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WO1996031561B1 - Biologically degradable polymer mixture - Google Patents

Biologically degradable polymer mixture

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Publication number
WO1996031561B1
WO1996031561B1 PCT/IB1996/000275 IB9600275W WO9631561B1 WO 1996031561 B1 WO1996031561 B1 WO 1996031561B1 IB 9600275 W IB9600275 W IB 9600275W WO 9631561 B1 WO9631561 B1 WO 9631561B1
Authority
WO
WIPO (PCT)
Prior art keywords
starch
polymer mixture
polyester
mixture according
aliphatic
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.)
Ceased
Application number
PCT/IB1996/000275
Other languages
German (de)
French (fr)
Other versions
WO1996031561A1 (en
Filing date
Publication date
Priority claimed from DE1995113237 external-priority patent/DE19513237A1/en
Priority to EP96905977A priority Critical patent/EP0819147B1/en
Priority to JP08525223A priority patent/JP3107830B2/en
Priority to DE59610506T priority patent/DE59610506D1/en
Priority to US08/930,748 priority patent/US6096809A/en
Priority to AT96905977T priority patent/ATE242295T1/en
Application filed filed Critical
Priority to AU49522/96A priority patent/AU705499B2/en
Priority to DK96905977T priority patent/DK0819147T3/en
Publication of WO1996031561A1 publication Critical patent/WO1996031561A1/en
Publication of WO1996031561B1 publication Critical patent/WO1996031561B1/en
Anticipated expiration legal-status Critical
Ceased legal-status Critical Current

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Abstract

A biologically degradable polymer mixture contains at least one biopolymer made from renewable raw materials and a polymer selected from the following materials: an aromatic polyester; a polyester-copolymer with both aliphatic and aromatic blocks; a polyester amide; a polyglycol; a polyester urethane; and/or mixtures of these components.

Claims

- 28 - - 28 - GEÄNDERTE ANSPRÜCHECHANGED CLAIMS [beim Internationalen Büro am 2. October 1996 (02.10.96) eingegangen; ursprüngliche Ansprüche 1-30 durch geänderte Ansprüche 1-29 ersetzt (7 Seiten)][received at the International Bureau on 2 October 1996 (02.10.96); original claims 1-30 replaced by amended claims 1-29 (7 pages)] 1. Biologisch abbaubare Polymermischung, umfassend mindestens ein auf nachwachsenden Rohstoffen basierend hergestelltes Biopolymer, dadurch gekennzeichnet, dass als Biopolymer min¬ destens Stärke, wie vorzugsweise thermoplastische Stärke, vorliegt, und dass in der Polymermischung mindestens ein Polymer, ausgewählt aus der nachfolgenden Liste, vorgesehen ist:1. A biodegradable polymer mixture, comprising at least one based on renewable raw materials produced biopolymer, characterized in that at least as a biopolymer strength, such as preferably thermoplastic starch, is present, and that provided in the polymer blend at least one polymer selected from the list below is: - ein aromatischer Polyester,an aromatic polyester, - ein Polyester-Copolymer, aufweisend sowohl aliphatische wie auch aromatische Blöcke,a polyester copolymer comprising both aliphatic and aromatic blocks, - ein Polyesteramid,a polyesteramide, - ein Polyethylenoxidpolymer bzw. ein Polyglykol,a polyethylene oxide polymer or a polyglycol, - ein Polyesterurethan- a polyester urethane - und/oder Mischungen davon.- and / or mixtures thereof. 2. Biologisch abbaubare Polymermischung nach Anspruch 1, da¬ durch gekennzeichnet, dass die Stärke als sogenannte thermo¬ plastische Stärke vorliegt, erhalten durch im wesentlichen wasserfreies Mischen von nativer Stärke mit mindestens einem Plastifizier- oder Quellmittel in der Grössenordnung von 10 - 40 Gew.