- DE-OS 44 18 678 it is possible to add aliphatic, saturated or unsaturated dicarboxylic acids and / or oxidicarboxylic acids and / or oxitricarboxylic acids to increase the melt stabilization of blends from starch esters with a degree of substitution ⁇ 3 and polyalkylene glycols and to improve their biodegradability.
- Packaging for cigarettes and other tobacco products are made in a variety of different materials, e.g. Pouch bag.
- Cans and cap boxes made of aluminum, sheet metal, cardboard or plastic are known.
- the most widespread packaging for cigarettes is the cap box (hinged-lid packs) according to DBP 34 14 214 (US Patent 53 79 889).
- the required protection of the contents is achieved through a multi-layer combination of different materials. It often consists of an inner wrap made of laminated or printed aluminum foil, a cardboard or paper wrap mostly printed with markings and an outer closed wrapping made of thermally weldable foil e.g. made of polypropylene (DE-OS 30 27 448, DE-OS 2844 238).
- Other packaging for cigarettes achieve the required protection of the contents against deformation, aroma and
- packaging has also been described which consists exclusively of foils made of thermoplastic (DE-OS 42 26 640).
- thermoplastic films used for cigarette packaging In order to improve the mechanical properties and the gas and water vapor impermeability of the thermoplastic films used for cigarette packaging, they become biaxial Stretch-oriented, optionally metallized, plastic films made of polypropylene or polyalkylene terephthalate are used (DE-OS 36 32 376. EP 454 003, EP 317 818).
- the disadvantages of all these solutions are that they only allow the protection of the filling material and the water vapor and gas tightness if materials are selected which consist at least of an aluminum foil, tinfoil or a biaxially stretched plastic film.
- the necessary markings are usually printed on a cardboard, sheet metal or paper cover used in the combination.
- the packaging After use, the packaging usually ends up in the waste, thus contributing to existing environmental problems. They only rot very slowly or not at all in landfills and in the wild under the influence of the weather. For their reprocessing in the usual recycling processes, a material separation must first take place. This is i. a. only possible incompletely. The processes are also sustainable, e.g. disrupted by contamination of the process water. The packaging cannot be reused for food law reasons.
- the object of the invention is. the features of DE-OS 43 26 118 and DE-OS 44 18 687 by improving the water stability, the mechanical parameters and the barrier properties of the blends to make it more advantageous and to develop packaging for goods of different types, which consist of single or multilayer film layers therrao plastic materials that can be produced without high technical effort, are lightweight, have good barrier properties against water vapor and gases without additional equipment or aftertreatment, are printable, but also have complete biodegradability, can be recycled and can be sent to a technical recycling process and when brought in usual recycling processes will not interfere.
- the blends according to the invention consist of starch esters, predominantly starch acetate, with a degree of substitution ⁇ 3, preferably from 1.8-2.6 and polyalkylene glycols (PAG) with a molar mass of 200-1000 g / mol, preferably from 200 to 600 g / mol with or without the addition of saturated dicarboxylic acids and / or oxidicarboxylic acids and / or oxi tricarboxylic acids with 2 to 10 carbon atoms in a ratio of 100: 2 to 1000: 1 starch ester to polyfunctional carboxylic acid, compounded with aliphatic polycarbonates and plasticizers as well as usual additives, especially fillers .
- PAG polyalkylene glycols
- al iphat ical polycarbonates are carbonic acid ester-containing polymers of the formula
- the use of polyethylene and polypropylene carbonate is particularly favorable.
- Aliphatic polycarbonates can also be polyalkylene co- or polyalkylene terpolymers.
- Biologically compatible compounds are preferably used as plasticizers: polyethylene glycols, mono- and
- Diesters of polyethylene glycols with C 1 -C 10 -carboxylic acids such as, for example, triethylene glycol diacetate, glycerol triacetate and trialkyl citrate.
- esters of phthalic acid with C 1 -C 10 -n-alkanols such as dimethyl phthalate, diethyl phthalate or dibutyl phthalate can be used.
- the ratio of starch acetate blend to aliphatic polycarbonates can be 5 95 to 95 5, preferably 30 70 to 70 30.
- the proportion of additives or plasticizers is 0 to 30%, preferably 0 to 15%.
- thermoplastically processable molding compounds can be used for all common processing methods, e.g. for injection molding, deep drawing, melt extrusion, etc. produce. These molding compounds are completely biodegradable and have increased water stability, good mechanical properties, in particular in the case of films, increased elongation at break and good barrier properties against gas and water vapor.
