Polyester blend for home composting applications

Abstract

For manufacturing household composting products, Based on the total weight of polylactic acid a) and aliphatic-aromatic biodegradable polyester b), 10 to 85% by weight of at least one polylactic acid a), Based on the total weight of polylactic acid a) and aliphatic-aromatic biodegradable polyester b), 15 to 90% by weight of at least one biodegradable aliphatic-aromatic polyester and Use of polymer compositions containing the above.

Description

[Technical Field]

[0001] This invention relates to improving the compostability of polylactic acid in households, specifically to aliphatic C6-C 18 Dicarboxylic acids, aromatic dicarboxylic acids, and aliphatic C2-C 10 This invention relates to the use of compostable aliphatic-aromatic polyesters derived from diols, and to the use of mixtures containing such aliphatic-aromatic polyesters and polylactic acid for the production of compostable articles. The invention also relates to a method for producing compostable articles from compositions containing such aliphatic-aromatic polyesters and polylactic acid.

[0002] The use of thermoplastic materials such as polystyrene, polyethylene, and polyurethane has long been established in many technological fields, particularly in packaging. However, these conventional thermoplastic materials are increasingly criticized for environmental reasons, especially regarding plastic litter and a sustainable circular economy. To avoid such problems, biodegradable thermoplastic polymers have been developed from both natural and fossil resources. Such biodegradable alternatives include aliphatic-aromatic polyesters such as poly(butylene-co-adipate-co-terephthalate) (PBAT), poly(butylene-co-azelate-co-terephthalate) (PBAzT), and poly(butylene-co-sebacate-co-terephthalate) (PBSeT), aliphatic polyesters such as poly(butylene-co-succinate) (PBS), starches and their derivatives such as thermoplastic starch (TPS), polylactic acid (PLA), polycaprolactone (PCL), polyglycolic acid (PGA), and polyhydroxyalkanoates (PHA).

[0003] It should be noted that terms such as "biodegradability," "biodegradable," and "compostable" are used to describe biological decomposition under a wide range of different environmental conditions. Biodegradability generally means that a polymer or polymer mixture decomposes within a reasonable and demonstrable timeframe. Biological decomposition can occur enzymatically, hydrolyzably, oxidatively, and / or through exposure to electromagnetic radiation such as UV irradiation, but is mostly triggered by exposure to microorganisms such as bacteria, yeasts, fungi, and algae, and is dependent on specific ambient conditions. As a result, various standards have been developed to determine biodegradability or compostability under specific conditions.

[0004] Requirements and examples of methods for quantifying the biodegradability of polyester in compost are defined in DIN EN 13432 (December 2000, "Requirements for packaging recoverable through composting and biodegradation"). Compostability under this standard simulates decomposition in an industrial composting plant and requires that materials mixed with compost under specified conditions of 58±2°C, oxygen, and moisture in the presence of microorganisms specified in ISO 14855:1999, be biodegraded to at least 90% overall ("absolute" CO2 emissions), or to 90% of the maximum biodegradation of a reference material, such as cellulose ("relative" CO2 emissions), within a maximum of six months. The biodegradation rate is based on the conversion of the test material's carbon to carbon dioxide. Compostability under these conditions is also called industrial compostability.

[0005] Another example is DIN EN 17033:2018, which defines a polymer blend used in the manufacture of soil biodegradable root cover films as "biodegradable in soil" if, under the conditions specified in DIN EN ISO 17556, it achieves at least 90% biodegradation overall or 90% of the maximum biodegradation of the reference material within two years.

[0006] Other methods for determining biodegradability are described, for example, in ASTM D5338 and ASTM D6400.

[0007] The home compostability of a polymer composition can also be determined by following the methods described in ISO 14855-1 (2012) or EN ISO 14855-2, but at a lower temperature. The criteria for achieving home compostability are defined, for example, in ISO DIN EN 17427:2022. According to this standard, a polymer composition can be classified as home compostable if it reaches 90% absolute or relative CO2 generation within 365 days at a temperature within the range of 25 + / - 5 °C, i.e., the polymer composition is biodegradable under conditions simpler than industrial composting conditions.

[0008] Home compostability is valuable, for example, in the home for items used as single-use packaging. In particular, the value of biodegradation is preferred for food-soiled packaging that cannot be appropriately mechanically recycled. Home composting is beneficial in countries and regions where there is no access to established infrastructure of industrial bio-waste treatment facilities such as composting plants or anaerobic digestion plants.

[0009] Articles such as food containers made of home compostable polymers are not automatically considered and recognized as home compostable. This is due to changes that can be made to the article, such as size, shape, thickness, and other possible components that may be present. Therefore, the manufacturer of the article must prove home compostability. For example, depending on the information already available on the home compostability of other articles made from home compostable compositions, the article itself may have to be tested according to ISO DIN EN 17427:2022.

[0010] Some of the biodegradable polymers mentioned above are compostable under industrial conditions but not under home composting conditions. Examples include polylactic acid, polyhydroxyoctanoate, poly(butylene-co-succinate), and mixtures of polylactic acid and polyhydroxybutyrate. There are also those that are compostable under both industrial and simpler home composting conditions, such as thermoplastic starch, polyhydroxybutyrate, poly(butylene-co-sebacate-co-terephthalate), polycaprolactone, and certain mixtures of polylactic acid and polycaprolactone; see, for example, Environ.Sci.Technol.2018, 52, pp. 10441-10452.

[0011] Biodegradable polymers are typically used in mixtures combining different biodegradable polymers. Ideally, these mixtures combine the desirable properties of the individual components, such as good overall processing and mechanical properties, relatively low-cost availability, and environmentally friendly polymer preparation and disposal.

[0012] U.S. Patent Application Publication No. 2008 / 0281018(A1) describes a biodegradable polyester mixture comprising 5 to 80% by weight of a biodegradable aliphatic-aromatic polyester and 20 to 95% by weight of a biodegradable polyester selected from polylactic acid, polycaprolactone, polyhydroxyalkanoates, and aliphatic polyesters, epoxy group copolymers, and optionally further additives and fillers. Such compositions are widely used in a variety of applications, such as the manufacture of flexible films for root covering films, consumer bags and garbage bags, and coatings and laminations on substrates. The addition of the rigid polymer polylactide to the biodegradable polyester increases the E modulus and tensile strength of the polyester composition and improves the processability of the composition during film blowing. The polylactic acid and biodegradable polyester composition may also contain further components such as fillers and additional biodegradable polymers.

[0013] As mentioned above, polylactic acid itself is not compostable, and compositions containing polylactic acid (>10%) and other biodegradable polymers such as polyhydroxybutyrate are also not compostable. Similar behavior is expected for mixtures mainly containing polylactic acid and small amounts of aliphatic-aromatic polyesters such as poly(butylene-co-adipate-co-terephthalate). However, this is different for compositions containing polycaprolactone and polylactic acid, which are fully compostable. Unfortunately, polycaprolactone is very expensive and only available from fossil sources.

[0014] Given the increasing problem of plastic litter and the objective of establishing sustainable economics, there is still a need to provide further means to provide polylactic acid-containing polymer materials that can be used to manufacture articles for various different applications that are biodegradable not only under industrial composting conditions but also under domestic composting conditions, in order to improve the compostability of polylactic acid and to meet the requirements of common polymer processing technologies such as film blowing, extrusion coating, thermoforming, extrusion, injection molding, blow molding, or fiber spinning.

[0015] Therefore, the fundamental objective of this invention is to improve the compostability of polylactic acid in households. Another objective is to provide a household compostable article containing polylactic acid.

[0016] Surprisingly, b-1) Based on the total amount of components b-1) and b-2), 20-70 mol% of at least one aliphatic C6-C 18 Dicarboxylic acid or C6-C 18 Dicarboxylic acid derivatives, b-2) Based on the total amount of components b-1) and b-2), 80 to 30 mol% of at least one aromatic dicarboxylic acid or aromatic dicarboxylic acid derivative, Based on the total amount of b-3)b-1) and b-2), 98-102 mol% aliphatic C2-C 10 Diol and, b-4) Based on the total weight of components b-1), b-2), and b-3), 0 to 2% by weight of at least a trivalent alcohol, b-5) Based on the total weight of components b-1), b-2), and b-3), 0 to 2% by weight of a chain extender and Biodegradable aliphatic-aromatic polyesters derived from this material have been found to improve the compostability of polylactic acid in households.

[0017] Similarly, and surprisingly, a) 10 to 85% by weight of at least one polylactic acid a) based on the total weight of polylactic acid a) and aliphatic-aromatic biodegradable polyester b), b) 15 to 90% by weight of at least one biodegradable aliphatic-aromatic polyester (b) derived from the following, based on the total weight of polylactic acid a) and aliphatic-aromatic biodegradable polyester b): b-1) Based on the total amount of components b-1) and b-2), 20-70 mol% of at least one aliphatic C6-C 18 Dicarboxylic acid or C6-C 18 Dicarboxylic acid derivatives, b-2) Based on the total amount of components b-1) and b-2), 80 to 30 mol% of at least one aromatic dicarboxylic acid or aromatic dicarboxylic acid derivative, Based on the total amount of b-3)b-1) and b-2), 98-102 mol% aliphatic C2-C 10 Diol, b-4) 0 to 2% by weight of at least trivalent alcohols based on the total weight of components b-1), b-2), and b-3), and b-5) 0-2% by weight of a chain extender based on the total weight of components b-1), b-2), and b-3), c) 0 to 40% by weight of at least one biodegradable polyester based on the constituent components a) to f), d) 0 to 55% by weight of at least one starch-based polymer or cellulose-based polymer based on components a) to f), e) 0 to 40% by weight of at least one inorganic filler based on the constituent components a) to f), f) 0 to 40% by weight of at least one compound selected from crosslinking agents, chain extenders, stabilizers, nucleating agents, lubricants, mold release agents, surfactants, waxes, antistatic agents, antifogging agents, dyes, pigments, UV absorbers, UV stabilizers, oxygen scavengers, dispersants, and other plastic additives, based on components a) to f) A polymer composition containing the following: It has been found that it can be used to manufacture compostable materials for home use.

[0018] The present invention also relates to a process for producing compostable articles for home use.

[0019] The present invention will be described in more detail below.