%, vorzugsweise 20 - 36 Gew.%, bezogen auf die Mischung mit nativer Stärke oder einem Derivat davon, wobei das Plastifizier- oder Quellmittel dazu geeignet ist, die Stärke bzw. das Derivat mindestens anzuquellen oder anzule¬ sen.2. Biodegradable polymer mixture according to claim 1, da¬ characterized in that the starch is present as a so-called thermo¬ plastic starch, obtained by substantially anhydrous mixing of native starch with at least one plasticizer or swelling agent in the order of 10 to 40 wt. %, preferably 20-36% by weight, based on the mixture with native starch or a derivative thereof, wherein the plasticizing or swelling agent is suitable for at least swelling or emulsifying the starch or the derivative. 3. Biologisch abbaubare Polymermischung nach Anspruch 2, da¬ durch gekennzeichnet, dass die thermoplastische Stärke als Quell- oder Plastifiziermittel mindestens eine der nachfol¬ genden Substanzen enthält: Sorbitol, Glyzerin, eine Hydroxi- säure, wie Milchsäure oder Oligomere davon und/oder deren Salze, Polyvinylalkohol, einen aliphatischer Polyester, wie vorzugsweise einen niedermolekularer aliphatischer Polyester, wie niedermolekulare Polymilchsäure oder Polycaprolacton, ein Polyesteramid, vorzugsweise ein niedermolekulares Polyeste¬ ramid und/oder Mischungen davon.3. Biodegradable polymer mixture according to claim 2, da¬ characterized in that the thermoplastic starch contains as swelling or plasticizing agent at least one of the fol lowing substances: sorbitol, glycerol, a hydroxy acid, such as lactic acid or oligomers thereof and / or their Salts, polyvinyl alcohol, an aliphatic polyester, such as preferably a low molecular weight aliphatic polyester, such as low molecular weight polylactic acid or polycaprolactone, a polyester amide, preferably a low molecular weight Polyeste¬ ramid and / or mixtures thereof. 4. Biologisch abbaubare Polymermischung nach einem der An¬ sprüche 1 - 3, dadurch gekennzeichnet, dass das Polyester-Co¬ polymer nebst Polyolen aus aromatischen oder aliphatischen Di-Carbonsäuren hergestellt ist.4. Biodegradable polymer mixture according to any one of An¬ claims 1 - 3, characterized in that the polyester Co¬ polymer together with polyols is prepared from aromatic or aliphatic di-carboxylic acids. 5. Biologisch abbaubare Polymermischung nach einem der An¬ sprüche 1 - 4, dadurch gekennzeichnet, dass das Polyester-Co¬ polymer die folgende allgemeine Struktur aufweist:5. Biodegradable polymer mixture according to one of claims 1 to 4, characterized in that the polyester copolymer has the following general structure: 0 0 O O0 0 O O H0- - (CH2)χ-0-C- (CH2) -C-0- - (CH2)χ-0-C- -C-O- H (CH2)χ-OHH0- - (CH 2) χ -0-C- (CH2) -C-0 - (CH2) χ -0-C H -CO- (CH2) χ-OH 1 m n1 m n wobei 1 und m variabel sind und einer Verteilung unterliegen sowie deren Mittelwerte sich nach der Zusammensetzung des Reaktionsgemisches richten.where 1 and m are variable and subject to a distribution and their mean values depend on the composition of the reaction mixture. 