Composition comprising polybutylene succinate and amorphous polyhydroxyalkanoate, and packaging containing same

Abstract

The invention relates to a portion capsule (10) comprising a composition containing polybutylene succinate (PBS) and at least one amorphous polyhydroxyalkanoate (aPHA) copolymer of 3-hydroxybutyric acid (3HB) and at least one comonomer other than 3-hydroxybutyric acid (3HB), wherein the mass fraction of polybutylene succinate (PBS), based on the total weight of the composition, is between 75 wt.% and 90 wt.%, wherein the mass fraction of the amorphous polyhydroxyalkanoate (aPHA) copolymer, based on the total weight of the composition, is between 10 wt.% and 25 wt.%, and wherein the mass fraction of the at least one comonomer other than 3-hydroxybutyric acid (3HB), based on the weight of the amorphous polyhydroxyalkanoate (aPHA) copolymer, is between 25 wt.% and 85 wt.%.

Description

[0001] Composition comprising polybutylene succinate and amorphous polyhydrooxyalkanoate, and packaging containing the same

[0002] The present invention relates to biodegradable polymer compositions, in particular for portion capsules. The invention relates to a composition, a portion capsule consisting of or comprising such a composition, and the use of such compositions for packaging a beverage base material, in particular coffee.

[0003] So-called capsule machines for preparing beverages or beverage components using a portion capsule containing a pre-portioned amount of a beverage starting material are enjoying increasing popularity due to their user-friendliness and the wide selection of available flavors. The beverage starting material can be, in particular, a coffee powder mix or tea. In these systems, hot water – usually under pressure – is generally introduced into a portion capsule to prepare a coffee or tea beverage by extraction. To introduce the hot water, the capsule is often pierced on one side (injection side). Various options are known for dispensing the brewed beverage, generally on the other side of the capsule (extraction side). On the one hand, there are systems in which piercing is also provided on the extraction side using appropriate perforation pins.On the other hand, systems are known in which an extraction-side boundary of the capsule is punctured or torn under the internal pressure during the brewing process. This can be achieved by means external to the capsule (located in the brewing chamber of the corresponding capsule machine) or internal to the capsule. Finally, there are also capsules that are already opened, meaning no puncturing or torn of the capsule wall or membrane is required to expel the beverage.

[0004] Consequently, portion capsules typically have to meet stringent requirements with regard to various parameters. For example, portion capsules must exhibit good mechanical properties, be easy to process, and be cost-effective to produce. For sensitive foods such as coffee, low oxygen and water vapor permeability is also desired to ensure the packaged goods can be stored for as long as possible without any loss of quality.

[0005] In order to meet these requirements, portion capsules are known from the prior art, for example from EP I 165 398 A1, which consist to a large extent of multi-layer films or multi-layer materials such as PET / Alu / PE or paper / PET / Alu / PE. The main disadvantage of such portion capsules is the waste generated after use and the problematic environmental impact, since the different materials cannot be separated, or at least not easily. The only possible disposal methods are therefore often thermal treatment, i.e. incineration, or landfill, where corresponding multi-layer materials can remain virtually unchanged for several hundred years.

[0006] Against this backdrop, there is a growing demand for packaging materials in general, and portion capsules in particular, to be disposed of in a more environmentally friendly manner after use. It is therefore desirable for packaging such as portion capsules to be biodegradable within a practical timeframe and thus decompose when released into the environment.

[0007] In recent years, a number of biodegradable polymers have been developed for technical and / or industrial applications, such as aliphatic polyester resins, polyvinyl alcohol, and polysaccharides. However, it has been shown that these materials degrade only slowly in soil, and even in compost, elevated temperatures are required for extensive biodegradation within a practically usable period of approximately three months, and in any case no longer than one year. Furthermore, the available biodegradable polymers often exhibit poorer and sometimes unsatisfactory material properties than the polymers commonly used in portion capsules for capsule machines, which has so far prevented their widespread use in these applications.

[0008] It is an object of the present invention to provide portion capsules which are characterized by particularly good biodegradability combined with mechanical properties which are advantageous for use as portion capsules, in particular with regard to weldability, pressure resistance and / or extensibility.

[0009] This object is achieved by a single-portion capsule, a method for producing a single-portion capsule, and the use of a composition for packaging a beverage starting material comprising the features of the independent claims. The dependent claims, the description, and the figures describe further developments and particular embodiments of the invention.

[0010] The object is achieved in particular by a portion capsule comprising a composition comprising i. polybutylene succinate, and ii. at least one amorphous polyhydroxyalkanoate copolymer of a) 3-hydroxybutanoic acid and b) at least one comonomer other than 3-hydroxybutanoic acid.