[0020] Home compostability can be determined by various methods and standards specified in various norms and regulatory requirements. Such norms and regulatory requirements may differ from one another depending on the current laws and regulations concerning home compostability certification implemented in different regions and countries. Examples include ISO DIN EN 17427:2022 and the French standard NF T 51-800 Plastics - Specifications for plastics suitable for home compositing (2015). In principle, home compostability can be determined according to any of these norms and standards.

[0021] According to a preferred example of determining the compostability of a polymer or polymer composition, such a polymer or polymer composition is classified as compostable if the particles of the polymer or polymer composition having a particle size in the range of 100 to 300 microns reach 90% absolute or relative CO2 emissions within 365 days at a temperature of 25+ / -5°C, as determined according to 14855-1(2012) or EN ISO 14855-2(2012).

[0022] A preferred example for determining the compostability of an item is ISO DIN EN 17427:2022.

[0023] The polymer composition contains at least one polylactic acid a) in an amount of 10 to 85% by weight based on the total weight of the polylactic acid a) and the aliphatic-aromatic biodegradable polyester b).

[0024] Polylactic acid (PLA), also known as polylactide, is a thermoplastic polyester having a backbone formula (C3H4O2) n or [-C(CH3)HC(=O)O-] n and is formally obtained by the condensation of lactic acid C(CH3)(OH)HCOOH with dehydration. Polylactic acid can also be prepared by ring-opening polymerization of any of D-lactide, L-lactide, mesolactide, or mixtures thereof. When only D-lactide or only L-lactide is polymerized, the resulting polymer chains consist essentially of D-lactic acid units or L-lactic acid units, respectively. In the case of polymerization of a mixture of D-lactide and L-lactide, random polymerization of D-lactide and L-lactide results in longer sequences of -(D) n and -(L) n The minimum block length of D-lactic acid units and L-lactic acid units in the polylactide is 2 from a theoretical point of view when PLA is prepared only from D-lactide and L-lactide, i.e., without containing mesolactide. This would only apply in the case of a strict alternating reaction of D-lactide and L-lactide. The latter also applies when a mixture of either L-lactide and a small amount of mesolactide or D-lactide and a small amount of mesolactide is polymerized.

[0025] The term "unit derived from lactic acid" is also called "lactic acid unit" and means a monomeric lactic acid unit derived from L-lactic acid or D-lactic acid.

[0026] Polylactic acid, which mainly contains repeating units derived from mesolactide, is also called poly(mesolactide) or poly(mesolactic acid), and is sometimes abbreviated as PMLA herein. Mesolactide is a cyclic diester of D-lactic acid and L-lactic acid. Essentially, the homopolymerization of mesolactide is a head-to-head reaction involving two L-lactic acid units or two D-lactic acid units, resulting in -(LDDL-) n Or -(DLLD-) n This can result in the following sequence, or through the reaction between L-lactate units and D-lactate units (head-tail reaction), -(DLDL) n Because this arrangement can be obtained, polymers are produced in which D-lactic acid units and L-lactic acid units are distributed very regularly within the polymer chain. This means that the average sequence length of L-lactic acid units and D-lactic acid units resulting from ring-opening polymerization, also called the average block length, is a minimum of 1 and a maximum of 2, neglecting transesterification reactions. Random polymerization of mesolactide yields average sequence lengths of D-lactic acid units and L-lactic acid units that are continuous between these limits, i.e., 1 to 2. In addition, the ratio of D-lactic acid units to L-lactic acid units in polymers derived solely from mesolactide is close to 1:1. Further details and information regarding the preparation of poly(mesolactide) are described in U.S. Patent No. 5,142,023 and International Publication No. 2020 / 251745(A1).

[0027] Polylactic acid may further contain repeating units formed from other monomers copolymerizable with mesolactides or D- or L-lactides, such as alkylene oxides (including ethylene oxide, propylene oxide, butylene oxide, tetramethylene oxide, etc.), cyclic lactones, or carbonates. These repeating units derived from other monomers may be present in block and / or random configurations. These other repeating units may constitute up to 10% by weight of polylactic acid, preferably 0% to 5% by weight of PLA, and particularly preferably about 0% to 2% by weight, or may not be present at all. The remaining weight of polylactic acid may consist of residues of initiator compounds, often used during the polymerization process to provide molecular weight control. Suitable initiators include, for example, water, alcohols, various types of polyhydroxy compounds (e.g., ethylene glycol, propylene glycol, polyethylene glycol, polypropylene glycol, other glycol ethers, glycerin, trimethylolpropane, pentaerythritol, hydroxyl-terminated butadiene polymers, etc.), polycarboxyl-containing compounds, and compounds having at least one carboxyl group and one hydroxyl group (e.g., lactic acid or lactic acid oligomers). The initiator residues preferably constitute 5% or less, particularly 2% or less, of the weight of the polylactic acid, except when the initiator is a residue of lactic acid or a lactic acid oligomer, and in these cases, they can constitute any proportion of the polylactic acid.

[0028] When polylactic acid is measured by GPC against a polystyrene standard in THF, it may have a number average molecular weight of at least 5000 g / mol, preferably at least 20000 g / mol, more preferably at least 30000 g / mol, and most preferably greater than 50000 g / mol. Preferably, the upper limit of the number average molecular weight is 200000 g / mol, and more preferably 130000 g / mol. Preferably, the polylactic acid has a number average molecular weight in the range of 5000 g / mol to 200000, more preferably in the range of 20000 to 200000 g / mol, even more preferably in the range of 30000 to 130000 g / mol, and particularly in the range of 50000 to 130000 g / mol.

[0029] Polylactic acid can have a relative viscosity of 1.1 to 6, for example, 1.25 to 5, or 1.5 to 3.5, when measured with a capillary viscometer at 30°C using a 1% wt / vol solution of polylactic acid in chloroform relative to a chloroform standard.

[0030] Polylactic acid should be 0.5 to 80, preferably 2 to 40 cm³, relative to EN ISO 1133 (190°C, 2.16 kgf). 3 It may have a melt volume rate (MVR) of 10 minutes.

[0031] Polylactic acid can be crystalline, semi-crystalline, or amorphous. In particular, suitable polylactic acid has a melting or softening point below 240°C, especially below 230°C, and especially below 220°C, as determined by DSC. Generally, the melting point of crystalline or semi-crystalline polylactic acid is at least 120°C.

[0032] Polylactic acid is commercially available from NatureWorks under trade names such as Ingeo® 6201D, Ingeo® 6202D, Ingeo® 6251D, Ingeo® 3051D, Ingeo® 4043D, and Ingeo® 3251D; from Total Corbion under trade names such as Luminy® LX975, Luminy® LX930, Luminy® LX175; Luminy® LX575, Luminy® L130, Luminy® LX530, and Luminy® L105; and from Hisun under trade names such as Revode 110, Revode 190, and Revode 290.

[0033] Particularly preferred polylactic acid has the following properties: • 0.5 to 80 degrees Celsius, especially between 2 and 40 cm, relative to EN ISO 1133 (190°C, 2.16 kgf). 3 Melt volume rate (MVR) / 10 minutes • Melting point below 240℃ • Water content less than 1000 ppm, • Residual (lactide) monomer content of less than 0.3% • Molecular weight exceeding 80,000 Daltons M w .

[0034] The concentration of polylactic acid a) in the polymer composition is at least 10% by weight, preferably at least 15% by weight, more preferably at least 20% by weight, even more preferably at least 25% by weight, most preferably at least 35% by weight, and particularly preferably at least 45% by weight, based on the total weight of components a) and b). The maximum concentration of polylactic acid a) in the polymer composition is 85% by weight, preferably 80% by weight, and more preferably 75% by weight, based on the total weight of components a) and b). The preferred concentration range of polylactic acid a) is 10-80% by weight and 15-85% by weight, more preferably 15-80% by weight and 20-80% by weight, even more preferably 25-80% by weight, most preferably 35-75% by weight, and particularly preferably 45-75% by weight, based on the total weight of components a) and b).

[0035] Polymer compositions for use in producing household compostable articles consist of 10-85% by weight of polylactic acid a) and aliphatic-aromatic biodegradable polyester b) based on their total weight. b-1) Based on the total amount of components b-1) and b-2), 20-70 mol% of at least one aliphatic C6-C 18 Dicarboxylic acid or C6-C 18 Dicarboxylic acid derivatives, b-2) Based on the total amount of components b-1) and b-2), 80 to 30 mol% of at least one aromatic dicarboxylic acid or aromatic dicarboxylic acid derivative, Based on the total amount of b-3)b-1) and b-2), 98-102 mol% aliphatic C2-C 10 Diol and, b-4) Based on the total weight of components b-1), b-2), and b-3), 0 to 2% by weight of at least a trivalent alcohol, b-5) Based on the total weight of components b-1), b-2), and b-3), 0 to 2% by weight of a chain extender and It comprises at least one biodegradable aliphatic-aromatic polyester (b) derived from.

[0036] Aliphatic C6-C 18Dicarboxylic acids and C6-C 18 The dicarboxylic acid derivative b-1) is preferably C6-C 16 , more preferably C6-C 13 Dicarboxylic acids, their derivatives, and mixtures thereof are selected. Preferably, they are α,ω-dicarboxylic acids. The derivatives may be C1-C6 dialkyl esters or anhydrides. Examples of C1-C6 dialkyl esters are dimethyl, diethyl, di-n-propyl, diisopropyl, di-n-butyl, diisobutyl, di-tert-butyl, di-n-pentyl, diisopentyl, and di-n-hexyl esters. C1-C4 dialkyl esters are preferred, and dimethyl esters are particularly preferred.

[0037] Suitable examples of aliphatic dicarboxylic acids and their derivatives include adipic acid, pimelic acid, suberic acid, azelaic acid, sebacic acid, undecanediic acid, dodecanediic acid, brassic acid, tetradecanediic acid, pentadecanediic acid, hexadecanedioic acid, heptadecanedioic acid, octadecanediic acid, their derivatives, particularly C1-C4 dialkyl esters, and mixtures thereof. Preferably, aliphatic C6-C 18 Dicarboxylic acids are selected from adipic acid, azelaic acid, sebacic acid, 1,12-dodecanoic acid, brassic acid, their derivatives, more preferably C1-C4 alkyl esters, and mixtures thereof. Particularly preferred aliphatic dicarboxylic acids are selected from adipic acid, azelaic acid, sebacic acid, and brassic acid, their C1-C4 alkyl esters, and mixtures thereof. Azelaic acid, sebacic acid, and brassic acid have the further advantage of being available from renewable raw materials. Sebacic acid, its derivatives, and mixtures thereof are most preferred.