- Suitable fillers such as chalk, talc, anhvdrite or kaolin can also be added to the foils to create surfaces for advertising-effective, attractive prints.
- the preferred concentration of the fillers is 1 to 30% by mass.
- Water vapor and gases, in particular air, without aftertreatment by biaxial stretching or metal vapor deposition can in particular advantageously be designed as single-layer packaging.
- These can be ordinary sales packaging, primary packaging, transport packaging or even full packaging for a system for reusable sales packaging.
- the single-layer design of the packaging saves a great deal of effort in terms of manufacturing costs and packaging material, while still ensuring full protection of the quality of the packaged goods.
- multilayer film cuts can also be used, which can have different compositions depending on their position in the composite.
- the biodegradability or the compostability of the claimed film packaging is excellent, so that after several weeks of storage under rotting conditions, these are completely degraded.
- a particular advantage of the blends according to the invention is that fillers can be easily incorporated and, in addition to the price advantage, individual mechanical parameters can also be improved.
- ISO rods were manufactured from mixtures 1, 2, 3, 4 and 8 and their mechanical properties were examined.
- mixture 4 in particular being unsuitable for injection molding. Such mixtures are more suitable for film applications.
- Width 15 mm
- Dry blends of the mixture constituents for Examples 1 to 3 from Table 5 were processed into granules in an extruder and then extruded or blown into films.
- Table 6 shows the mechanical measured values and the permeation properties of the films.
- Foil cuts from material compositions according to d # n Examples 1 to 3 are easy to weld.
- the measured strength properties of the films document that they are outstandingly suitable for tobacco products, in particular for cigarette packaging, and protect the pack inhal t from damage during transport, storage and handling.
- the measured permeation values were achieved without a biaxial stretching of the films.
- empty packaging casings of the above-mentioned compositions were deposited under rotting conditions in an industrial composting plant. The condition of the packaging was checked weekly and the time after which the morphology of the film cut was no longer recognizable. (Table 7)
- Fig. 1 is a cigarette pack with an inner
- Fig. 2 shows a cigarette pack from a single layer
- FIG. 3 shows a cigarette packet made of cardboard material which is laminated with the material according to the invention
- FIG. 4 shows a cross section through the material of the packet of
- an inner packaging 10 is in the form of a conventional one
- Cigarette box made of cardboard material provided.
- the cardboard material consists of cellulose-containing material, in particular conventional cardboard. Such material has a relatively high vapor permeability.
- the inner packaging 10 completely encloses the cigarettes contained therein. It has a conventional separating seam 12 or cutting seam in order to be able to lift off the cover 13, which is designed in the manner of an upper cap.
- the inner packaging 10 has an outer packaging 11 made of the material according to the invention explained above
- the outer packaging 11 consists of a thin, preferably clear film, which around the Inner packaging 10 is wrapped around and forms a wrap 14 along one narrow side.
- the outer packaging 11 is closed by folding 15 on the end faces. Furthermore, there is a circumferential on the outer packaging 11
- Tear tape 16 is provided, which is limited by two lines of weakness 17. After tearing off the tear tape 16, the upper cap part of the outer packaging 11 can be removed, so that the inner packaging 10 for opening the
- Outer packaging 11 can be sealed in a vapor-tight manner.
- the cigarette packaging is designed as a single-substance packaging 20, which is made from the material according to the invention
- the single material packaging 20 is also of rectangular shape here.
- Packaging material is placed on top of one another by folding 22, the layers lying one above the other being sealed.
- an integrated tear strip 23 is provided, which is delimited by lines of weakness 24 and runs around the packaging near one end wall.
- Packing 30 is also a one-pack, but is made of two layers and a cardboard mat rial 31, which is laminated with the film 32 of the invention.
- the outer shape of the packaging 30 is identical to the outer shape of the single-substance packaging 20 of the exemplary embodiment from FIG. 2.