6. Biologisch abbaubare Polymermischung nach einem der An¬ sprüche 1 - 5, dadurch gekennzeichnet, dass das Polyester-Co¬ polymer durch Polykondensation von einerseits mindestens ei¬ nem Diol aus der Reihe 1,2-Ethandiol, 1,3-Propandiol, 1,4- Butandiol und/oder 1,6 Hexandiol mit andererseits mindestens einer aromatischen Di-Carbonsäure, wie beispielsweise Terephthalsäure und gegebenenfalls mindestens einer aliphati¬ schen Di-Carbonsäure, wie Adipinsäure und/oder Sebacinsäure hergestellt ist. 7. Biologisch abbaubare Polymermischung nach einem der An¬ sprüche 1 - 6, dadurch gekennzeichnet, dass das Polyester-Co¬ polymer ein Polyalkylenterephthalat oder ein Polyethylenter- ephthalat ist.6. Biodegradable polymer mixture according to any one of An¬ claims 1-5, characterized in that the polyester copolymer Co by polycondensation of on the one hand at least ei¬ nem diol from the series 1,2-ethanediol, 1,3-propanediol, 1 4-butanediol and / or 1,6-hexanediol with, on the other hand, at least one aromatic di-carboxylic acid, for example terephthalic acid and optionally at least one aliphatic di-carboxylic acid, such as adipic acid and / or sebacic acid. 7. Biodegradable polymer mixture according to one of claims 1 to 6, characterized in that the polyester copolymer is a polyalkylene terephthalate or a polyethylene terephthalate. 8. Biologisch abbaubare Polymermischung nach einem der An¬ sprüche 1 - 7, dadurch gekennzeichnet, dass als weitere Kom¬ ponente ein aliphatischer Polyester bzw. Copolyester vorgese¬ hen ist, wie beispielsweise Polymilchsäure, Polyhydroxybut- tersäure, Polyhydroxybenzoesäure, Polyhydroxybuttersäure-Hy- droxyvaleriansäure-Copolymer oder Polycaprolacton.8. Biodegradable polymer mixture according to any one of An¬ claims 1-7, characterized in that as a further Kom component an aliphatic polyester or copolyester is hen vorgese¬, such as polylactic acid, polyhydroxybutyric acid, polyhydroxybenzoic acid, polyhydroxybutyric acid hydroxyvaleriansäure Copolymer or polycaprolactone. 9. Biologisch abbaubare Polymermischung nach Anspruch 8, ge¬ kennzeichnet durch thermoplastische Stärke, mindestens ein Polyethylenterephthalat oder ein Polyalkylenterephthalat so¬ wie durch Polycaprolacton.9. Biodegradable polymer mixture according to claim 8, characterized by thermoplastic starch, at least one polyethylene terephthalate or a polyalkylene terephthalate and polycaprolactone. 10. Biologisch abbaubare Polymermischung nach einem der An¬ sprüche 1 - 9, dadurch gekennzeichnet, dass die Mischung ein Blockcopolymer als Phasenvermittler enthält, beispielsweise erhalten durch wasserfreies Mischen und Reagieren in der Schmelze von Stärke oder thermoplastischer Stärke mit minde¬ stens einem der nachfolgenden Polymeren: einem Polyester-Copolymer mit aliphatischen und aromatischen Blöcken, einem aromatischen Polyester, einem aliphatischen Polyester, einem Polyesteramid und/oder einem Polyesterurethan.10. Biodegradable polymer mixture according to any one of An¬ claims 1-9, characterized in that the mixture contains a block copolymer as a phase mediator, for example, obtained by anhydrous mixing and reacting in the melt of starch or thermoplastic starch with minde¬ least one of the following polymers a polyester copolymer having aliphatic and aromatic blocks, an aromatic polyester, an aliphatic polyester, a polyester amide and / or a polyester urethane. 11. Biologisch abbaubare Polymermischung nach einem der An¬ sprüche 1 - 10, dadurch gekennzeichnet, dass mindestens eine weitere Komponente, wie ein Additiv, Zuschlagstoff oder Füll¬ stoff miteingeschlossen ist, wie ein Weichmacher, ein Stabi- - 31 -11. Biodegradable polymer mixture according to one of claims 1 to 10, characterized in that at least one further component, such as an additive, additive or filler, is included, such as a plasticizer, a stabilizer, - 31 - lisator, ein Antiflammmittel, ein weiteres biologisch abbau¬ bares Biopolymer, wie Celluloseester, Cellulose, Polyhydroxy- buttersäure, ein