[0011] The mass fraction of polybutylene succinate is between 75 wt.% and 90 wt.%, based on the total weight of the composition. The mass fraction of polybutylene succinate is preferably between 76 wt.% and 88 wt.%, more preferably between 77 wt.% and 86 wt.%, even more preferably between 78 wt.% and 84 wt.%, most preferably between 79 wt.% and 81 wt.%, in each case based on the total weight of the composition. The mass fraction of amorphous polyhydroxyalkanoate copolymer is between 10 wt.% and 25 wt.%, likewise based on the total weight of the composition. The mass fraction of the at least one comonomer other than 3-hydroxybutanoic acid is between 25 wt.% and 85 wt.%, based on the weight of the amorphous polyhydroxyalkanoate copolymer.

[0012] In the event that the composition contains two or more amorphous polyhydroxyalkanoate copolymers, the above mass fractions apply to the total amount of all amorphous polyhydroxyalkanoate copolymers of component ii of the composition.

[0013] It has been found that the addition of at least one amorphous polyhydroxyalkanoate copolymer to polybutylene succinate can significantly improve the biodegradability of the resulting composition. Surprisingly, it has been shown that the mechanical properties of the resulting compositions relevant for packaging use, in particular the weldability, pressure resistance, and extensibility of the resulting compositions, are not unduly impaired compared to corresponding reference compositions without amorphous polyhydroxyalkanoate copolymer.

[0014] Without wishing to be limited to this explanation, the addition of the amorphous polyhydroxyalkanoate copolymer increases the amorphous portions in the composition, so that microorganisms in composting and / or fermentation have better opportunities to attack the composition, thereby accelerating the decomposition of the composition. With regard to the use of the compositions described herein for packaging a beverage starting material, in particular for producing portion capsules for the production of a beverage or beverage component by extraction with the addition of pressurized hot water, described in more detail below, it has surprisingly been found that the addition of amorphous polyhydroxyalkanoate copolymer to polybutylene succinate increases the flexibility of the resulting polymer blend to such an extent that cracking at sharp transitions of the portion capsules during welding processes can be prevented.The increased flexibility also prevents breakage during the brewing process and makes piercing the brewing chamber easier.

[0015] For the purposes of this text, "biodegradable" refers to the potential for decomposition of the composition by organisms (especially saprobiotics) or their enzymes. In particular, the term "biodegradable" for the purposes of this text may refer to biodegradability according to the European standard EN 13432 (from the end of 2021). Additionally or alternatively, it may refer to biodegradability according to the European standard EN 14995 (from the end of 2021). Thus, "biodegradable" refers in particular to "biodegradable according to EN 13432 and / or EN 14995."

[0016] Although the term "compostable" is often used synonymously, its meaning differs from the term "biodegradable." While "biodegradable" simply means that an organic material can be consumed (mineralized) by microorganisms, e.g., in soil, activated sludge, or water, "compostable" has the specific requirement that the organic material degrades under composting conditions, i.e., usually at elevated temperatures. For the purposes of this text, "industrial compostable" and "home compostable" mean compostable and home compostable, respectively, according to European standard EN 13432 (from the end of 2021) for packaging and / or according to European standard EN 14995 (from the end of 2021) for plastics / synthetic materials in general. In one embodiment, the composition is industrially compostable and / or home compostable.

[0017] In one embodiment of the composition, the amorphous polyhydroxyalkanoate copolymer is a bio-based amorphous polyhydroxyalkanoate copolymer.

[0018] An amorphous polyhydroxyalkanoate copolymer is understood to be bio-based in the context of the invention if at least 51 wt.%, preferably more than 75 wt.%, more preferably more than 95 wt.%, based on the weight of the amorphous polyhydroxyalkanoate copolymer, was or is obtained from substances that are renewable substances or that were obtained from renewable substances. The bio-based portion can be determined using the radiocarbon method according to DIN EN 16640:2017-08. This method of determination takes advantage of the fact that small amounts of the radioactive carbon isotope are constantly present in the atmosphere. 14 C. This isotope enters the atmosphere as 14CO2 in plants and microorganisms and is then used in various biomasses. Due to the radioactive decay of 14 C can be determined by the proportion of 14C a conclusion can be drawn about how old the starting compounds used to produce the materials are and thus whether a material was produced from fresh biomass or from fossil carbon sources, such as petroleum. The term “biobased” is used in the context of the invention as defined in DIN EN 16640:2017-08. Biobased materials are therefore completely or partially derived from biomass. In the context of the invention, a biobased material is understood to mean, for example, plants, microorganisms or animals as well as their metabolites and parts, but also materials obtained therefrom by mechanical and / or chemical transformation. A biobased amorphous polyhydroxyalkanoate (aPHA) copolymer is therefore a polymer that contains at least 51 wt.%, preferably more than 75 wt.%, more preferably more than 95 wt.-%, (most preferably completely) based on the weight of the amorphous polyhydroxyalkanoate (aPHA) copolymer, is obtained or derived from renewable substances.

[0019] As is generally the case, bio-based materials in this text do not refer to petroleum or other fossil sources, even if these originated in geological times from the decomposition products of dead plants and animals.