Landscapes
- Chemical & Material Sciences (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Medicinal Chemistry (AREA)
- Polymers & Plastics (AREA)
- Organic Chemistry (AREA)
- Health & Medical Sciences (AREA)
- Wrappers (AREA)
- Compositions Of Macromolecular Compounds (AREA)
- Laminated Bodies (AREA)
- Absorbent Articles And Supports Therefor (AREA)
- Orthopedics, Nursing, And Contraception (AREA)
- Sealing Material Composition (AREA)
- Table Devices Or Equipment (AREA)
- Addition Polymer Or Copolymer, Post-Treatments, Or Chemical Modifications (AREA)
- Biological Depolymerization Polymers (AREA)
Abstract
Description
Claims
Priority Applications (7)
Application Number | Priority Date | Filing Date | Title |
---|---|---|---|
EP95940136A EP0796294B1 (de) | 1994-12-07 | 1995-12-06 | Bioabbaubare thermoplastisch verformbare materialien und verpackungen daraus |
KR1019970703739A KR100310740B1 (ko) | 1994-12-07 | 1995-12-06 | 생분해성열가소성물질및이들로부터제조된포장재 |
JP8517243A JPH10510853A (ja) | 1994-12-07 | 1995-12-06 | 生分解性の熱可塑性成形材料およびそれより成る包装材料 |
PL95320672A PL184210B1 (pl) | 1994-12-07 | 1995-12-06 | Termoplastycznie odkształcalne materiały opakowaniowe ulegające biodegradacji |
DE59506856T DE59506856D1 (de) | 1994-12-07 | 1995-12-06 | Bioabbaubare thermoplastisch verformbare materialien und verpackungen daraus |
US08/860,427 US5936014A (en) | 1994-12-07 | 1995-12-06 | Biodegradable deformable thermoplastic materials and packages made thereof |
MXPA/A/1997/004046A MXPA97004046A (en) | 1994-12-07 | 1997-06-02 | Biodegradable thermoplastic materials and packaging of mis |
Applications Claiming Priority (4)
Application Number | Priority Date | Filing Date | Title |
---|---|---|---|
DEP4443539.8 | 1994-12-07 | ||
DE19944443539 DE4443539A1 (de) | 1994-12-07 | 1994-12-07 | Bioabbaubare thermoplastisch verformbare Materialien |
DE19519495.0 | 1995-05-27 | ||
DE1995119495 DE19519495A1 (de) | 1995-05-27 | 1995-05-27 | Verpackung aus thermoplastischem Werkstoff mit vollständiger biologischer Abbaubarkeit, vorzugsweise für Tabakwaren |
Publications (1)
Publication Number | Publication Date |
---|---|
WO1996017888A1 true WO1996017888A1 (de) | 1996-06-13 |
Family
ID=25942641
Family Applications (1)
Application Number | Title | Priority Date | Filing Date |
---|---|---|---|
PCT/DE1995/001732 WO1996017888A1 (de) | 1994-12-07 | 1995-12-06 | Bioabbaubare thermoplastisch verformbare materialien und verpackungen daraus |
Country Status (9)
Country | Link |
---|---|
US (1) | US5936014A (de) |
EP (1) | EP0796294B1 (de) |
JP (1) | JPH10510853A (de) |
KR (1) | KR100310740B1 (de) |
AT (1) | ATE184620T1 (de) |
CA (1) | CA2206668A1 (de) |
DE (1) | DE59506856D1 (de) |
PL (1) | PL184210B1 (de) |
WO (1) | WO1996017888A1 (de) |
Cited By (6)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
WO1998007782A1 (de) * | 1996-08-20 | 1998-02-26 | Buna Sow Leuna Olefinverbund Gmbh | Bioabbaubare thermoplastisch verformbare materialien für lebensmittelverpackungen |
DE19830775A1 (de) * | 1998-07-09 | 2000-01-13 | Buna Sow Leuna Olefinverb Gmbh | Thermoplastisch verarbeitbare Formmassen auf Basis von Stärkeestern und Naturfaserkomponenten und Verfahren zu deren Herstellung |
EP1072657A1 (de) * | 1999-07-16 | 2001-01-31 | National Starch and Chemical Investment Holding Corporation | Beschichtungen auf Basis von Stärkeestern |
DE102010012386A1 (de) | 2010-03-22 | 2011-09-22 | Jörg Beckmann | Verfahren zur Herstellung eines polymeren Kunststoffs sowie ein damit hergestelltes Erzeugnis |
EP3307648B1 (de) | 2015-06-09 | 2020-02-19 | K-fee System GmbH | Portionskapsel, system und verfahren zur herstellung eines getränks |