hydrophobes Protein, Polyvinylalkohol, Gela¬ tine, Zein, Polysaccarid, Polylactid, Polyvinylacetat, Poly- acrylat, ein Zuckeralkohol, Schellack, Casein, ein Fettsäure¬ derivat, Pflanzenfasern, Lecithin oder Chitosan.lisator, an antiflaming agent, another biodegradable biopolymer, such as cellulose ester, cellulose, polyhydroxybutyric acid, a hydrophobic protein, polyvinyl alcohol, gelatures, zein, polysaccharide, polylactide, polyvinyl acetate, polyacrylate, a sugar alcohol, shellac, casein , a fatty acid derivative, plant fibers, lecithin or chitosan. 12. Biologisch abbaubare Polymermischung nach einem der An¬ sprüche l - ll, dadurch gekennzeichnet, dass die Polymermi¬ schung mindestens einen organischen Füllstoff erhalten aus nachwachsenden Rohstoffen, wie insbesondere Cellulosefasern.12. Biodegradable polymer mixture according to claim 1, characterized in that the polymer mixture comprises at least one organic filler obtained from renewable raw materials, in particular cellulose fibers. 13. Biologisch abbaubare Polymermischung nach einem der An¬ sprüche 1 - 12, dadurch gekennzeichnet, dass zur weiteren Reduktion der hydrophilen Eigenschaften der thermoplastischen Stärke ein Vernetzungsmittel vorgesehen ist, wie bei¬ spielsweise eine Dicarbonsäure bzw. eine Polycarbonsäure so¬ wie deren Anhydrid, ein Isocyanat, Formaldehyd und deren De¬ rivate, Harnstoff-Formaldehyd, ein Melamin-Formaldehyd bzw. ein Phenol-Formaldehyd-Harz, Phosphat, Polyphosphat und/oder ein Alkylketendimeres der allgemeinen Formel:13. Biodegradable polymer mixture according to any one of An¬ claims 1-12, characterized in that to further reduce the hydrophilic properties of the thermoplastic starch, a crosslinking agent is provided, such as spielsweise a dicarboxylic acid or a polycarboxylic acid so¬ as their anhydride, a Isocyanate, formaldehyde and their derivatives, urea-formaldehyde, a melamine-formaldehyde or a phenol-formaldehyde resin, phosphate, polyphosphate and / or an alkyl ketene dimer of the general formula: R 0R 0 C = C C = 0 H CC = C C = 0 H C R HR H wobei R = linear gesättigte Alkylgruppe im Bereich von C12 bis C24.where R = linearly saturated alkyl group in the range of C12 to C24. 14. Biologisch abbaubare Polymermischung nach einem der An¬ sprüche 1 - 13, dadurch gekennzeichnet, dass der Anteil ther¬ moplastische Stärke, enthaltend ein Plastifizier- bzw. ein - 32 -14. Biodegradable polymer mixture according to any one of claims An¬ 1-13, characterized in that the proportion ther¬ moplastic starch containing a plasticizer or a - 32 - 19. Verfahren nach einem der Ansprüche 17 oder 18, dadurch gekennzeichnet, dass der Wassergehalt vor oder beim Misch auf < 0,5 Gew.%, vorzugsweise < 0,1 Gew.%, reduziert wird.19. The method according to any one of claims 17 or 18, characterized in that the water content before or during mixing to <0.5 wt.%, Preferably <0.1 wt.% Is reduced. 20. Verfahren nach einem der Ansprüche 17 - 19, dadurch ge¬ kennzeichnet, dass das Mischen der Schmelze in einem Tempera¬ turbereich von 120 - 260°C erfolgt, vorzugsweise in einem Be¬ reich von ca. 140 - 160°C.20. The method according to any one of claims 17 - 19, characterized ge indicates that the mixing of the melt in a tempera ture range of 120 - 260 ° C, preferably in a range of about 140 - 160 ° C. 21. Verfahren nach einem der Ansprüche 17 - 20, dadurch ge¬ kennzeichnet, dass das Mischen in einem Extruder oder Kneter erfolgt, und dass nach Abzug der Schmelze aus der Düse diese in einem Wasserbad gekühlt und konditioniert wird, um an- schliessend beispielsweise granuliert zu werden.21. The method according to any one of claims 17 - 20, characterized ge indicates that the mixing takes place in an extruder or kneader, and that after deduction of the melt from the nozzle, this is cooled and conditioned in a water bath, then, for example, granulated to become. 