[0020] In one embodiment of the composition, the at least one comonomer other than 3-hydroxybutanoic acid (3HB) is selected from the group consisting of 3-hydroxypropionic acid (3HP), 3-hydroxyvaleric acid (3HV), 4-

[0021] Hydroxybutanoic acid (4HB), 5-hydroxyvaleric acid (5HV), 3-hydroxyhexanoic acid (3HH), 3-hydroxyoctanoic acid (3HO), and combinations of these compounds are selected. Amorphous polyhydroxy alkanoates of 3-hydroxybutyric acid and one or more of these comonomers are widely available commercially and have proven particularly effective for increasing the amorphous portion of the composition. The selection of 4-hydroxybutanoic acid (4HB) as a comonomer is particularly advantageous because the resulting P(3HB-co-4HB) is a biodegradable and biocompatible thermoplastic that can be obtained by microbial fermentation from a wide range of renewable raw materials and exhibits a wide range of mechanical strengths and viscoelastic properties, depending on the proportion of 4-hydroxybutanoic acid (4HB) in the monomer composition.

[0022] In one embodiment of the composition, the mass fraction of amorphous polyhydroxyalkanoate copolymer, based on the total weight of the composition, is between 12 wt.% and 24 wt.%, preferably between 14 wt.% and 23 wt.%, more preferably between 16 wt.% and 22 wt.%, even more preferably between 18 wt.% and 22 wt.%, most preferably between 19 wt.% and 21 wt.%. In this range, a particularly advantageous balance was found between the biodegradability and the viscoelastic properties of the composition relevant for processability. A mass fraction of amorphous polyhydroxyalkanoate copolymer of approximately 20 wt.%, based on the total weight of the composition, has proven particularly advantageous in this regard.

[0023] In one embodiment of the composition, the mass fraction of 3-hydroxybutyric acid (3HB) is between 9 wt.% and 15 wt.%, preferably between 11 wt.% and 13 wt.%, particularly preferably about 12 wt.%, based on the total weight of the composition. In this range, the crystallinity is reduced compared to pure polyhydroxybutyrate (P3HB) to such an extent that the biodegradability of the composition is significantly increased.

[0024] In one embodiment of the composition, the mass fraction of comonomer other than 3-hydroxybutyrate (3HB) is between 4 wt.% and 10 wt.%, preferably between 6 wt.% and 8 wt.%, particularly preferably about 7 wt.%, based on the total weight of the composition. In this range, the crystallinity is reduced to such an extent compared to pure polyhydroxybutyrate (P3HB) that the biodegradability of the composition is significantly increased. At the same time, such compositions exhibit sufficient tear strength and toughness for thermoforming compared to corresponding compositions without amorphous polyhydroxyalkanoate.

[0025] In particular, the comonomer other than 3-hydroxybutanoic acid (3HB) can be 4-hydroxybutanoic acid (4HB), wherein the mass fraction of 4-hydroxybutanoic acid (4HB) is between 4 wt.% and 10 wt.%, preferably between 6 wt.% and 8 wt.%, particularly preferably about 7 wt.%, based on the total weight of the composition. In this range, the advantages mentioned above for P(3HB-co-4HB) are achieved, particularly with regard to the use of a composition according to one of the embodiments described herein for the production of portion capsules.

[0026] In one embodiment, the composition further comprises at least one filler selected from the group consisting of carbon black, cyanuric acid, uracil, thymine, mica, talc, silicon dioxide, boron nitride, barium nitride, nanoclay, calcium carbonate, synthesized silica and its salts, metal salts of organophosphates, kaolin, and combinations of these substances. The selection of talc as a filler is particularly advantageous because talc can increase the strength, stiffness, and hardness of the polymer blend and lead to better temperature resistance. The addition of talc can increase the dimensional stability of the polymer blend because it reduces shrinkage and deformation of the polymer blend upon cooling. Finally, talc can help improve the surface quality of the polymer blend by reducing the formation of surface defects such as bubbles or bumps.Talc also helps prevent the composition in polymer granulate form from clogging.

[0027] In embodiments, the mass fraction of fillers is between 1 wt.% and 10 wt.%, preferably about 5 wt.%, based on the total weight of the composition.

[0028] In one embodiment, the composition further comprises at least one agent for preventing degradation (corrosion) by autoxidation, alkyl radical scavengers, stabilizers, compatibilizers, processing aids, antistatic agents, dyes, optical brighteners, blowing agents, flame retardants, fillers, reinforcing agents, adhesion promoters, and biocides. Such agents, also called additives, are known to those skilled in the art.

[0029] In embodiments, the mass fraction of additives is between 0 wt% and 5 wt%, preferably between 0.1 wt% and 3.5 wt%, particularly preferably between 0.5 wt% and 2.5 wt%, based on the total weight of the composition.

[0030] In one embodiment, the composition exhibits at least a 25% faster biodegradation rate, determined according to ISO 14855-1, compared to a reference composition without amorphous polyhydroxyalkanoate copolymer. Alternatively or additionally, one embodiment of the composition exhibits at least a 90% faster biodegradation rate, determined according to ISO 15985, compared to a reference composition without amorphous polyhydroxyalkanoate copolymer.