[0038] Aliphatic C6-C 18The dicarboxylic acids and their derivatives (b-1) may be selected from a mixture of at least two aliphatic acids or their derivatives. A mixture comprising a first aliphatic dicarboxylic acid selected from adipic acid, sebacic acid, their derivatives, and mixtures thereof, and a second aliphatic dicarboxylic acid selected from suberic acid, azelaic acid, undecanedioic acid, dodecanedioic acid, brassic acid, tetradecanedioic acid, pentadecanedioic acid, hexadecanedioic acid, heptadecanedioic acid, octadecanedioic acid, their derivatives, and mixtures thereof is preferred. A mixture comprising sebacic acid and / or its derivatives and one or more aliphatic acids selected from adipic acid, azelaic acid, brassic acid, their derivatives, and mixtures thereof is preferred, as is a mixture comprising adipic acid and / or its derivatives and one or more aliphatic acids selected from sebacic acid, azelaic acid, brassic acid, their derivatives, and mixtures thereof. Most preferred are mixtures of sebacic acid and / or its derivatives with azelaic acid and / or its derivatives, mixtures of sebacic acid and / or its derivatives with adipic acid and / or its derivatives, and mixtures of adipic acid and / or its derivatives with azelaic acid and / or its derivatives. Preferred derivatives of dicarboxylic acids are C1-C4 dialkyl esters.

[0039] Aromatic dicarboxylic acids or aromatic dicarboxylic acid derivatives b-2) are preferably aromatic and heteroaromatic C6-C 12Dicarboxylic acids and their derivatives are selected, more preferably from aromatic and heteroaromatic C6-C8 dicarboxylic acids and their derivatives. Examples of such aromatic and heteroaromatic dicarboxylic acids and their derivatives are terephthalic acid, isophthalic acid, 2,6-naphthoic acid and 1,5-naphthoic acid, 2,5-franzicarboxylic acid, 2,4-franzicarboxylic acid, 2,3-franzicarboxylic acid, 3,4-franzicarboxylic acid, their C1-C6 dialkyl esters, their anhydrides where applicable, and mixtures thereof. C1-C4 dialkyl esters are preferred, and methyl esters are particularly preferred. Examples of C1-C6 dialkyl esters are dimethyl, diethyl, di-n-propyl, diisopropyl, di-n-butyl, diisobutyl, di-tert-butyl, di-n-pentyl, diisopentyl, and di-n-hexyl esters. Preferably, aromatic dicarboxylic acids or their derivatives are selected from terephthalic acid, 2,5-franzicarboxylic acid, and their derivatives, preferably their C1-C4 alkyl esters. Terephthalic acid and its C1-C4 alkyl esters are particularly preferred.

[0040] Preferably, biodegradable polyester b) is b-1) Based on the total amount of components b-1) and b-2), 20-70 mol% of at least one aliphatic C6-C 13 Dicarboxylic acid or C6-C 13 Dicarboxylic acid derivatives, b-2) 80 to 30 mol% of at least one dicarboxylic acid selected from terephthalic acid, franzicarboxylic acid, their derivatives, and mixtures thereof, based on the total amount of components b-1) and b-2). It is derived from this.

[0041] The concentration of the aromatic dicarboxylic acid or aromatic dicarboxylic acid derivative b-2) is 80 to 30 mol% based on the total amount of components b-1) and b-2). If the aromatic dicarboxylic acid or dicarboxylic acid derivative is terephthalic acid or a derivative thereof, the concentration in the polyester is preferably 70 to 30 mol%. If the aromatic dicarboxylic acid or dicarboxylic acid derivative is frangic acid or a derivative thereof, such as 2,5-frangic acid, the concentration in the polyester is preferably 80 to 50 mol% based on the total amount of components b-1) and b-2).

[0042] Aliphatic diols (b-3) are aliphatic C2-C 10 Selected from diols, preferably from C2-C6 diols, more preferably from C2-C4 diols, and particularly preferably from C3-C4 diols. Suitable aliphatic C2-C 10 Examples of diols include 1,2-ethanediol, 1,2-propanediol, 1,3-propanediol, 1,2-butanediol, 1,4-butanediol, 1,5-pentanediol, 2,2-dimethyl-1,3-propanediol (neopentyl glycol), 1,6-hexanediol, 2,4-dimethyl-2-ethyl-1,3-hexanediol, 2,2-dimethyl-1,3-propanediol, 2-ethyl-2-butyl-1, These include 3-propanediol, 2-ethyl-2-isobutyl-1,3-propanediol and 2,2,4-trimethyl-1,6-hexanediol, cyclopentanediol, 1,4-cyclohexanediol, 1,2-cyclohexanedimethanol, 1,3-cyclohexanedimethanol, 1,4-cyclohexanedimethanol, isosorbide, isoiodide, and 2,2,4,4-tetramethyl-1,3-cyclobutanediol. Preferred aliphatic C2-C 10The diol is 1,2-ethanediol, 1,3-propanediol, 1,4-butanediol, and 1,6-hexanediol, more preferably 1,3-propanediol and 1,4-butanediol, and most preferably 1,4-butanediol. It is also possible to use a mixture of different aliphatic diols. Preferably, the aliphatic diol b-3) contains at least 50 mol% of one or more diols selected from 1,2-ethanediol, 1,3-propanediol, 1,6-hexanediol, and 1,4-butanediol, particularly preferably at least 50 mol% of 1,4-butanediol.

[0043] Diols produced from renewable resources such as 1,4-butanediol from direct fermentation (International Publication No. 2008 / 115840) or bio-based hydrogenation of succinic acid, or 1,3-propanediol from fermentation developed by DuPont and Tate & Lyle are particularly preferred.

[0044] Aliphatic diols b-3) are present at a concentration of 98-102 mol% based on the total amount of b-1) and b-2).

[0045] Preferred biodegradable polyester b) is, b-1) Based on the total amount of components b-1) and b-2), 20-70 mol% of at least one aliphatic C6-C 13 Dicarboxylic acid or C6-C 13 Dicarboxylic acid derivatives, b-2) Based on the total amount of components b-1) and b-2), at least one dicarboxylic acid selected from terephthalic acid, franzicarboxylic acid, their derivatives, and mixtures thereof, in an amount of 80 to 30 mol%, Based on the total amount of b-3)b-1) and b-2), 98-102 mol% of aliphatic C3-C4 diols, b-4) Based on the total weight of components b-1), b-2), and b-3), 0 to 2% by weight of at least a trivalent alcohol, b-5) Based on the total weight of components b-1), b-2), and b-3), 0 to 2% by weight of a chain extender and It is derived from this.

[0046] Aliphatic C6-C 18 Aliphatic-aromatic polyesters are more preferred, in which the dicarboxylic acid and its derivatives b-1) are selected from adipic acid, azelaic acid, sebacic acid, 1,12-dodecanediic acid, brassic acid, their derivatives, and mixtures thereof; the aromatic dicarboxylic acid and aromatic dicarboxylic acid derivative b-2) are selected from terephthalic acid, 2,5-franzicarboxylic acid, their derivatives, and mixtures thereof; and the diol b-3) is 1,4-butanediol. The dicarboxylic acid derivatives are preferably C1-C4 alkyl esters, particularly methyl esters.

[0047] Aliphatic C6-C 18 dicarboxylic acids and their derivatives b-1) - Sebacic acid, its derivatives, and mixtures thereof, -Sebacic acid and / or its derivatives, and mixtures thereof, and one or more aliphatic C6-C selected from adipic acid, azelaic acid, 1,12-dodecanediic acid, brassic acid, their derivatives, and mixtures thereof. 18 A mixture containing dicarboxylic acid, - Adipic acid, its derivatives, and mixtures thereof, - Adipic acid and / or its derivatives, and mixtures thereof, and one or more aliphatic C6-C selected from sebaciic acid, azelaic acid, 1,12-dodecanediic acid, brassic acid, their derivatives, and mixtures thereof. 18 Mixture containing dicarboxylic acid Selected from, Aliphatic-aromatic polyesters are particularly preferred, in which the aromatic dicarboxylic acid and aromatic dicarboxylic acid derivative b-2) are selected from terephthalic acid, 2,5-franzicarboxylic acid, their derivatives, and mixtures thereof, and the diol b-3) is 1,4-butanediol. The dicarboxylic acid derivative is preferably a C1-C4 alkyl ester, particularly a methyl ester.

[0048] The biodegradable polyester b) may contain a branching agent as component b-4) containing at least three functional groups that can react with diols or dicarboxylic acids. Examples include at least trihydric alcohols such as glycerol, trimethylolpropane, trimethylolethane, pentaerythritol, polyethertriol, and sorbitol, or carboxylic acids and hydroxy acids or anhydrides containing three or more groups selected from carboxylic acid groups, carboxylic acid anhydride groups, and hydroxy groups, such as tartaric acid, citric acid, malic acid, trimesic acid, trimellitic acid, trimellitic anhydride, pyromellitic acid, and pyromellitic dianhydride, with trimethylolpropane, pentaerythritol, and glycerol being preferred, and trimethylolpropane and glycerol being particularly preferred. Component b-4) can be used to construct a biodegradable polyester having structural viscosity. The melt rheology is improved in that the biodegradable polyester is easier to process, for example, by melt solidification, making it easier to pull into a self-supporting film / sheet.

[0049] The concentration of at least trifunctional branching agent b-4) in the biodegradable polyester is 0 to 2% by weight based on the total weight of components b-1), b-2), and b-3) in the final polyester. When at least trifunctional branching agent b-4) is present in the biodegradable polyester, the concentration is usually 0.01 to 2% by weight, preferably 0.05 to 1% by weight, and particularly preferably 0.08 to 0.20% by weight, based on the total weight of components b-1), b-2), and b-3) in the final polyester.

[0050] Biodegradable polyester b) may contain a chain extender as component b-5). The chain extender is a polyfunctional and especially bifunctional isocyanate, isocyanurate, oxazoline, carboxylic acid anhydride, carbodiimide, or epoxide.