22. Verfahren zum Verarbeiten einer Polymermischung nach ei¬ nem der Ansprüche 1 - 16, dadurch gekennzeichnet, dass die beispielsweise als Granulat vorliegende Polymermischung vor dem Verarbeiten durch Spritzen, Extrudieren oder Blasen mit einem Weichmacher, wie Glyzerin, Sorbitol, etc. und/oder Was¬ ser konditioniert wird.22. A process for processing a polymer mixture according to ei¬ nem of claims 1-16, characterized in that the example present as granules polymer mixture prior to processing by spraying, extruding or blowing with a plasticizer, such as glycerol, sorbitol, etc. and / or Was¬ water is conditioned. 23. Verfahren nach Anspruch 22, dadurch gekennzeichnet, dass die als Granulat vorliegende Polymermischung zu einem Wasser¬ gehalt von 1 - 6 Gew.% konditioniert wird, und anschliessend gespritzt, extrudiert oder zu Folien geblasen wird, wobei das hergestellte Spritzgussteil oder Extrudat bzw. die Folie vor¬ zugsweise noch unmittelbar nach Herstellen in relativ feuch¬ ter Umgebung gelagert wird, mit einer relativen Feuchte23. The method according to claim 22, characterized in that the present as granules polymer mixture to a water content of 1-6 wt.% Conditioned, and then sprayed, extruded or blown into films, wherein the produced injection molded part or extrudate or the film is preferably still stored immediately after production in a relatively humid environment, with a relative humidity > 40%.> 40%. 24. Ein- oder Mehrschichtfolie, mindestens enthaltend eine Schicht, bestehend aus einer Polymermischung, nach einem der Ansprüche 1 - 16. - 33 -24. Single-layer or multilayer film, at least containing a layer consisting of a polymer mixture, according to any one of claims 1-16. - 33 - Quellmittel 10 - 95 Gew.%, bezogen auf das Gesamtgewicht der Mischung, vorzugsweise 30 - 75 Gew.%, beträgt.Swelling agent 10 to 95 wt.%, Based on the total weight of the mixture, preferably 30 to 75 wt.% Is. 15. Biologisch abbaubare Polymermischung nach einem der An¬ sprüche 1 - 14, dadurch gekennzeichnet, dass der Anteil ther¬ moplastische Stärke in der Mischung 40 - 65 Gew.% beträgt.15. Biodegradable polymer mixture according to one of claims 1 to 14, characterized in that the proportion of thermoplastic starch in the mixture is 40 to 65% by weight. 16. Biologisch abbaubare Polymermischung nach einem der An¬ sprüche 1 - 6, gekennzeichnet durch thermoplastische Stärke, ein Polyester-Copolymer mit aliphatischen wie auch aromati¬ schen Blöcken sowie ein Copolymeres, ausgewählt aus Aethylen- acrylsäure-Copolymer und Aethylenvinylalkohol-Copolymer.16. A biodegradable polymer mixture according to any one of claims An¬ 1-6, characterized by thermoplastic starch, a polyester copolymer having aliphatic as well as aromati¬ rule blocks and a copolymer selected from Aethylen- acrylic acid copolymer and Aethylenvinylalkohol copolymer. 