[0031] For the purposes of the present invention, a "reference composition" is understood to mean a composition that is identical to a tested composition according to the claims, with the exception that it does not contain the amorphous polyhydroxyalkanoate copolymer. In particular, a "reference composition" is understood to mean a composition in which the amorphous polyhydroxyalkanoate copolymer is replaced by polyhydroxybutyrate (P3HB).

[0032] Unless otherwise stated, one or more of the aforementioned embodiments may be combined with each other as desired.

[0033] In one embodiment, the composition consists essentially of: i. 75 wt.% to 90 wt.% polybutylene succinate (PBS); ii. 10 wt.% to 25 wt.% amorphous polyhydroxyalkanoate (aPHA) copolymer of 3-hydroxybutanoic acid (3HB) and at least one comonomer selected from the group consisting of 3-hydroxypropionic acid (3HP), 3-hydroxyvaleric acid (3HV), 4-hydroxybutanoic acid (4HB), 5-hydroxyvaleric acid (5HV), 3-hydroxyhexanoic acid (3HH) and 3-hydroxyoctanoic acid (3HO), in particular poly(3-hydroxybutyrate-co-4-hydroxybutyrate); iii. Optionally, 1 wt.% to 10 wt.% of at least one filler, in particular talc; and iv. Optionally, up to 5 wt.% of at least one additive; in each case based on the total weight of the composition. The mass fraction of comonomer other than 3-hydroxybutanoic acid (3HB) is between 25 wt.% and 85 wt.%, based on the weight of the amorphous polyhydroxyalkanoate (aPHA) copolymer.

[0034] In the above embodiment, the mass fraction of component i., i.e. polybutylene succinate, is preferably between 76 wt.% and 88 wt.%, more preferably between 77 wt.% and 86 wt.%, even more preferably between 78 wt.% and 84 wt.%, most preferably between 79 wt.% and 81 wt.%, in each case based on the total weight of the composition. The mass fraction of component ii., i.e. amorphous polyhydroxyalkanoate (aPHA) copolymer, is preferably between 12 wt.% and 24 wt.%, more preferably between 14 wt.% and 23 wt.%, even more preferably between 16 wt.% and 22 wt.%, most preferably between 19 wt.% and 21 wt.%, in each case based on the total weight of the composition.

[0035] In the above embodiment, a portion capsule is obtained which essentially consists of a composition described herein, ie the weight proportions of components i. and ii., and optionally of the optional components iii. and iv., add up to 100 wt. %, based on the total weight of the composition or based on the weight of the portion capsule.

[0036] Within the scope of the invention, a portion capsule is understood to mean a package that can be inserted into a capsule receptacle of a beverage preparation machine and contains at least one beverage starting material that can be extracted using water, in particular coffee or tea. Parts of such a package are also understood within the scope of the invention as portion capsules, provided they are a self-contained unit. For example, a base element of a portion capsule is also understood to be a portion capsule, even if the combination of base element and capsule lid is usually used to package the beverage starting material.

[0037] In one embodiment, the portion capsule comprises a base element with a base region and a surrounding side wall, wherein the base region and the surrounding side wall form an interior space for storing a beverage starting material that can be extracted by means of water. The beverage starting material can be, in particular, coffee or tea. Thus, in one embodiment of the portion capsule, it is a coffee or tea capsule.

[0038] In one embodiment of the portion capsule, the base element comprises or consists of a composition according to one of the previously described embodiments. In particular, the base region and the circumferential side wall comprise or consist of the same composition according to one of the previously described embodiments. Such an embodiment has the previously described advantageous properties for the entire base element and is particularly easy to manufacture, for example, by deep-drawing or injection-molding.

[0039] In one embodiment, the wall thickness of the portion capsule is between 100 pm and 500 pm, preferably between 200 pm and 400 pm, in particular approximately 300 pm. In particular, the wall thickness of the peripheral side wall of a portion capsule with a base element is between 100 pm and 500 pm, preferably between 200 pm and 400 pm, in particular approximately 300 pm.

[0040] A further aspect of the invention relates to a method for producing a portion capsule according to one of the previously described embodiments. The method comprises the following steps: a) mixing and / or melting a composition according to one of the previously described embodiments to obtain a polymer blend; and b) reshaping the polymer blend obtained in step a) to obtain the portion capsule; c) optionally, filling the portion capsule obtained in step b) with a portion of a beverage starting material and closing the portion capsule filled with the beverage starting material with a capsule lid, in particular by welding a capsule lid comprising a composition according to one of the previously described embodiments to a base element of the portion capsule.

[0041] In one embodiment of the process, the mixing and / or melting of the composition in step a) takes place in an extruder. The use of extruders when mixing and / or melting the components of a composition according to one of the embodiments described herein enables particularly efficient, homogeneous, and controlled processing of the composition.