[0051] The term "epoxide" should be understood to specifically refer to epoxy-containing copolymers based on styrene, acrylic acid esters and / or methacrylic acid esters, preferably of the styrene-glycidyl ether-methyl methacrylate type. The epoxy group-containing units are preferably glycidyl (meth)acrylates. Copolymers having a glycidyl methacrylate content of more than 20% by weight, more preferably more than 30% by weight, and even more preferably more than 50% by weight are found to be particularly advantageous. Epoxy-containing copolymers of the above type are commercially available, for example, from BASF Resins BV under the brand name Joncryl® ADR. Joncryl® ADR 4468 and ADR 4400 are particularly useful as chain extenders.

[0052] The bifunctional isocyanate may be an aromatic diisocyanate or an aliphatic diisocyanate.

[0053] Examples of aromatic diisocyanates include torylene 2,4-diisocyanate, torylene 2,6-diisocyanate, 2,2'-diphenylmethane diisocyanate, 2,4'-diphenylmethane diisocyanate, 4,4'-diphenylmethane diisocyanate, naphthylene 1,5-diisocyanate, or xylylene diisocyanate. Of these, 2,2'-, 2,4'-, and also 4,4'-diphenylmethane diisocyanate are particularly preferred. Generally, the latter diisocyanates are used as mixtures. The diisocyanates may also contain small amounts, for example, up to 5% by weight of urethion groups, based on total weight, for capping the isocyanate groups.

[0054] The term “aliphatic diisocyanate” as used herein specifically refers to linear or branched alkylene diisocyanates or cycloalkylene diisocyanates having 2 to 20 carbon atoms, preferably 3 to 12 carbon atoms, such as 1,6-hexamethylene diisocyanate, 1,5-pentamethylene diisocyanate, isophorone diisocyanate, or methylenebis(4-isocyanatocyclohexane). Particularly preferred aliphatic diisocyanates are isophorone diisocyanate and especially 1,6-hexamethylene diisocyanate.

[0055] Preferred isocyanurates include alkylene diisocyanates or cycloalkylene diisocyanates having 2 to 20 carbon atoms, preferably 3 to 12 carbon atoms, such as isophorone diisocyanate or aliphatic isocyanurates derived from methylenebis(4-isocyanatocyclohexane). The alkylene diisocyanate may be linear or branched. Isocyanurates based on n-hexamethylene diisocyanate, such as cyclic trimers, pentamers, or higher-order oligomers of 1,6-hexamethylene diisocyanate, are particularly preferred.

[0056] 2,2'-Bisoxazolines are generally obtained by the process described in Angew. Chem. Int. Ed., Vol. 11 (1972), pp. 287-288. Particularly preferred bisoxazolines are those in which R1 is a single bond, a (CH2)z alkylene group (z=2, 3, or 4), such as methylene, 1,2-ethanediyl, 1,3-propanediyl, 1,2-propanediyl, or phenylene group. Particularly preferred bisoxazolines are 2,2'-bis(2-oxazoline), bis(2-oxazolinyl)methane, 1,2-bis(2-oxazolinyl)ethane, 1,3-bis(2-oxazolinyl)propane, or 1,4-bis(2-oxazolinyl)butane, especially 1,4-bis(2-oxazolinyl)benzene, 1,2-bis(2-oxazolinyl)benzene, or 1,3-bis(2-oxazolinyl)benzene.

[0057] Carbodiimides and polymeric carbodiimides are commercially available, for example, by Lanxess under the trademark Stabaxol®, by BASF Polyurethane GmbH under the trademark Elastostab®, or by Nisshinbo Chemical Inc. under the trademarks Carbodilite HMV-15CA or Carbodilite HMV-5CA-LC.

[0058] Examples include poly(4,4'-dicyclohexylmethanecarbodiimide) (Carbodilite® type), poly(isophoronecarbodiimide), poly(meth-tetramethylxylylenecarbodiimide) (Elastostab® type), poly(2,2',6,6'-tetraisopropyldiphenylenecarbodiimide) (Stabaxol® D), poly(2,4,6-triisopropyl-1,3-phenylenecarbodiimide) (Stabaxol® P-100), and poly(2,6-diisopropyl-1,3-phenylenecarbodiimide) (Stabaxol® P).

[0059] Preferably, the chain extender b-5) is selected from isophorone diisocyanate, 1,6-hexamethylene diisocyanate, 1,5-pentamethylene diisocyanate, 4,4-diphenylmethane diisocyanate, and epoxy-containing copolymers of the styrene-glycidyl ether-methyl methacrylate type, which are based on styrene, acrylic acid esters, and methacrylic acid esters.

[0060] The concentration of the chain extender b-5) is 0 to 2% by weight based on the total weight of components b-1), b-2), and b-3). If the chain extender b-5) is present, its concentration is in the range of 0.01% to 2% by weight based on the total weight of components b-1), b-2), and b-3).

[0061] The number-average molecular weight (Mn) of the aromatic-aliphatic polyester used as component b) is generally in the range of 5,000 to 100,000, preferably 10,000 to 75,000 g / mol, and more preferably 15,000 to 50,000 g / mol, measured in a hexafluoroisopropanol (HFIP) solution relative to a narrow polymethyl methacrylate (PMMA) standard at a molecular weight exclusion limit of 100-1,000,000 g / mol. The weight-average molecular weight (Mw) is generally in the range of 30,000 to 300,000, preferably 60,000 to 200,000 g / mol, and the Mw / Mn ratio is generally in the range of 1 to 6, preferably 2 to 4. The viscosity number is between 30 and 450 g / mL, preferably 50 to 400 g / mL. Here, and throughout this specification, the viscosity number (VN) is determined according to DIN 53728-3:1985-1 at 25°C using a solution of each polymer in a 50:50 w / w mixture of phenol and 1,2-dichlorobenzene. The melting point, measured at 23°C and 50% relative humidity by DSC at a heating rate of 20°C, is in the range of 85–150°C, preferably in the range of 95–140°C.

[0062] Polyesters suitable for use in polymer compositions generally have a yield of 0.5 to 40 cm² relative to EN ISO 1133 (190°C, 2.16 kgf). 3 10 minutes, preferably 0.8-15 cm 3 It has a melt volume rate (MVR) of 10 minutes.

[0063] Examples of biodegradable aliphatic-aromatic polyesters include poly(butylene-co-adipate-co-terephthalate) ("PBAT"), poly(butylene-co-sebacate-co-terephthalate) ("PBSeT"), poly(butylene-co-azelate-co-terephthalate) ("PBAzT"), poly(butylene-co-adipate-co-sebacinate-co-terephthalate) ("PBASeT"), poly(butylene-co-adipate-co-azelate-co-terephthalate) ("PBAAzT"), and poly(butylene-co-adipate-co-brazilate-co These are poly(butylene-co-azelate-co-sebasinate-co-terephthalate) ("PBABrT"), poly(butylene-co-azelate-co-brassate-co-terephthalate) ("PBAzSeT"), poly(butylene-co-azelate-co-brassate-co-terephthalate) ("PBAzBrT"), poly(butylene-co-brassate-co-sebasinate-co-terephthalate) ("PBBrSeT"), poly(butylene-co-azelate-co-2,5-furanoate) ("PBAzF"), and poly(butylene-co-sebacate-co-2,5-furanoate) ("PBSeF"). Poly(butylene-co-sebacate-co-terephthalate), poly(butylene adipate-co-terephthalate), poly(butylene azelate-co-terephthalate), poly(butylene adipate-co-sebacate-co-terephthalate), poly(butylene adipate-co-azelate-co-terephthalate), poly(butylene azelate-co-sebacate-co-terephthalate), and mixtures thereof are preferred. Poly(butylene-co-sebacate-co-terephthalate) is particularly preferred.

[0064] Biodegradable aliphatic-aromatic polyesters like those described above are commercially available, for example, from BASF under the trade name ecoflex®.

[0065] Aliphatic-aromatic polyester b) is preferably compostable at home. Compostability at home can be determined as described above.

[0066] The concentration of biodegradable polyester b) in the polymer composition is at least 15% by weight, preferably at least 20% by weight, and more preferably at least 25% by weight, based on the total weight of components a) and b). The maximum concentration of biodegradable polyester b) in the polymer composition is 90% by weight, preferably 85% by weight, more preferably 80% by weight, even more preferably 75% by weight, most preferably 65% ​​by weight, and particularly preferably 55% by weight, based on the total weight of components a) and b). The preferred concentration range of biodegradable polyester b) is 20-90% by weight and 15-85% by weight, more preferably 20-85% by weight and 20-80% by weight, even more preferably 25-75% by weight, most preferably 25-65% by weight, and particularly preferably 25-55% by weight, based on the total weight of components a) and b).

[0067] The total inclusion concentration of polylactic acid a) and biodegradable polyester b) in the polymer composition is preferably at least 10% by weight, more preferably at least 20% by weight, even more preferably 25% by weight, and particularly preferably 50% by weight, based on the total weight of components a) to f). The maximum concentration of polylactic acid a) and biodegradable polyester b) in the polymer composition is 100% by weight, based on the total weight of components a) to f).

[0068] The polymer composition may contain 0 to 40% by weight of at least one biodegradable polyester c) different from aliphatic-aromatic polyester b) based on components a) to f). Biodegradable polyester c) is preferably an aliphatic polyester. c-1) At least one aliphatic C4-C 18 Dicarboxylic acid or C4-C 18 Dicarboxylic acid derivatives, or mixtures thereof, Based on the total amount of b-3)c-1), 98-102 mol% of at least one aliphatic C2-C 10 Diol and, b-4) Based on the total weight of components c-1) and b-3), 0 to 2% by weight of at least a trivalent branching agent, b-5) Based on the total weight of components c-1) and b-3), 0 to 2% by weight of a chain extender and Polyester derived from, or c-6) At least one type of C2-C 18 Hydroxycarboxylic acid or C2-C 18 Hydroxycarboxylic acid derivatives, or mixtures thereof, b-4) Based on the total weight of component b-6), 0 to 2% by weight of at least trivalent alcohol, b-5) Based on the total weight of component b-6), 0-2% by weight of a chain extender and Polyester derived from It can be selected from the following.

[0069] Components b-3), b-4), and b-5) are the same as described above and are preferred for aliphatic-aromatic polyester b).