17. Verfahren zur Herstellung einer Polymermischung nach ei¬ nem der Ansprüche 1 - 16, dadurch gekennzeichnet, dass Stär¬ ke, wie insbesondere thermoplastische Stärke, mit mindestens einem der nachfolgenden Polymeren gemischt wird:17. A process for preparing a polymer mixture according to ei¬ nem of claims 1-16, characterized in that starch ke, in particular thermoplastic starch, is mixed with at least one of the following polymers: - einem aromatischen Polyester- an aromatic polyester - einem Polyester-Copolymeren mit aromatischen und aliphatischen Blöcken,a polyester copolymer with aromatic and aliphatic blocks, - einem Polyesteramid,a polyesteramide, - einem Polyethylenoxidpolymer bzw. Polyglycol,a polyethylene oxide polymer or polyglycol, - einem Polyesterurethan- a polyester urethane - und/oder Mischungen, wobei das Mischen der Schmelze erfolgt und wobei vor und/oder beim Mischen der Wassergehalt auf < 1,0 Gew.%, bezogen auf das Gewicht der Mischung, reduziert wird.- And / or mixtures, wherein the mixing of the melt takes place and wherein before and / or during mixing, the water content is reduced to <1.0 wt.%, Based on the weight of the mixture. 18. Verfahren nach Anspruch 17, dadurch gekennzeichnet, dass der Schmelze zusätzlich ein aliphatischer Polyester zugefügt wird. - 3418. The method according to claim 17, characterized in that the melt is additionally added to an aliphatic polyester. - 34 25. Behältnis oder Flasche, hergestellt mittels Formblasen, bestehend im wesentlichen aus einer Polymermischung nach ei¬ nem der Ansprüche 1 - 16.25. Container or bottle, produced by means of blow molding, consisting essentially of a polymer mixture according to ei¬ nem of claims 1-16. 26. Textiles Erzeugnis, wie Fasern, Monofile, Garne, Seile, Leinen, Flocken, Watten, Gewebe, Filze, Vliese, bestehend im wesentlichen aus einer Polymermischung nach einem der An¬ sprüche 1 - 16.26. Textile product, such as fibers, monofilaments, yarns, ropes, lines, flakes, wadding, fabrics, felts, nonwovens, consisting essentially of a polymer mixture according to any one of claims An¬ 1-16. 27. Hygieneartikel, wie Windeln, Binden, Inkontinenzprodukte, Betteinlagen und dgl., aufweisend mindestens ein Vlies und/- oder ein Backsheet, im wesentlichen bestehend aus einer Polymermischung nach einem der Ansprüche 1 - 16.27. Hygiene articles, such as diapers, sanitary napkins, incontinence products, bed inserts and the like, comprising at least one nonwoven and / or a backsheet, essentially consisting of a polymer mixture according to one of claims 1-16. 28. Klebstoff, im wesentlichen bestehend aus einer Polymermi¬ schung nach einem der Ansprüche 1 - 16 oder einer alkoholi¬ schen Lösung davon.28. An adhesive, consisting essentially of a Polymermi¬ Schung according to one of claims 1-16 or a alkoholi¬'s solution thereof. 29. Beschichtung, wie insbesondere ein Imprägnierungsmittel, im wesentlichen bestehend aus einer Polymermischung nach ei¬ nem der Ansprüche 1 - 16 oder einer alkoholischen Lösung da¬ von. 29. Coating, in particular an impregnating agent, consisting essentially of a polymer mixture according to ei¬ nem of claims 1-16 or an alcoholic solution da¬ of. - 35 -- 35 - IN ARTIKEL 19GENANNTEERKLÄRUNGIN ARTICLE 19 DECLARATION OF CONTRACT Aufgrund des internationalen Recherchenberichtes wurden die Ansprüche der vorliegenden internationalen Patentanmeldung dahingehend eingeschränkt bzw. präzisiert, dass in der biolo¬ gisch abbaubaren Polymermischung als Biopolymer Stärke, vor¬ zugsweise thermoplastische Stärke, vorliegt.On the basis of the international search report, the claims of the present international patent application were limited or specified in that the biologically degradable polymer mixture contains starch, preferably thermoplastic starch, as the biopolymer. Im Stand der Technik werden in Dokument Dl, einem Artikel in der Zeitschrift Stärke 45 (1993) Nr. 9, Seite 314 bis 