[0042] In one embodiment of the process, the polymer blend obtained in step a) is formed by deep drawing. Compared to other forming processes such as injection molding, deep drawing is often more cost-effective because it requires less tooling and machine setup. Nevertheless, deep drawing allows for the rapid production of large quantities of parts, making it ideal for mass production. Deep drawing allows for a wide variety of shapes to be realized with relatively little effort, increasing the design freedom of the portion capsules.

[0043] In one embodiment of the process, the polymer blend obtained in step a) is formed by injection molding. The injection molding process allows for particularly rapid production of large quantities of single-portion capsules with even greater design freedom compared to the deep-drawing process. Furthermore, the injection molding process allows for the production of single-portion capsules with precisely defined, particularly uniform, wall thicknesses.

[0044] In one embodiment of the process, the composition according to one of the previously described embodiments is provided as granules in step a). The granules used comprise the composition according to one of the previously described embodiments in a homogeneous and solid form. In other words, the granules already consist of the polymer blend to be obtained, and the granules essentially only need to be melted in step a).

[0045] In one embodiment of the method, the weight of the portion of a beverage starting material, in particular a coffee powder mixture, with which the portion capsule is filled in step c), is between 5 and 10 grams.

[0046] A further aspect of the invention relates to the use of a composition according to one of the previously described embodiments for packaging a beverage base material. The beverage base material to be packaged or packaged can be, in particular, coffee or tea.

[0047] The subject matter of the invention is explained in more detail below using exemplary embodiments illustrated in the accompanying figures. Each of these figures schematically shows:

[0048] Figure 1: a side view of an exemplary packaging;

[0049] Figure 2: a perspective view of a longitudinally halved base element of an exemplary portion container;

[0050] Figure 3: a cross section through a side wall of a base element in

[0051] Area X from Figure 2;

[0052] Figure 4: Degradation curves for comparison experiment 1 (thermophilic anaerobic);

[0053] Figure 5: Degradation curves for Comparative Experiment 2 (aerobic). The exemplary embodiments described below are merely examples of the subject matter of the invention and are not limiting. In principle, identical parts are provided with identical reference numerals in the figures.

[0054] Figure 1 shows an exemplary packaging in the form of a portion capsule 10. The portion capsule 10 has a base element 11 with a base element axis 15, a base region 16, and a circumferential side wall 12. The base element 11 shown here has the shape of a cup, with the base element axis 15 being a cup axis. The base region 16 and the circumferential side wall 12 form an interior space in which a beverage base material that can be extracted using water, such as a coffee powder mix or tea, can be stored. The portion capsule 10 further has a capsule lid 21, which is fastened along a circumferential flange 14 of the base element 11, with the base element 11 and the capsule lid 21 together forming an outer container wall and defining a hermetically sealed capsule interior.Base element 11 and capsule lid 21 together thus delimit a hermetically sealed volume for storing a substance, in particular a water-extractable beverage starting material for preparing a beverage by flowing water through the portion capsule. The flange 14 shown is realized as a collar of the circumferential side wall 12 and can accordingly also be referred to as a circumferential collar 14. In the embodiment shown, at least the base element 11, i.e. the base region 16 and the circumferential side wall 12, comprises one and the same embodiment of a composition as described above. However, it is also conceivable for the base element 11 and the capsule lid 21 to comprise one and the same embodiment of a composition as described above.

[0055] Figure 2 shows a perspective view of a longitudinally halved base element 11a of an exemplary portion capsule. In addition to a portion of the base region 16 and the flange 14, a portion of the side wall 12 is shown. A possible material structure of the base element 11a is described in more detail below in Figure 3 using a schematic cross-section through the side wall 12 in region X.

[0056] Figure 3 shows a cross section through a side wall of a base element in the area X from Figure 2, as an example for the structure of the entire base element 11, i.e. the circumferential collar 14, the side walls 12 and the bottom area 16. The side wall has a sandwich structure of two outer layers 1, each of which is formed from a composition consisting of 80 wt.% polybutylene succinate (PBS), 19 wt.% amorphous poly(3-hydroxybutyrate-co-4-hydroxybutyrate) with 30 wt.% 4-hydroxybutanoic acid (corresponding to 12 wt.% 3-hydroxybutanoic acid and 7 wt.% 4-hydroxybutanoic acid), and 1 wt.% talc, in each case based on the total weight of the composition of the outer layers 1.The intermediate layer 2, enclosed by the two outer layers 1, consists of a polyvinyl alcohol, which, due to its hydrophilic properties and hydrogen bonds between the polymer chains, provides a barrier against fats, oils, and oxygen. The intermediate layer 2 is therefore a barrier layer. The mass fraction of the two outer layers 1 is 49 wt.% each, and the mass fraction of the intermediate or barrier layer 2 is 2 wt.%, each based on the total weight of the base element 11.

[0057] Comparative tests

[0058] The following comparative tests were used to demonstrate the beneficial effect.