[0070] Aliphatic dicarboxylic acids (c-1) are at least one aliphatic C4-C 18 Dicarboxylic acid or C4-C 18 Selected from dicarboxylic acid derivatives or mixtures thereof. Aliphatic dicarboxylic acid c-1) is the above aliphatic C6-C 18 Dicarboxylic acid or C6-C 18 The dicarboxylic acid derivatives (b-1) are included, but the further includes aliphatic dicarboxylic acids having 4 to 7 C atoms. Examples of such dicarboxylic acids are succinic acid, 2-ethyl succinic acid, glutaric acid, 2-methylglutaric acid, 3-methylglutaric acid, 2,2-dimethylglutaric acid, diglycolic acid, adipic acid, pimelic acid, octadecanediic acid, oxaloacetate, glutamic acid, aspartic acid, itaconic acid and maleic acid, their derivatives, especially C1-C4 dialkyl esters, and mixtures thereof. More preferably, aliphatic C4-C 18 The dicarboxylic acid c-1) is selected from succinic acid, adipic acid, azelaic acid, sebacic acid, 1,12-dodecanoic acid, brassic acid, their derivatives, especially C1-C4 alkyl esters, and mixtures thereof, with succinic acid being particularly preferred.

[0071] C2-C 18 Hydroxycarboxylic acid or C2-C 18 The hydroxycarboxylic acid derivatives c-6) may be selected from glycolic acid, hydroxypropionic acid, hydroxybutanoic acid, hydroxyvaleric acid, hydroxyhexanoic acid, hydroxydecanoic acid, hydroxydodecanoic acid, hydroxyhexadecanoic acid, hydroxyoctadecanoic acid, γ-butyrolactone, and ε-caprolactone. Within the scope of this specification, polylactides are not included in b-6), and aliphatic polyesters derived from b-4) and / or b-5) as they may be.

[0072] Examples of polyester c) include polyhydroxyalkanoates, polyglycolic acid, polycaprolactone, and polybutyrolactone.

[0073] Polyhydroxyalkanoates, also known as polyhydroxy fatty acids, are understood in the context of this invention to mean polymers containing monomers with a chain length of at least three carbon atoms in their polymer backbone. Therefore, polylactic acid and polyhydroxyacetic acid (also known as polyglycolic acid) are not polyhydroxyalkanoates in the context of this invention. Polycaprolactone (PCL) is also not understood as a polyhydroxyalkanoate in the context of this invention.

[0074] According to the present invention, the repeating monomer unit of formula (1): [-O-CHR-(CH2)] m -CO-] (1) (In the formula, R is hydrogen, or a linear or branched alkyl group having 1 to 20 carbon atoms, preferably 1 to 16 carbon atoms, preferably 1 to 6 carbon atoms, and m = 1 to 18, preferably 1, 2, 3, 4, 5, and 6) It is preferable to use a homopolymer of at least one polyhydroxyalkanoate containing and / or 2-hydroxybutyric acid.

[0075] Polyhydroxy fatty acids include homopolymers, i.e., polyhydroxy fatty acids composed of identical hydroxy fatty acid monomers, and copolymers, i.e., polyhydroxy fatty acids composed of different hydroxy fatty acid monomers.

[0076] Examples of polyhydroxyalkanoates include polyhydroxybutyrate, polyhydroxybutyrate-valerate, polyhydroxybutyrate-propanoate, polyhydroxybutyrate-hexanoate, polyhydroxybutyrate-decanoate, polyhydroxybutyrate-dodecanoate, polyhydroxybutyrate-hexadecanoate, polyhydroxybutyrate-octadecanoate, and poly-3-hydroxybutyrate-4-hydroxybutyrate.

[0077] Poly-3-hydroxybutyrate is available from Tianan under the name Enmat®. Poly(3-hydroxybutyrate-co-4-hydroxybutyrate) was first developed by Metabolix and commercialized by CJ CheilJedang. Poly(3-hydroxybutyrate-co-3-hydroxyhexanoate) is commercially available from Kaneka (Aonilex®) or Danimer Scientific (Nodax®). Poly(3-hydroxybutyrate-co-3-hydroxyhexanoate) generally has a 3-hydroxyhexanoate content of 1 to 20, preferably 3 to 15 mol%, based on polyhydroxyalkanoate. Poly(hydroxybutyrate-co-hydroxyhexanoate), particularly poly(3-hydroxybutyrate-co-3-hydroxyhexanoate), is preferred.

[0078] The molecular weight Mw of polyhydroxyalkanoates is generally determined by GPC (Geomorphic Propagation) against a narrowly distributed PMMA standard in HFIP (hexafluoro-2-propanol) as a solvent, and is in the range of 100,000 to 1,000,000 g / mol, preferably in the range of 300,000 to 600,000 g / mol.

[0079] Polycaprolactone, more precisely poly-ε-caprolactone, is a class of linear aliphatic polyesters obtained by ring-opening polymerization of ε-caprolactone monomer under the catalytic action of a metal-organic compound (such as tetraphenyltin). Generally, polycaprolactone has a melting point of 59-64°C and a glass transition temperature of -60°C. Its structural repeating unit has five nonpolar methylene-CH2- and one polar ester group-COO-, i.e., -(COOCH2CH2CH2CH2CH2-)n. Due to this structure, polycaprolactone has good flexibility, processability, and good biocompatibility.

[0080] The number-average molecular weight of polycaprolactone is generally determined by GPC against a narrowly distributed PMMA standard in HFIP (hexafluoro-2-propanol) as a solvent, and is in the range of 40,000 to 100,000 g / mol, preferably in the range of 45,000 to 85,000 g / mol.

[0081] Polycaprolactone is commercially available, for example, under the product name Placel® by Daicel or under the product name Capa® by Ingevity.

[0082] Polyglycolic acid, also known as polyglycolide, is a biodegradable thermoplastic polymer and the simplest linear aliphatic polyester. It can be prepared by polycondensation starting from glycolic acid, or by ring-opening polymerization starting from glycolide.

[0083] Polyglycolic acid includes glycolic acid homopolymers consisting solely of glycolic acid repeating units represented by the formula -(O-CH2-CO)- (including ring-opening polymerization products of glycolide, which is a bicyclic ester of glycolic acid), and glycolic acid copolymers containing at least 70% by weight of the aforementioned glycolic acid repeating units.

[0084] Examples of comonomers for providing polyglycolic acid copolymers with glycolic acid monomers such as glycolides include, but are not limited to, ethylene oxalates (i.e., 1,4-dioxane-2,3-dione); lactides; cyclic monomers containing lactones such as β-propiolactone, β-butyrolactone; pivalolactone, γ-butyrolactone, δ-valerolactone, β-methyl-δ-valerolactone, and ε-caprolactone; carbonates such as trimethylene carbonate; ethers such as 1,3-dioxane; ether esters such as dioxanone; and amides such as ε-caprolactam; hydroxycarboxylic acids such as lactic acid, 3-hydroxypropanoic acid, 4-hydroxybutanoic acid, and 6-hydroxycaproic acid, and their alkyl esters; substantially equimolar mixtures of aliphatic diols such as ethylene glycol and 1,4-butanediol with aliphatic dicarboxylic acids such as succinic acid and adipic acid, and their alkyl or aromatic esters; and two or more of these. These monomers may be substituted with the polymer, which can be used as a starting material to provide polyglycolic acid copolymers together with the aforementioned glycolic acid monomers such as glycolide.

[0085] Preferably, the biodegradable polyester c) is selected from polycaprolactone (PCL), polybutylene succinate-co-adipate (PBSA), polybutylene succinate-co-sebacate (PBSSe), polybutylene succinate-co-azelate (PBSAz), and polybutylene succinate (PBS).

[0086] If the polymer composition contains one or more biodegradable polyesters c), their concentration is at least 1% by weight, preferably at least 2% by weight, and more preferably at least 5% by weight, based on components a) to f). The maximum concentration is 40% by weight, preferably 20% by weight, and more preferably 10% by weight, based on components a) to f).

[0087] The polymer composition contains 0 to 55% by weight of at least one starch or cellulose-based polymer d) based on components a) to f).

[0088] As used herein, the term “starch-based polymer” means starch itself and polymers derived from starch.

[0089] Starch is a natural polymer composed of amylose and amylopectin. Amylose is essentially a linear polymer with a molecular weight in the range of 100,000 to 500,000, while amylopectin is a highly branched polymer with a molecular weight of up to several million. Starch is produced in many plants, but typical sources include the seeds of cereals such as maize, waxy corn, wheat, sorghum, rice, and glutinous rice; tubers such as potatoes; roots such as tapioca (i.e., cassava and manioc), sweet potatoes, and arrowroot; and the pith of the sago palm. Broadly speaking, any natural (unmodified) and / or modified starch can be used as component c) in a polymer composition. For example, modified starch, which has been chemically modified by typical processes known in the art (e.g., esterification, etherification, oxidation, acid hydrolysis, enzymatic hydrolysis, etc.), is often used. Starch ethers and / or esters such as hydroxyalkyl starch and carboxymethyl starch may be particularly desirable. The hydroxyalkyl group of hydroxyalkyl starch may contain, for example, 2 to 10 carbon atoms, 2 to 6 carbon atoms in some embodiments, and 2 to 4 carbon atoms in some embodiments. Typical hydroxyalkyl starches include, for example, hydroxyethyl starch, hydroxypropyl starch, hydroxybutyl starch, and their derivatives. For example, starch esters can be prepared using a wide variety of anhydrides (e.g., acetic acid, propionic acid, butyric acid, etc.), organic acids, acid chlorides, or other esterification reagents. The degree of esterification can vary as desired, for example, 1 to 3 ester groups per starch glucoside unit.

[0090] Thermoplastic starches contain plasticizers that help make starch melt-processable. For example, starch usually exists in the form of granules with a coating or outer film, which encapsulates more water-soluble amylose and amylopectin chains within the granules. When heated, the plasticizer softens and penetrates the outer film, allowing the internal starch chains to absorb water and swell. This swelling can cause the outer shell to rupture at some point, resulting in the irreversible structural collapse of the starch granules. Once structural collapse occurs, the starch polymer chains containing amylose and amylopectin polymers, which were initially compressed within the granules, stretch, forming a disordered mixture of polymer chains. However, upon re-solidification, the chains can re-orient themselves, forming crystalline or amorphous solids with varying strengths depending on the orientation of the starch polymer chains. Thus, since starch can melt and re-solidify at certain temperatures, it is generally considered a "thermoplastic starch."