RU2796759C1 (ru) * | 2022-05-11 | 2023-05-29 | Общество с ограниченной ответственностью "Гринбиотех" | Модифицированный термопластичный органический материал и способ его получения |
Families Citing this family (15)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
CA2328628A1 (en) * | 1999-12-21 | 2001-06-21 | Cecile J. Schoenheider | Moldable compositions |
JP2001180741A (ja) * | 1999-12-27 | 2001-07-03 | Toppan Printing Co Ltd | オーバーラップ包装体 |
US8698262B2 (en) * | 2004-09-14 | 2014-04-15 | Semiconductor Energy Laboratory Co., Ltd. | Wireless chip and manufacturing method of the same |
CA2647358A1 (en) * | 2005-03-24 | 2006-09-28 | Madrisano Catinari | Biodegradable plastic material |
US8853386B2 (en) * | 2006-12-18 | 2014-10-07 | Celanese Acetate Llc | Starch esters, methods of making same, and articles made therefrom |
DE102007038473C5 (de) * | 2007-08-14 | 2013-11-07 | Huhtamaki Films Germany Gmbh & Co. Kg | Folienanordnung, Verfahren zu deren Herstellung und Verwendung |
FR2937040B1 (fr) * | 2008-10-13 | 2012-07-27 | Roquette Freres | Compositions thermoplastiques ou elastomeriques a base d'esters d'une matiere amylacee et procede de preparation de telles compositions |
FR2937039B1 (fr) * | 2008-10-13 | 2011-11-18 | Roquette Freres | Compositions elastomeriques a base d'esters d'une matiere amylacee et procede de preparation de telles compositions |
BR112012004887A2 (pt) * | 2009-09-03 | 2019-09-24 | Co2Starch Pty Ltd | composição de polimero amido termoplastico |
WO2012043817A1 (ja) * | 2010-09-30 | 2012-04-05 | 積水化学工業株式会社 | 合わせガラス用中間膜及び合わせガラス |
CN102020838A (zh) * | 2010-11-11 | 2011-04-20 | 中山大学 | 一种可完全降解的聚甲基乙撑碳酸酯共混材料及其制备方法 |
KR101805103B1 (ko) * | 2010-11-19 | 2018-01-10 | 에스케이씨 주식회사 | 환경친화형 다층 필름 |
KR101902281B1 (ko) * | 2011-05-19 | 2018-09-28 | 에스케이이노베이션 주식회사 | 수지 조성물용 가소제 및 이를 포함하는 수지 조성물 |
CN102943416B (zh) * | 2012-10-17 | 2014-12-24 | 云南瑞升烟草技术(集团)有限公司 | 一种具有高阻隔性能的易降解卷烟内衬纸 |
WO2021117937A1 (ko) * | 2019-12-12 | 2021-06-17 | 이문희 | 아밀로펙틴을 포함하는 생분해성 고분자 조성물 및 그의 제조방법 |
Citations (3)
Publication number | Priority date | Publication date | Assignee | Title |
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US4137280A (en) * | 1978-04-19 | 1979-01-30 | Air Products And Chemicals, Inc. | Polyalkylene carbonates as processing aids for polyvinyl chloride |
JPH0539412A (ja) * | 1991-08-02 | 1993-02-19 | Calp Corp | 分解性樹脂組成物 |
WO1994007953A1 (en) * | 1992-10-07 | 1994-04-14 | Parke, Davis & Company | Starch ester blends with linear polyesters |
Family Cites Families (13)
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DE2844238C2 (de) * | 1978-10-11 | 1984-08-23 | Focke & Co, 2810 Verden | Packung, insbesondere Zigaretten-Packung, aus Verbundfolie sowie Vorrichtung zum Herstellen von Reißlinien in einer Verbundfolie |
DE3027448A1 (de) * | 1980-07-19 | 1982-02-18 | Focke & Co, 2810 Verden | Weichpackung fuer zigaretten sowie zuschnitt, verfahren und vorrichtung zum herstellen derselben |
US4405731A (en) * | 1982-01-12 | 1983-09-20 | Mobay Chemical Corporation | Polycarbonate-starch compositions |
DE3263716D1 (en) * | 1982-02-27 | 1985-06-27 | Tabac Fab Reunies Sa | Apparatus in a cigarette packing machine for transferring stamped and prefolded inner collars of a cigarette box |
DE3414214A1 (de) * | 1984-04-14 | 1985-10-24 | Maschinenfabrik Fr. Niepmann GmbH u. Co, 5820 Gevelsberg | Verpackung fuer laengliche gegenstaende, insbesondere zigaretten oder zigarillos |
DE3632376A1 (de) * | 1986-09-24 | 1988-03-31 | Hoechst Ag | Verwendung einer metallisierten, biaxial streckorientierten, opaken kunststoffolie |
US4807745A (en) * | 1987-11-27 | 1989-02-28 | R. J. Reynolds Tobacco Company | Barrier sealed packages for cigarettes and other smoking articles |