[0059] Materials

[0060] Samples consisting of different materials were tested under two different conditions according to Comparative Experiment 1 (thermophilic anaerobic) and Comparative Experiment 2 (aerobic). "A" refers to samples made of microcrystalline cellulose (20 pm, 42% TOC); "B" refers to samples made of a composition of 81 wt% polybutylene succinate (PBS) and 19 wt% poly(3-hydroxybutyrate-co-4-hydroxybutyrate) (P(3HB-co-4HB)) with a mass fraction of 4-hydroxybutyrate acid of 30 wt%, based on the weight of poly(3-hydroxybutyrate-co-4-hydroxybutyrate), corresponding to 12 wt% 3-hydroxybutyrate acid and 7 wt% 4-hydroxybutyrate acid, based on the total weight of composition "B"; "C" refers to samples made of polybutylene succinate (PBS). All materials required for sample preparation are commercially available.

[0061] Comparison experiment 1 (thermophilic anaerobic)

[0062] Biodegradation under thermophilic anaerobic conditions was determined according to the test method described in ISO 15985 (Plastics - Determination of ultimate anaerobic biodegradation and disintegration under high solids anaerobic digestion conditions - Method by analysis of evolved biogas (2014)). ISO 15985 is equivalent to ASTM D5511. The tests were conducted according to ISO 15985 under screening conditions. Specifically, two or three parallel experiments were conducted in 1000 mL incubation flasks at an incubation temperature of 52 °C and a substrate moisture content of 60%-95% over an incubation period of 32 days. The inoculum used had a dry matter content of 26.7%, a pH of 8.8, a volatile organic acid content of <1.0 g / kg, and an ammonia nitrogen (NH4-N) content of 1.8 g / kg, and an inoculum mass per incubation bottle of 500 g, with pre-incubation of the inoculum being 15 days. The sample mass per incubation bottle was 15.0 - 16.0 g / 1000 g, with an organic carbon content of 4.3 - 5.0 g.

[0063] The test unit consisted of a 400 mL eudiometer, graduated from top to bottom at 2 mL intervals. This eudiometer is connected to a 1000 mL incubation bottle with a ground joint. A connecting tube is inserted through the bottom of the eudiometer tube to allow the gas generated in the incubation bottle to enter the eudiometer tube and displace the barrier fluid through a tube into a 750 mL leveling bottle. An acidic solution with a high salt content was used as the barrier fluid for the volumetric biogas measurement.

[0064] As can be seen from the following table and the biodegradability curves shown in Figure 4, the biodegradability of the inventive sample "B," calculated from the carbon content of the biogas in the test according to ISO 15985, is on average approximately 100% higher after 32 days, i.e., approximately twice as high as the percentage biodegradability of the corresponding sample "C" without amorphous polyhydroxyalkanoate copolymer. For sample "A," the values ​​given in the table refer to the average obtained from three parallel tests. In the case of samples "B" and "C," the values ​​given in the table refer to the average obtained from two parallel tests.

[0065] Comparison experiment 2 (aerobic)

[0066] Biodegradation under aerobic conditions was determined according to ISO 14855-1 (Determination of ultimate aerobic biodegradability of plastic materials under controlled composting conditions - Method by analysis of released carbon dioxide - Part 1: General method (December 2012)). The theoretical amount of carbon dioxide (TI1CO2) of the reference sample "A", i.e., microcrystalline cellulose, is 132.2 g / 50 g wet weight. Two or three parallel experiments were conducted in 2000 mL incubation flasks at an incubation temperature of 58 °C over an incubation period of 100 days. The inoculum used had a dry solids content (ds) of 52.8%, a volatile solids content of 31.5%, and a pH of 8.2.Each incubation flask was filled with 600 g of a compost matrix consisting of compost and vermiculite as a mix component, with a compost-to-vermiculite ratio of 15:1 and a pH of 8.3. The dry mass ratio of the inoculum to the samples was 5.9:1. A respirometer (ECHO doo) was used as the apparatus. The air flow was 500 mL / min in the first week and 200 mL / min in the subsequent weeks. During the experiments, the activity of the inoculum was determined in three blank samples, "D1-D3," by measuring the carbon dioxide production in the respective blank samples after 10 days.

[0067] The carbon dioxide released from the blank samples "D" was 137 mg / g volatile solids after 10 days. The compost used as inoculum therefore showed sufficient biological activity.

[0068] As can be seen from the following table and the biodegradability curves shown in Figure 5, the biodegradation rate of samples "C" containing only polybutylene succinate (PBS) after 100 days was 76.5% and 89% of the maximum degradation rate of reference samples "A," respectively. Over the same period, the biodegradation rate of the inventive samples "B" containing polybutylene succinate (PBS) and amorphous polyhydroxyalkanoate copolymer (aPHA) was 95.9% and 112% of the maximum degradation rate of reference samples "A," respectively. In other words, after 100 days, samples "B" containing amorphous polyhydroxyalkanoate copolymer (aPHA) exhibited an average carbon dioxide production approximately 10% higher than samples "C" without amorphous polyhydroxyalkanoate copolymer (aPHA).