[0091] Suitable plasticizers include, for example, water, polyhydric alcohol plasticizers such as sugars (e.g., glucose, sucrose, fructose, raffinose, maltodextrose, galactose, xylose, maltose, lactose, mannose, and erythrose), sugar alcohols (e.g., erythritol, xylitol, malitol, mannitol, and sorbitol), and polyols (e.g., ethylene glycol, glycerol, polyglycerol, propylene glycol, dipropylene glycol, butylene glycol, and hexanetriol). If the starch particles contain a sufficiently large amount of water, the water present in the starch particles can also be used as a plasticizer. Hydrogen-bonding organic compounds that do not have hydroxyl groups are also suitable, and these include urea and urea derivatives; anhydrous sugar alcohols such as sorbitan; animal proteins such as gelatin; plant proteins such as sunflower protein, soy protein, and cotton seed protein; and mixtures thereof. Other suitable plasticizers include phthalates, dimethyl succinate and diethyl succinate, and related esters, glycerol triacetates, glycerol mono and diacetates, glycerol mono, di and trippropionates, butanoates, stearates, lactic acid esters, citrate esters, adipic acid esters, stearic acid esters, oleic acid esters, and other acid esters. Aliphatic acids such as copolymers of ethylene and acrylic acid, polyethylene grafted with maleic acid, polybutadiene-co-acrylic acid, polybutadiene-co-maleic acid, polypropylene-co-acrylic acid, polypropylene-co-maleic acid, and other hydrocarbon acids can also be used. Low molecular weight plasticizers are preferred, for example, less than about 20,000 g / mol, preferably less than about 5,000 g / mol, and more preferably less than about 1,000 g / mol. Preferred plasticizers are water, glycerol, oligoglycerol, sorbitol, and hydrolyzed hydrogenated starch syrup (CAS 68425-17-2).

[0092] The relative amounts of starch and plasticizer used in thermoplastic starch can vary depending on various factors such as the desired molecular weight, the type of starch, and the affinity of the plasticizer to the starch. However, starch typically constitutes about 30% to 95% by weight of the thermoplastic starch, about 40% to 90% by weight in some embodiments, and about 50% to 85% by weight in some embodiments. Similarly, plasticizer typically constitutes about 5% to 55% by weight of the thermoplastic composition, about 10% to 45% by weight in some embodiments, and about 15% to 35% by weight in some embodiments. Different composition ranges may be more suitable depending on the intended use of the polymer composition (see below).

[0093] Starch polymer d) may be selected from wheat flour, natural starch, modified starch, hydrolyzed starch, structurally disintegrated starch, gelatinized starch, plasticized starch, thermoplastic starch, complex starch containing biofillers, and mixtures thereof.

[0094] Preferably, the starch polymer used as component d) is selected from natural starch, more preferably from corn starch, potato starch, tapioca starch, pea starch, wheat starch, or rice starch, most preferably from natural corn starch or wheat starch, and particularly preferably from corn starch.

[0095] Preferably, the polymer composition contains at least one starch polymer d). In this case, the concentration of starch polymer d) is usually at least 2% by weight, preferably at least 5% by weight, more preferably 10% by weight, even more preferably at least 25% by weight, most preferably at least 30% by weight, and particularly preferably at least 35% by weight, based on the total weight of components a) to f) of the polymer composition. The maximum concentration of starch polymer d) is usually 55% by weight, preferably 50% by weight, and more preferably 45% by weight, based on the total weight of components a) to f) of the polymer composition. The preferred concentration range of starch polymer d) is 2 to 55% by weight, more preferably 10 to 50% by weight, even more preferably 25 to 50% by weight, most preferably 30 to 45% by weight, and particularly preferably 35 to 45% by weight, based on the total weight of components a) to f) of the polymer composition. Depending on the specific application field of the film prepared from the polymer composition, different concentration ranges of starch polymer d) may be preferred.

[0096] As used herein, the weight of starch polymer refers to the total weight of the starch polymer itself and any plasticizers present, and does not include water.

[0097] As used herein, the term “cellulose-based” means cellulose itself and polymers derived from cellulose, such as cellulose hydrate, also known as “cellophane,” or partially hydrolyzed cellulose acetate.

[0098] The polymer composition may contain at least one inorganic filler f) in an amount of 0 to 40% by weight based on components a) to f). The filler may be selected from alkaline earth metal salts, silicic acid and its salts, silica gel, silicates, silicon dioxide (quartz), bentonite, graphite, carbon black, iron oxide, kaolin, sodium carbonate, titanium dioxide, wollastonite, mica, bentonite, montmorillonite, and mineral fibers.

[0099] Alkaline earth salts include sulfates such as natural gypsum, natural anhydrous gypsum, and gypsum (CaSO4 hydrate) in different forms such as gypsum prepared from exhaust gases; halides such as calcium chloride; carbonates such as dolomite (MgCa(CO3)2) or chalk (CaCO3); phosphates such as calcium phosphate, e.g., apatite, and monobasic, dibasic, and tribasic phosphates of Mg; silicates; and talc (Mg3Si4O 10 Examples include (OH)2) and hydrates of the aforementioned salts such as gypsum.

[0100] Preferred inorganic fillers e) are talc and CaCO3, which can be used alone or in mixtures.

[0101] If inorganic filler e) is present in the polymer composition, the concentration of the inorganic filler is at least 2% by weight, preferably at least 5% by weight, based on the total weight of the polymer composition. The maximum concentration of the inorganic filler is typically 40% by weight, preferably 35% by weight, and more preferably 30% by weight, based on the total weight of components a) to f) of the polymer composition. Different compositional ranges may be more suitable depending on the intended use of the polymer composition (see below).

[0102] Calcium carbonate can be used in amounts of, for example, 10 to 30% by weight, preferably 10 to 28% by weight, and more preferably 12 to 20% by weight, based on the total weight of components a) to f) of the polymer composition. Calcium carbonate from Omya will prove to be particularly suitable. The average particle size of calcium carbonate measured with Malvern Mastersizer X is generally in the range of 0.2 to 10 micrometers, preferably 0.5 to 5, and more preferably 0.5 to 2.5 micrometers.

[0103] Talc can be used in amounts of, for example, 3 to 30% by weight, preferably 5 to 10% by weight, and more preferably 5 to 8% by weight, based on the total weight of components a) to f) of the polymer composition. Talc from Imerys and Elementis is found to be particularly suitable.

[0104] The polymer composition may contain, as component f), at least one compound selected from crosslinking agents, chain extenders, stabilizers, nucleating agents, lubricants, mold release agents, surfactants, waxes, antistatic agents, antifogging agents, dyes, pigments, UV absorbers, UV stabilizers, oxygen scavengers, dispersants, and other plastic additives in an amount of 0 to 40% by weight based on components a) to f).

[0105] Examples of branching agents and chain extenders are the compounds listed in b-4) and b-5), with preferred branching agents and chain extenders being epoxy-containing copolymers based on styrene, acrylic acid esters, and methacrylic acid esters, preferably of the styrene-glycidyl ether-methyl methacrylate type, and carbodiimides, with epoxy-containing copolymers based on styrene, acrylic acid esters, and methacrylic acid esters, preferably of the styrene-glycidyl ether-methyl methacrylate type, being particularly preferred. Preferably, the polymer composition contains 0.05 to 1% by weight, preferably 0.05 to 0.2% by weight, of the epoxy-containing copolymer based on styrene, acrylic acid ester, and / or methacrylic acid ester, based on the total weight of components a) to f) of the polymer composition. Epoxy-containing copolymers of the above type are commercially available, for example, from BASF Resins BV under the brand name Joncryl® ADR. Joncryl® ADR 4468 and Joncryl® ADR 4400 are particularly suitable.

[0106] Examples of slip agents and release agents include C, such as stearamide, oleamide, ercamid, and behenamide. 18 -C 24 -Carboxamide, and stearates such as calcium stearate. Preferably, the polymer composition contains 0.05% to 1% by weight of C based on the total weight of components a) to f) of the polymer composition. 18 -C 24 -Carboxamide, preferably selected from stearamide, erucamide, and behenamide, or mixtures thereof.18 -C 24 -Contains carboxamide.

[0107] Examples of surfactants include polysorbates, palmitates, and laurates.

[0108] Examples of UV absorbers include 2-(4,6-bis-biphenyl-4-yl-1,3,5-triazine-2-yl)-5-(2-ethyl-(n)-hexyloxy)phenol and carbon black. The preparation and properties of these UV absorbers are known from International Publication No. 2009 / 071475.

[0109] An example of a dispersant is polyvinyl alcohol (PVOH).

[0110] Component f) is generally used at a concentration of 0 to 40% by weight, preferably 0 to 40% by weight, more preferably 0.05 to 40% by weight, even more preferably 0.1 to 40% by weight, and particularly preferably 0.1 to 35% by weight, based on the total weight of components a) to f) of the polymer composition.

[0111] Surprisingly, the addition of a compostable aliphatic-aromatic polyester b) to non-compostable PLA improves the compostability of the PLA, resulting in biodegradability under composting conditions even in compositions containing large amounts of PLA. The polymer compositions described herein are compostable even in compositions containing, for example, 60, 70, or 80% by weight of PLA and only 40, 30, or 20% by weight of a compostable aliphatic-aromatic polyester b) when PLA constitutes the main phase. Such compositions may even exhibit faster biodegradation under composting conditions than pure polybutyl sebacate-co-terephthalate, as demonstrated in the example using polybutyl sebacate-co-terephthalate. The addition of a biodegradable aliphatic-aromatic polyester b) to non-compostable PLA enables composting of the PLA and improves the compostability of the PLA so that the entire resulting polymer composition is compostable. A polymer composition in which the matrix phase is formed of PLA or a PLA-containing composition is preferred.