322 mit dem Titel "Der Einsatz von Stärke bei der Modifizierung syn¬ thetischer Kunststoffe" Werkstoffe beschrieben, enthaltend unter anderem destrukturierte Stärke sowie aliphatische Poly¬ ester, wie beispielsweise Polymilchsäure und Polycaprolacton. So werden beispielsweise auf den Seiten 319 und 320 verschie¬ dene Polymerblends beschrieben, wo auf Polymilchsäure und Polycaprolacton als mögliche Mischkomponenten zur Stärke hin¬ gewiesen wird. In der vorliegenden internationalen Patentan¬ meldung werden aber derartige Mischungen unter Hinweis auf die EP 535 994 als bekannt vorausgesetzt, indem in der ge¬ nannten europäischen Patentanmeldung Polymermischungen be¬ schrieben werden, bestehend im wesentlichen aus destruktu¬ rierter Stärke und einem aliphatischen Polyester, wie bei¬ spielsweise Polycaprolacton. Weiter wird in der Beschrei¬ bungseinleitung der vorliegenden internationalen Patentanmel¬ dung auf die Nachteile bei der Verwendung von aliphatischen Polyestern, in Mischungen mit Stärke, hingewiesen.In the prior art materials are described in document Dl, an article in the magazine strength 45 (1993) No. 9, pages 314 to 322 entitled "The use of starch in the modification of synthetic synthetic materials" containing inter alia destructured Starch and aliphatic poly esters, such as polylactic acid and polycaprolactone. For example, on pages 319 and 320, various polymer blends are described, where polylactic acid and polycaprolactone are shown as possible mixing components for starch. However, in the present international patent application, mixtures of this kind are assumed to be known, with reference to EP 535 994, in that polymer mixtures are described in the cited European patent application, consisting essentially of destructured starch and an aliphatic polyester, such as For example, polycaprolactone. Furthermore, the description of the preparation of the present international patent application points out the disadvantages in the use of aliphatic polyesters, in mixtures with starch. In Dokument D2, der internationalen Patentanmeldung WO92/09654 werden Polymerblends beschrieben, beinhaltend ali- phatisch, aromatische Copolyester und Celluloseester. Auf- 36 -In document D2, the international patent application WO92 / 09654 polymer blends are described, including aliphatic, aromatic copolyesters and cellulose esters. On- 36 - grund dieser Entgegenhaltung wurde die vorliegende interna¬ tionale Patentanmeldung dahingehend eingeschränkt, dass als auf nachwachsenden Rohstoffen basierend hergestelltes Biopo¬ lymer lediglich Stärke, wie vorzugsweise thermoplastische Stärke, Verwendung findet. Die in D2 genannten Celluloseester fallen somit nicht mehr unter den Wortlaut der neu überarbei¬ teten Ansprüche.For the purposes of this citation, the present international patent application has been limited to the effect that only biopoly- mer, such as preferably thermoplastic starch, is used as the biopolymer produced based on renewable raw materials. The cellulose esters mentioned in D2 thus no longer fall under the wording of the newly revised claims. In Dokument D3 , der internationalen Patentanmeldung WO93/07213 stehen wiederum lediglich aliphatische Polyester zur Diskussion, um mit Stärke gemischt zu werden. Somit gilt für D3 dieselbe Beurteilung wie für die oben erwähnte Entge¬ genhaltung Dl.Again, in document D3, International Patent Application WO93 / 07213, only aliphatic polyesters are contemplated to be blended with starch. Thus, the same assessment applies to D3 as for the above-mentioned condition