CA2039970C (en) * | 1990-04-23 | 1998-12-08 | Carl C. Hein, Iii | High barrier packages for smoking articles and other products |
DE4114185C1 (de) * | 1991-04-30 | 1993-02-04 | Battelle-Institut E.V., 6000 Frankfurt, De | |
DE4226640A1 (de) * | 1992-08-12 | 1994-02-17 | Hoechst Ag | Zigarettenverpackung aus Kunststoffolie |
US5462983A (en) * | 1993-07-27 | 1995-10-31 | Evercorn, Inc. | Biodegradable moldable products and films comprising blends of starch esters and polyesters |
DE4326118A1 (de) * | 1993-08-04 | 1995-02-09 | Buna Gmbh | Bioabbaubare, thermoplastisch verformbare Materialien aus Stärkeestern |
US5379889A (en) * | 1993-10-22 | 1995-01-10 | R. J. Reynolds Tobacco Company | Cigarette package |
-
1995
- 1995-12-06 WO PCT/DE1995/001732 patent/WO1996017888A1/de active IP Right Grant
- 1995-12-06 AT AT95940136T patent/ATE184620T1/de not_active IP Right Cessation
- 1995-12-06 PL PL95320672A patent/PL184210B1/pl unknown
- 1995-12-06 DE DE59506856T patent/DE59506856D1/de not_active Expired - Fee Related
- 1995-12-06 JP JP8517243A patent/JPH10510853A/ja active Pending
- 1995-12-06 US US08/860,427 patent/US5936014A/en not_active Expired - Fee Related
- 1995-12-06 CA CA002206668A patent/CA2206668A1/en not_active Abandoned
- 1995-12-06 KR KR1019970703739A patent/KR100310740B1/ko not_active IP Right Cessation
- 1995-12-06 EP EP95940136A patent/EP0796294B1/de not_active Expired - Lifetime
Patent Citations (3)
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US4137280A (en) * | 1978-04-19 | 1979-01-30 | Air Products And Chemicals, Inc. | Polyalkylene carbonates as processing aids for polyvinyl chloride |
JPH0539412A (ja) * | 1991-08-02 | 1993-02-19 | Calp Corp | 分解性樹脂組成物 |
WO1994007953A1 (en) * | 1992-10-07 | 1994-04-14 | Parke, Davis & Company | Starch ester blends with linear polyesters |
Non-Patent Citations (1)
Title |
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DATABASE WPI Week 9312, Derwent World Patents Index; AN 93-096870 * |
Cited By (7)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
WO1998007782A1 (de) * | 1996-08-20 | 1998-02-26 | Buna Sow Leuna Olefinverbund Gmbh | Bioabbaubare thermoplastisch verformbare materialien für lebensmittelverpackungen |
DE19633476A1 (de) * | 1996-08-20 | 1998-02-26 | Buna Sow Leuna Olefinverb Gmbh | Bioabbaubare thermoplastisch verformbare Materialien für Lebensmittelverpackungen |
DE19830775A1 (de) * | 1998-07-09 | 2000-01-13 | Buna Sow Leuna Olefinverb Gmbh | Thermoplastisch verarbeitbare Formmassen auf Basis von Stärkeestern und Naturfaserkomponenten und Verfahren zu deren Herstellung |
EP1072657A1 (de) * | 1999-07-16 | 2001-01-31 | National Starch and Chemical Investment Holding Corporation | Beschichtungen auf Basis von Stärkeestern |
DE102010012386A1 (de) | 2010-03-22 | 2011-09-22 | Jörg Beckmann | Verfahren zur Herstellung eines polymeren Kunststoffs sowie ein damit hergestelltes Erzeugnis |
EP3307648B1 (de) | 2015-06-09 | 2020-02-19 | K-fee System GmbH | Portionskapsel, system und verfahren zur herstellung eines getränks |
RU2796759C1 (ru) * | 2022-05-11 | 2023-05-29 | Общество с ограниченной ответственностью "Гринбиотех" | Модифицированный термопластичный органический материал и способ его получения |
Also Published As
Publication number | Publication date |
---|---|
KR980700371A (ko) | 1998-03-30 |
PL320672A1 (en) | 1997-10-27 |
EP0796294A1 (de) | 1997-09-24 |
MX9704046A (es) | 1997-10-31 |
KR100310740B1 (ko) | 2001-12-17 |
PL184210B1 (pl) | 2002-09-30 |
EP0796294B1 (de) | 1999-09-15 |
US5936014A (en) | 1999-08-10 |
DE59506856D1 (de) | 1999-10-21 |
JPH10510853A (ja) | 1998-10-20 |
CA2206668A1 (en) | 1996-06-13 |
ATE184620T1 (de) | 1999-10-15 |
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