[0112] The polymer compositions are compostable in their own state, and the addition of further compounds to promote biodegradation, such as dicarboxylic acids or metal elements, or adherence to certain concentration limits of such compounds, is not required. The polymer compositions described herein can be used at concentrations of metal elements less than 50 ppm and greater than 500 ppm, for example, at zinc concentrations less than 50 ppm and greater than 500 ppm, at zinc and calcium concentrations less than 50 ppm and greater than 500 ppm, or at concentrations of metal elements selected from sodium, magnesium, aluminum, potassium, calcium, barium, zinc, iron, copper, and tin less than 50 ppm and greater than 500 ppm. The polymer compositions described herein can also be used without aliphatic dicarboxylic acids or their salts, or aliphatic dicarboxylic acid anhydrides, at concentrations of 0.1 to 10% by weight based on the total weight of the composition. For example, the polymer composition described herein can be used without containing sebaciic acid, adipic acid, glutaric anhydride, or ammonium sebacate at a concentration of 0.1 to 10% by weight based on the total weight of the composition.

[0113] Preferably, the polymer composition is compostable in accordance with ISO 14855-1 (2012), determined by the polymer composition particles having a particle size of 100 to 300 microns, and achieving 90% absolute or relative CO2 emissions within 365 days at a temperature within the range of 25+ / -5°C.

[0114] Methods for producing the above-mentioned compostable polymer composition are known to those skilled in the art and include, for example, physical mixing in an extruder, and preferably the polymer composition is prepared by melt mixing.

[0115] Household compostable polymer compositions can be used to manufacture household compostable articles. Such household compostable articles may be in the form of single-layer films, multilayer films comprising at least one layer containing the polymer composition, injection-molded articles, thermoformed articles, fibers, or articles having a coating containing the polymer composition. For example, household compostable articles may be bags, agricultural or horticultural articles, flexible or rigid packaging articles, tableware, cutlery, nonwoven articles, foams, or expandable beads for foaming.

[0116] Examples of bags include garbage bags, especially organic garbage bags, fruit and vegetable bags, and consumer bags. Examples of agricultural or horticultural articles include root covering films, clips, twisted yarns, and planters. Examples of flexible or rigid packaging include packaging for dry compounds and liquids, especially food packaging for, for example, coffee, tea, soup powder, sauce powder, ice cream, confectionery (e.g., chocolate bars and mues bars), yogurt pots, fruit boxes, and meal trays; food or beverage containers for carrying food and frozen foods, such as bottles, clamshells, pots, cups, drink cartons, cartons, wrapping paper, and sachets; personal care packaging such as cosmetics and detergents; medical article packaging; and agricultural packaging. Examples of tableware and cutlery include disposable tableware such as cups, plates, and cutlery. Examples of foams include extruded foams and bead foams, and articles may also be nets or fabrics such as tea bags or sanitary articles, containing fibers, monofilaments, multifilaments, staple fibers, or such fibers.

[0117] Methods for producing compostable articles from compostable polymer compositions are known to those skilled in the art, and include, among others, extrusion, single-layer and multi-layer inflation film extrusion, cast film extrusion, extrusion coating, injection molding, injection blow molding, thermoforming, cast film extrusion / thermoforming, extrusion blow molding, and calendering / thermoforming.

[0118] Home compostable polymer compositions can also be used to produce home compostable fibers and nonwoven fabrics, for example, by carding, airlaid, wetlaid, spunbond, meltblowing, and electrospinning.

[0119] The household compostable polymer composition can be used to manufacture a household compostable article comprising a base layer and at least one layer containing the polymer composition, i.e., a household compostable article containing the multilayer film described above. The base layer may be selected from nonwoven fabric made of fibers, another polymer layer, paper, cardboard, board, and / or metal film.

[0120] The fibers of the nonwoven fabric used as the base material may be natural fibers or synthetic fibers of natural polymers. Natural fibers are typically cellulose fibers. Cellulose fibers may be obtained from plant sources such as wood, rugs, grasses, silphie, and bagasse, as well as from recycled cellulose fiber-containing materials such as paper. Synthetic fibers of natural polymers can be obtained by chemical treatment of natural polymers such as cellulose and chitin. A preferred synthetic fiber of natural polymers is viscose (which can be obtained by chemical treatment of cellulose). The thickness of such a preferred base material layer is preferably in the range of 10 μm to 500 μm, more preferably in the range of 30 μm to 300 μm. Nonwoven fabrics may be obtained by common prior art papermaking techniques or other wet techniques. Nonwoven fabric base materials may also be obtained by dry fiber forming processes or dry pulp forming processes.

[0121] Preferably, the base material is selected from paper, cardboard, paperboard, or fiberboard. Suitable fibers for the production of the paper products include all commonly used types, such as mechanical pulp, bleached and unbleached chemical pulp, papermaking pulp from any annual crop, and recycled paper (including waste paper, whether coated or uncoated). The above fibers can be used alone or in any mixture thereof to produce pulp from which paper products are made. For example, the term wood pulp includes wood pulp, thermomechanical pulp (TMP), chemothermetic pulp (CTMP), compressed wood pulp, semi-chemical pulp, high-yield chemical pulp, and refiner pulp (RMP). Exemplary chemical pulps include sulfuric acid pulp, sulfite pulp, and soda pulp. Examples of annual plants suitable for pulp production include rice, wheat, sugarcane, and kenaf.

[0122] A household compostable article comprising a base layer and at least one layer containing or consisting of the above-mentioned polymer composition may be manufactured by known techniques commonly applied in the field of packaging, such as heat pressing, injection molding, co-injection molding, extrusion, particularly co-extrusion, cast film extrusion, or inflation film extrusion, lamination, adhesive bonding, and vapor deposition.

[0123] A household compostable article comprising a base layer and at least one layer containing or consisting of the above-mentioned polymer composition may be processed by known techniques commonly applied in the field of packaging, such as thermoforming, sealing, folding, embossing, stenciling, printing, lamination, in-mold labeling, adhesive bonding, coating (e.g., spray coating, gravure or reverse gravure coating, roller coating, flexographic coating, air knife coating, dip coating, slot die coating, curtain coating, screen coating, extrusion coating), and corona treatment.

[0124] The polymer compositions described herein are particularly suitable for use in the method for coating paper and cardboard described herein, in whole, in European Patent Application Publication No. 2331602(A1).

[0125] Paper, cardboard, or paperboard containing layers made of the above polymer composition is particularly well suited for the manufacture of paper bags for dry foods such as coffee, tea, soup powder, and sauce powder; paper bags for liquids such as coffee or tea cups, coffee or tea capsules, cosmetics, cleaning agents, and beverages; tube laminates; paper carry bags; paper laminates and co-extrudeds for ice cream and confectionery (e.g., chocolate bars and mues bars); paper adhesive tapes; cardboard cups (paper cups), yogurt pots; meal trays; rolled cardboard containers (cans, drums); wet-strength cartons for outer packaging (wine bottles, food); coated cardboard fruit boxes; fast food plates; clamshells; beverage cartons, as well as cartons for liquids such as detergents and cleaning agents, frozen food cartons, ice packaging (e.g., ice cups, wrapping material for cone-shaped ice cream wafers); paper labels; flower pots and planters.

[0126] Another object of the present invention is a process for producing compostable articles for home use, (i) A step of preparing a household compostable polymer composition as defined above, (ii) Depending on the case, a step of processing the polymer composition, (iii) A process for producing a household compostable article comprising a polymer composition obtained after step (i) or (ii). This is a process that includes [something].

[0127] The technologies that can be used in process (iii) are listed above.

[0128] A further object of the present invention is a method for producing a household compostable article containing polylactic acid, b-1) Based on the total amount of components b-1) and b-2), 20-70 mol% of at least one aliphatic C6-C 18 Dicarboxylic acid or C6-C 18 Dicarboxylic acid derivatives, b-2) Based on the total amount of components b-1) and b-2), 80 to 30 mol% of at least one aromatic dicarboxylic acid or aromatic dicarboxylic acid derivative, Based on the total amount of b-3)b-1) and b-2), 98-102 mol% aliphatic C2-C 10 Diol and, b-4) Based on the total weight of components b-1), b-2), and b-3), 0 to 2% by weight of at least a trivalent alcohol, b-5) Based on the total weight of components b-1), b-2), and b-3), 0 to 2% by weight of a chain extender and This method involves adding at least one biodegradable aliphatic-aromatic polyester derived from to polylactic acid.

[0129] Preferred polyesters b) and polylactic acid a) are those described above.

[0130] Another objective of the present invention is to improve the compostability of polylactic acid at home. b-1) Based on the total amount of components b-1) and b-2), 20-70 mol% of at least one aliphatic C6-C 18 Dicarboxylic acid or C6-C 18 Dicarboxylic acid derivatives, b-2) Based on the total amount of components b-1) and b-2), 80 to 30 mol% of at least one aromatic dicarboxylic acid or aromatic dicarboxylic acid derivative, Based on the total amount of b-3)b-1) and b-2), 98-102 mol% aliphatic C2-C 10 Diol and, b-4) Based on the total weight of components b-1), b-2), and b-3), 0 to 2% by weight of at least a trivalent alcohol, b-5) Based on the total weight of components b-1), b-2), and b-3), 0 to 2% by weight of a chain extender and This involves the use of domestically compostable aliphatic-aromatic polyesters derived from [source].

[0131] Preferred polyesters b) and polylactic acid a) are those described above.

[0132] It is assumed that those skilled in the art can utilize the above description in the broadest sense without further description. Therefore, preferred embodiments and examples should be interpreted solely as descriptive frameworks, without any limiting effect.

[0133] Examples: material: cellulose Polylactic acid (PLA): Ingeo 3251 D (NatureWorks LLC) Poly(butylene-co-sebacate-co-terephthalate) (PBSeT): According to EN ISO 1133 (190℃, 2.16 kgf), Se:T ratio is 52:48, MVR is 6+ / -2cm². 3 / 10 minutes of PBSeT

[0134] Preparation of polymer compositions: All blends were prepared by extrusion at a rotational speed of 300 rpm using a Coperion ZSK 26 MC twin-screw extruder (11 zones; zone 2 = 140°C, zones 3-11 = 190°C). Individual components were added in zone 1 using separate weight scales and melted and mixed in the following zones. The polymer molten material was degassed in zone 9 at 600 mbar. The die plate temperature was 215-225°C. The resulting compound was formed into strand pellets. The amounts of polymer components forming the blends of Comparative Examples CE1 and CE2 and Examples IE1 and IE2 of the present invention are summarized in Table B below. The amounts of blend components are given as weight % based on the total weight of the blend.