Dl. Derselbe Kommentar trifft zu auf das Dokument D4, die europä¬ ische Patentanmeldung 0 596 437, in welcher Anmeldung erneut Stärke mit aliphatischen Polyestern gemischt wird.The same comment applies to document D4, European Patent Application 0 596 437, in which application starch is again mixed with aliphatic polyesters. In Dokument D5, der deutschen Offenlegungsschrift DE 43 27 024, werden aliphatische Polyesteramide beschrieben. Als mög¬ licher Biopolymermischpartner wird lediglich Cellulose ge¬ nannt, und Stärke steht in dieser Offenlegungsschrift nicht zur Diskussion. Somit gilt derselbe Kommentar wie unter Bezug auf das oben erwähnte Dokument D2 angeführt.In document D5, German Offenlegungsschrift DE 43 27 024, aliphatic polyester amides are described. As a possible Biopolymermischpartner only cellulose is called ge, and starch is not discussed in this publication. Thus, the same comment applies as with reference to the above-mentioned document D2. Das Dokument D6 schlussendlich, die deutsche Offenlegungs- schrift D 43 35 983 wurde erst veröffentlicht nach dem Prio¬ ritätstag der vorliegenden internationalen Patentanmeldung. Zudem wird in diesem Dokument wiederum nur Stärke im Zusam¬ menhang mit beispielsweise Polycaprolactonen, Polylactiden und dgl . genannt, d.h. es werden Stoffkombinationen zur Her¬ stellung einer Polymermischung genannt, welche nicht unter den Wortlaut von Anspruch 1 fallen. - 37 -Finally, document D6 was published after the priority date of the present international patent application. In addition, in this document, in turn, only starch in connection with, for example, polycaprolactones, polylactides and the like. called, ie substance combinations for the preparation of a polymer mixture are called, which do not fall under the wording of claim 1. - 37 - Somit sind gegenüber dem ursprünglichen Anspruch 1 der vor¬ liegenden internatinalen Patentanmeldung lediglich die beiden Dokumente D2 und D5 zu beachten, wobei durch Einschränkung des auf nachwachsenden Rohstoffen basierend hergestellten Biopolymers auf Stärke, wie vorzugsweise thermoplastische Stärke, auch diese beiden Dokument nicht mehr relevant sind.Thus, compared to the original claim 1 of the present international patent application, only the two documents D2 and D5 are to be observed, whereby these two documents are no longer relevant by restricting the biopolymer based on renewable raw materials to starch, such as preferably thermoplastic starch. Der weiteren Prüfung ist somit der überarbeitete und ein¬ geschränkte Anspruchssatz zugrunde zu legen. The further examination must therefore be based on the revised and limited set of claims.
PCT/IB1996/000275 1995-04-07 1996-04-02 Biologically degradable polymer mixture Ceased WO1996031561A1 (en)

Priority Applications (7)

Application Number Priority Date Filing Date Title
DK96905977T DK0819147T3 (en) 1995-04-07 1996-04-02 Polymer blend which is biodegradable
JP08525223A JP3107830B2 (en) 1995-04-07 1996-04-02 Biologically degradable polymer mixtures
DE59610506T DE59610506D1 (en) 1995-04-07 1996-04-02 BIODEGRADABLE POLYMER BLEND
US08/930,748 US6096809A (en) 1995-04-07 1996-04-02 Biologically degradable polymer mixture
AT96905977T ATE242295T1 (en) 1995-04-07 1996-04-02 BIODEGRADABLE POLYMER BLEND
EP96905977A EP0819147B1 (en) 1995-04-07 1996-04-02 Biologically degradable polymer mixture
AU49522/96A AU705499B2 (en) 1995-04-07 1996-04-02 Biologically degradable polymer mixture

Applications Claiming Priority (4)

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