[0069] The biodegradation rate of reference sample "A" was >70% after 37 days. The difference between the percentage biodegradation of reference substance "A" in the three parallel experiments was 4% after 100 days. Finally, carbon dioxide production in blank sample "D" was 50-150 mg / g volatile solids after 10 days. Thus, the results meet the validity criteria of ISO standard 14855-1 (2012).

[0070] The present invention may further relate to the following embodiments:

[0071] I. Composition, in particular for the production of portion capsules, comprising i. polybutylene succinate (PBS), and ii. at least one amorphous polyhydroxyalkanoate (aPHA) copolymer of a) 3-hydroxybutanoic acid (3HB) and b) at least one comonomer other than 3-hydroxybutanoic acid (3HB), wherein the mass fraction of polybutylene succinate (PBS), based on the total weight of the composition, is between 75 wt.% and 90 wt.%, wherein the mass fraction of amorphous polyhydroxyalkanoate (aPHA) copolymer, based on the total weight of the composition, is between 10 wt.% and 25 wt.%, and wherein the mass fraction of the at least one comonomer other than 3-hydroxybutanoic acid (3HB), based on the weight of the amorphous

[0072] Polyhydroxyalkanoate (aPHA) copolymer, between 25 wt% and 85 wt%.

[0073] II. The composition according to embodiment I, wherein the at least one comonomer other than 3-hydroxybutanoic acid is selected from the group consisting of

[0074] Group consisting of 3-hydroxypropionic acid (3HP), 3-hydroxyvaleric acid (3HV), 4-hydroxybutanoic acid (4HB), 5-hydroxyvaleric acid (5HV), 3-hydroxyhexanoic acid (3HH), 3-hydroxyoctanoic acid (3HO) and combinations of these compounds, in particular 4-hydroxybutanoic acid (4HB).

[0075] III. The composition according to embodiment I or II, wherein the mass fraction of amorphous polyhydroxyalkanoate (aPHA) copolymer, based on the total weight of the composition, is between 18 wt.% and 22 wt.%, preferably about 20 wt.%.

[0076] IV. The composition according to any one of the preceding embodiments, wherein the mass fraction of 3-hydroxybutanoic acid (3HB), based on the total weight of the composition, is between 9 wt.% and 15 wt.%, preferably between 11 wt.% and 13 wt.%, particularly preferably about 12 wt.%.

[0077] V. The composition according to any one of the preceding embodiments, wherein the mass fraction of comonomer other than 3-hydroxybutanoic acid (3HB), in particular 4-hydroxybutanoic acid (4HB), based on the total weight of the composition, is between 4 wt.% and 10 wt.%, preferably between 6 wt.% and 8 wt.%, particularly preferably about 7 wt.%.

[0078] VI. The composition according to any one of the preceding embodiments,

[0079] 5 wherein the composition has at least a 25% faster biodegradation rate, determined according to ISO 14855-1, and / or at least a 90% faster biodegradation rate, determined according to ISO 15985, compared to a reference composition without amorphous polyhydroxyalkanoate (aPHA) copolymer. 0

[0080] VII. Portion capsule (10) consisting of or comprising a composition according to one of the preceding embodiments.

[0081] VIII. The portion capsule (10) according to embodiment VII, comprising a5 base element (11) with a bottom region (16) and a circumferential

[0082] Side wall (12), wherein the base region (16) and the surrounding side wall (12) form an interior space for storing a beverage starting material extractable by means of water, in particular coffee or tea, wherein the base region (16) and the surrounding side wall (12) preferably consist of the same composition according to one of the embodiments I to VI or comprise such a composition.

[0083] IX. The portion capsule (10) according to embodiment VIII, further comprising a capsule lid (21) which closes the interior formed by the base region (16) and the surrounding side wall (12) or is designed to close the interior formed by the base region (16) and the surrounding side wall (12), wherein the capsule lid (21) preferably consists of or comprises a composition according to one of embodiments I to VI. X. The portion capsule (10) according to embodiment VIII or IX, wherein the base element (11) and / or the capsule lid (21) has or have a layer (2) selected from the group consisting of a sealing layer, a barrier layer and a combination of these layers.

[0084] XI. A method for producing a portion capsule (10) according to one of embodiments VII to X, the method comprising the following steps: a) mixing and / or melting a composition according to one of embodiments I to VI, preferably in an extruder, for

[0085] Obtaining a polymer blend; b) forming, in particular deep drawing or injection molding, the polymer blend obtained in step a) to obtain the portion capsule (10); c) optionally, filling the portion capsule (10) obtained in step b) with a portion of a beverage starting material and closing the portion capsule filled with the beverage starting material with a capsule lid (21), in particular by welding a capsule lid (21) comprising a composition according to one of embodiments I to VI to a base element of the portion capsule (10).