[0135] The composition is shown in Table 1. The concentration is given in weight percent. [Table 1]

[0136] Sample preparation for biodegradation testing: Plastic samples were cryogenically ground and sieved using a Retsch ZM 300 ultracentrifuge mill. Isolated fractions with a size of less than 0.5 mm were collected and dried in a vacuum oven at 36°C for 48 hours. Subsequently, particles with a size of 100 μm to 300 μm were sieved using a Retsch AS 200 machine. Biodegradable / home compostable:

[0137] To demonstrate biodegradability under home composting conditions, a scaled-down and adapted version of the standard ISO 14855—Determination of the ultimate aerobic biodegradability of plastic materials under controlled composting conditions—Method by analysis of evolved carbon dioxide—was used. Biodegradation experiments were conducted using an ECHO instruments respiratory meter, and the generated carbon dioxide was measured by IR-based measurement. The reactor was a 1L size (pressure DURAN laboratory glass bottle) closed with a cap having one air inlet and one air outlet. During incubation, air saturated with 100% moisture was blown in through the inlet over the compost from a distance of approximately 5 cm, then flowed through the outlet and then reached the measurement unit. For each reactor, 118.8 g of 20-week-old OWS Belgium compost (sieve fraction less than 0.5 cm) was mixed with 1.2 g of 2-week-old compost (sieve fraction less than 0.5 cm) and 8 g of the test material. A blank, positive control, and each material were tested in triplicates. The samples were incubated at 28°C ± 2°C for at least 176 days. During the experiment, the reactor was opened periodically, and the contents were mixed twice during the first week and once per week thereafter. The results are shown in Table 2. Biodegradation is given as a percentage of decomposition.

[0138] Equivalent measurements were performed using a static system in which blank compost (3 reactors), positive control and compost (3 reactors), and test material and compost (3 reactors) were tested. Each replicate test contained 49.5 g of 20-week-old OWS Belgium compost (sieve fraction less than 0.5 cm) mixed with 1.2 g of 2-week-old compost (fraction less than 0.5 cm). 3.33 g of test material (or positive control) was mixed with the compost in each bottle. The compost had a total solids content of approximately 52.5%, a volatile solids content of more than 30% relative to dry solids, and a pH of 7.0–9.0. A plastic cup was placed in a 1750 mL container (Weck jar) along with two other cups; the first cup contained 15 mL of Millipore water to adjust humidity, and the second cup contained 32 mL of 1 M NaOH used as a CO2 absorbent. The reactor was sealed airtight and incubated at 28°C ± 2°C.

[0139] During the first week, the CO2 absorbent was replaced with a fresh 1M NaOH solution, and the reactor was aerated daily. Compost was mixed in on days 3 and 7. From the second week onward, the absorbent was replaced, the reactor was aerated three times a week, and compost was mixed in once a week. The amount of carbon dioxide produced during incubation was determined using the CO2 absorbent removed from the experiment. The carbon concentration in the solution was measured using a Shimadzu Total Organic Carbon Analyzer. The results are incorporated in Table 2.

[0140] The degree of mineralization is the amount of carbon in the absorbent solution of the test material.

number

number

number

[0141] [Table 2]

[0142] Compositions containing 90-100% by weight of PLA and up to 10% by weight of PBSeT hardly decompose under home composting conditions, while compositions containing more than 10% by weight of polybutylene-co-sebacate-terephthalate and less than 90% by weight of polylactic acid show strong biodegradation under home composting conditions. Compositions containing both PLA and PBSeT with a PLA concentration of less than 90% by weight decompose even faster than pure PBSeT. This is an indicator of the synergistic effect of PLA and PBSeT mixtures on biodegradability.

Claims

1. For manufacturing household compostable materials, a) 15 to 85% by weight of at least one polylactic acid a) based on the total weight of polylactic acid a) and aliphatic-aromatic biodegradable polyester b), b) 15 to 85% by weight of at least one biodegradable aliphatic-aromatic polyester (b) derived from the following, based on the total weight of the polylactic acid a) and the aliphatic-aromatic biodegradable polyester b): b-1) 20 to 70 mol% of at least one aliphatic C based on the total amount of components b-1) and b-2). ６ -C １８ Dicarboxylic acid or C ６ -C １８ Dicarboxylic acid derivatives, b-2) Based on the total amount of components b-1) and b-2), 80 to 30 mol% of at least one aromatic dicarboxylic acid or aromatic dicarboxylic acid derivative, Based on the total amount of b-3), b-1), and b-2), 98 to 102 mol% of aliphatic C ２ -C １０ Diol, b-4) 0 to 2% by weight of at least trivalent alcohols based on the total weight of components b-1), b-2), and b-3), and b-5) A chain extender in an amount of 0 to 2% by weight based on the total weight of components b-1), b-2), and b-3), c) 0 to 40% by weight of at least one biodegradable polyester different from the biodegradable aliphatic-aromatic polyester b) based on the constituent components a) to f), d) 0 to 55% by weight of at least one starch-based polymer or cellulose-based polymer based on the constituent components a) to f), e) At least one inorganic filler in an amount of 0 to 40% by weight based on the constituent components a) to f), f) 0 to 40% by weight of at least one compound selected from crosslinking agents, chain extenders, stabilizers, nucleating agents, lubricants, mold release agents, surfactants, waxes, antistatic agents, antifogging agents, dyes, pigments, UV absorbers, UV stabilizers, oxygen scavengers, dispersants, and other plastic additives, based on components a) to f). Use of polymer compositions containing the above.

2. The biodegradable polyester b) is, Based on the total amount of components b-1) and b-2), 20 to 70 mol% of at least one aliphatic C ６ -C １３ dicarboxylic acid or C ６ -C １３ dicarboxylic acid derivative, and b-2) Based on the total amount of components b-1) and b-2), at least one dicarboxylic acid selected from terephthalic acid, franzicarboxylic acid, their derivatives, and mixtures thereof, in an amount of 80 to 30 mol%, Based on the total amount of b-3), b-1), and b-2), 98 to 102 mol% of aliphatic C ３ -C ４ Diol and, b-4) Based on the total weight of components b-1), b-2), and b-3), 0 to 2% by weight of at least a trivalent alcohol, b-5) 0 to 2% by weight of a chain extender based on the total weight of components b-1), b-2), and b-3) The use according to claim 1, derived from the above.

3. The use according to claim 1 or 2, wherein the biodegradable polyester b) is selected from poly(butylene sebacate-co-terephthalate), poly(butylene adipate-co-terephthalate), poly(butylene azelate-co-terephthalate), poly(butylene adipate-co-sebacate-co-terephthalate), poly(butylene adipate-co-azelate-co-terephthalate), poly(butylene azelate-co-sebacate-co-terephthalate), and mixtures thereof.

4. The use according to any one of claims 1 to 3, wherein, based on the total weight of the polylactic acid a) and the aliphatic-aromatic biodegradable polyester b), the concentration of the polylactic acid a) is in the range of 10% to 80% by weight, and the concentration of the biodegradable aliphatic-aromatic polyester b) is in the range of 20% to 90% by weight.

5. The use according to any one of claims 1 to 4, wherein the total concentration of the polylactic acid a) and the biodegradable polyester b) in the polymer composition is 10 to 100% by weight based on the total weight of the constituent components a) to f).

6. The polymer composition is determined by the particles of the polymer composition having a particle size of 100 to 300 microns, and 90% of the absolute or relative CO2 is removed within 365 days at a temperature within the range of 25 ± 5°C. ２ The use according to any one of claims 1 to 5, which is compostable in a home environment in accordance with ISO 14855-1 (2012), reaching the point of generation.

7. The use according to any one of claims 1 to 6, wherein the household compostable article is a single-layer film, a multilayer film comprising at least one layer containing a household compostable polymer composition, an injection-molded article, a thermoformed article, a fiber, or an article having a coating containing a household compostable polymer composition.

8. The use according to any one of claims 1 to 7, wherein the household compostable article is a bag, an agricultural or horticultural article, a flexible or rigid packaging article, tableware, cutlery, a nonwoven article, a foam or expandable beads for foaming.

9. The use according to any one of claims 1 to 8, wherein the household compostable article comprises a base layer and at least one layer containing the household compostable polymer composition.

10. A process for producing compostable materials for home use, (i) A step of preparing a household compostable polymer composition according to any one of claims 1 to 6, (ii) Depending on the case, a step of processing the polymer composition, (iii) A process for producing a household compostable article comprising the polymer composition obtained after step (i) or (ii). A process that includes this.

11. A method for producing a household compostable article containing polylactic acid, 15-85% by weight, b-1) 20 to 70 mol% of at least one aliphatic C based on the total amount of components b-1) and b-2). ６ -C １８ Dicarboxylic acid or C ６ -C １８ Dicarboxylic acid derivatives, b-2) Based on the total amount of components b-1) and b-2), at least 80 to 30 mol% of at least one aromatic dicarboxylic acid or aromatic dicarboxylic acid derivative, Based on the total amount of b-3), b-1), and b-2), 98 to 102 mol% of aliphatic C ２ -C １０ Diol and, b-4) Based on the total weight of components b-1), b-2), and b-3), 0 to 2% by weight of at least a trivalent alcohol, b-5) 0 to 2% by weight of a chain extender based on the total weight of components b-1), b-2), and b-3) This is achieved by adding at least one biodegradable aliphatic-aromatic polyester derived from to the polylactic acid, A method wherein the weight percentage is based on the total weight of the aliphatic-aromatic polyester and polylactic acid.

12. To improve the compostability of polylactic acid at home b-1) 20 to 70 mol% of at least one aliphatic C based on the total amount of components b-1) and b-2). ６ -C １８ Dicarboxylic acid or C ６ -C １８ Dicarboxylic acid derivatives, b-2) Based on the total amount of components b-1) and b-2), at least 80 to 30 mol% of at least one aromatic dicarboxylic acid or aromatic dicarboxylic acid derivative, Based on the total amount of b-3), b-1), and b-2), 98 to 102 mol% of aliphatic C ２ -C １０ Diol and, b-4) Based on the total weight of components b-1), b-2), and b-3), 0 to 2% by weight of at least a trivalent alcohol, b-5) 0 to 2% by weight of a chain extender based on the total weight of components b-1), b-2), and b-3) Use of biodegradable aliphatic-aromatic polyesters derived from [source].

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