[0086] XII. Use of a composition according to any one of embodiments I to VI for packaging a beverage starting material, in particular coffee or tea.

Claims

PATENT CLAIMS 1. Portion capsule (10) comprising a composition comprising i. polybutylene succinate (PBS), and ii. at least one amorphous polyhydroxyalkanoate (aPHA) copolymer of a) 3-hydroxybutanoic acid (3HB) and b) at least one comonomer other than 3-hydroxybutanoic acid (3HB), wherein the mass fraction of polybutylene succinate (PBS), based on the total weight of the composition, is between 75 wt.% and 90 wt.%, preferably between 76 wt.% and 88 wt.%, more preferably between 77 wt.% and 86 wt.%, even more preferably between 78 wt.% and 84 wt.%, most preferably between 79 wt.% and 81 wt.%, wherein the mass fraction of amorphous polyhydroxyalkanoate (aPHA) copolymer, based on the total weight of the composition, is between 10 wt.% and 25 wt.%, and wherein the mass fraction of the at least one comonomer other than 3-hydroxybutanoic acid (3HB), based on the weight of the amorphous polyhydroxyalkanoate (aPHA) Copolymers, between 25 wt.-% and 85 wt.-%.

2. The portion capsule (10) according to claim 1, wherein the at least one comonomer other than 3-hydroxybutanoic acid is selected from the group consisting of 3-hydroxypropionic acid (3HP), 3-hydroxyvaleric acid (3HV), 4-hydroxybutanoic acid (4HB), 5-hydroxyvaleric acid (5HV), 3-hydroxyhexanoic acid (3HH), 3-hydroxyoctanoic acid (3HO) and combinations of these compounds, in particular 4-hydroxybutanoic acid (4HB).

3. The portion capsule (10) according to claim 1 or 2, wherein the mass fraction of amorphous polyhydroxyalkanoate (aPHA) copolymer, based on the Total weight of the composition is between 12 wt% and 24 wt%, preferably between 14 wt% and 23 wt%, more preferably between 16 wt% and 22 wt%, even more preferably between 18 wt% and 22 wt%, most preferably between 19 wt% and 21 wt%, in particular about 20 wt%.

4. The portion capsule (10) according to any one of the preceding claims, wherein the mass fraction of 3-hydroxybutanoic acid (3HB), based on the total weight of the composition, is between 9 wt.% and 15 wt.%, preferably between 11 wt.% and 13 wt.%, particularly preferably about 12 wt.%.

5. The portion capsule (10) according to one of the preceding claims, wherein the mass fraction of comonomer other than 3-hydroxybutanoic acid (3HB), in particular 4-hydroxybutanoic acid (4HB), based on the total weight of the composition, is between 4 wt.% and 10 wt.%, preferably between 6 wt.% and 8 wt.%, particularly preferably about 7 wt.%.

6. The portion capsule (10) according to any one of the preceding claims, wherein the composition has at least a 25% faster biodegradation rate, determined according to ISO 14855-1, and / or at least a 90% faster biodegradation rate, determined according to ISO 15985, compared to a reference composition without amorphous polyhydroxyalkanoate (aPHA) copolymer.

7. The portion capsule (10) according to one of the preceding claims, comprising a base element (11) with a bottom region (16) and a circumferential side wall (12), wherein the bottom region (16) and the circumferential side wall (12) form an interior space for storing a Water-extractable beverage raw material, especially coffee or tea.

8. The portion capsule (10) according to claim 7, wherein the bottom region (16) and the circumferential side wall (12) consist of the same composition as defined in any one of claims 1 to 6 or comprise such a composition.

9. The portion capsule (10) according to claim 7 or 8, further comprising a capsule lid (21) which closes the interior formed by the base region (16) and the circumferential side wall (12) or is adapted to close the interior formed by the base region (16) and the circumferential side wall (12).

10. The portion capsule (10) according to claim 9, wherein the capsule lid (21) consists of or comprises a composition as defined in any one of claims 1 to 6.

11. The portion capsule (10) according to one of claims 7 to 10, wherein the base element (11) and / or the capsule lid (21) has or have a layer (2) selected from the group consisting of a sealing layer, a barrier layer and a combination of these layers.

12. A method for producing a portion capsule (10) according to any one of the preceding claims, the method comprising the following steps: a) mixing and / or melting a composition as defined in any one of claims 1 to 6, preferably in an extruder, to obtain a polymer blend; b) forming, in particular deep drawing or injection molding, the polymer blend obtained in step a) to obtain the portion capsule (10); c) Optionally, filling the portion capsule (10) obtained in step b) with a portion of a beverage starting material and closing the portion capsule filled with the beverage starting material with a capsule lid (21), in particular by welding a capsule lid (21) comprising a composition as defined in any one of claims 1 to 6 to a base element of the portion capsule (10).

13. Use of a composition as defined in any one of claims 1 to 6 for packaging a beverage base material, in particular Coffee or tea.

Images