Articles containing a melt-processable cellulose ester composition including an alkaline filler.

Abstract

The present application discloses a melt-processable cellulose ester composition comprising a cellulose ester, at least one alkaline additive, and at least one neutralizing agent. Optionally, a plasticizer can be used in the composition. The present application also discloses a method for preparing the composition, and an article that can be made from the composition. The composition shows improved decomposition properties.

Description

[Background technology]

[0001] There is a well-known global problem with waste management, particularly the disposal of large quantities of consumer products such as plastics or polymers that are not considered biodegradable within acceptable time limits. It is socially desirable to incorporate these types of waste into recycled products by recycling, reuse, or otherwise reducing the amount of waste in the circulation or landfill. This is especially true for single-use plastic items / materials.

[0002] Consumer sentiment regarding the environmental dynamics of single-use plastics such as straws, takeout cups, and plastic bags is a global trend, and bans on plastic products are being considered and enacted worldwide in both developed and developing countries. Bans in the US alone, for example, range from shopping bags to straws, knives, and clamshell packaging. Some countries are taking even stricter measures; for instance, across the EU, a list of 10 single-use items is banned, restricted, or requires extended producer responsibility. As a result, industry leaders, brand owners, and retailers are eagerly working to implement recyclable, reusable, or compostable packaging in the coming years. While recyclable materials are preferable in some applications, compostable and / or biodegradable materials are more suitable in others, such as when items are contaminated with food or when there is a high level of environmental leakage due to inadequate waste management systems.

[0003] In food service, single-use plastic items are frequently used, intended for one-time use to store or serve food, after which they are discarded. To prevent the persistence of these items, it is desirable that they disintegrate and biodegrade, even in thicker parts such as cup rims and cooking utensils. Disintegration in compost is the end of life that redirects these single-use plastic items away from landfills. Single-use plastic items can range in thickness from less than 5 mils (e.g., straws) to over 100 mils (e.g., cooking utensils). For some materials, the rate of disintegration in compost is proportional to the thickness of the item; that is, thicker items take longer to disintegrate or may not disintegrate within the standard timeframe of the composting cycle.

[0004] Even when articles have a thickness of 30 mils or more, it is desirable to manufacture them from bio-based materials formulated to disintegrate in compost. Furthermore, the appearance of the articles should be suitable for their intended use (not dark in color and not opaque).

[0005] Therefore, there is a market need for disposable consumer products that possess performance characteristics appropriate for their intended use and are compostable and / or biodegradable. It is beneficial to provide products that possess such characteristics and have a high content of renewable, recycled, and / or reused materials. [Overview of the Initiative] [Means for solving the problem]

[0006] This application relates to a melt-processable cellulose ester composition, The composition comprises at least one cellulose ester, at least one alkaline additive, and at least one neutralizing agent, wherein a 1% by weight suspension of the alkaline additive has a pH of 8 or higher, the water solubility of the alkaline filler at 20-25°C is greater than 1 ppm but less than 1,000 ppm, and the alkaline filler is present in an amount of about 0.1% to about 35% by weight based on the weight of the cellulose ester composition; or The present invention discloses a cellulose ester composition comprising at least one type of cellulose acetate, at least one type of plasticizer, at least one type of alkaline additive, and at least one type of neutralizing agent, wherein a 1% by weight suspension of the alkaline additive has a pH of 8 or higher, the water solubility of the alkaline filler at 20-25°C is greater than 1 ppm but less than 1,000 ppm, and the alkaline filler is present in an amount of about 0.1% to about 35% by weight based on the weight of the cellulose acetate composition.

[0007] This application discloses a method for producing a melt-workable cellulose ester composition. The method comprises the step of contacting at least one cellulose ester, optionally at least one plasticizer, at least one alkaline additive, and at least one neutralizing agent, wherein a 1 wt% suspension of the alkaline additive has a pH of 8 or higher, the water solubility of the alkaline filler at 20-25°C is greater than 1 ppm but less than 1,000 ppm, and the alkaline filler is present in an amount of about 0.1 wt% to about 35 wt% based on the weight of the cellulose ester composition.

[0008] This application discloses a method for producing a melt-processable cellulose acetate composition. The method comprises the step of contacting at least one cellulose acetate, at least one plasticizer, at least one alkaline additive, and at least one neutralizing agent, wherein the 1 wt% suspension of the alkaline additive has a pH of 8 or higher, the water solubility of the alkaline filler at 20-25°C is greater than 1 ppm but less than 1,000 ppm, and the alkaline filler is present in an amount of about 0.1 wt% to about 35 wt% based on the weight of the cellulose acetate composition.

[0009] This application discloses an article comprising a melt-processable cellulose ester composition, wherein the cellulose ester composition is The composition comprises at least one cellulose ester, at least one alkaline additive, and at least one neutralizing agent, wherein a 1% by weight suspension of the alkaline additive has a pH of 8 or higher, the water solubility of the alkaline filler at 20-25°C is greater than 1 ppm but less than 1,000 ppm, and the alkaline filler is present in an amount of about 0.1% to about 35% by weight based on the weight of the cellulose ester composition; or The composition comprises at least one type of cellulose acetate, at least one type of plasticizer, at least one type of alkaline additive, and at least one type of neutralizing agent. A 1% by weight suspension of the alkaline additive has a pH of 8 or higher, and the water solubility of the alkaline filler at 20-25°C is greater than 1 ppm but less than 1,000 ppm. The alkaline filler is present in an amount of approximately 0.1% to approximately 35% by weight based on the weight of the cellulose acetate composition.

[0010] This application discloses a cellulose acetate tow band comprising a cellulose acetate composition; at least one cellulose acetate, at least one plasticizer, at least one alkaline additive, and at least one neutralizing agent, wherein a 1% by weight suspension of the alkaline additive has a pH of 8 or higher, the water solubility of the alkaline filler at 20-25°C is greater than 1 ppm but less than 1,000 ppm, and the alkaline filler is present in an amount of about 0.1% to about 35% by weight based on the weight of the cellulose acetate composition. [Modes for carrying out the invention]

[0011] This application relates to a melt-processable cellulose ester composition, The composition comprises at least one cellulose ester, at least one alkaline additive, and at least one neutralizing agent, wherein a 1% by weight suspension of the alkaline additive has a pH of 8 or higher, the water solubility of the alkaline filler at 20-25°C is greater than 1 ppm but less than 1,000 ppm, and the alkaline filler is present in an amount of about 0.1% to about 35% by weight based on the weight of the cellulose ester composition, or The present invention provides a cellulose ester composition comprising at least one type of cellulose acetate, at least one type of plasticizer, at least one type of alkaline additive, and at least one type of neutralizing agent, wherein a 1% by weight suspension of the alkaline additive has a pH of 8 or higher, the water solubility of the alkaline filler at 20-25°C is greater than 1 ppm but less than 1,000 ppm, and the alkaline filler is present in an amount of about 0.1% to about 35% by weight based on the weight of the cellulose acetate composition.

[0012] Cellulose ester The cellulose ester used in the present invention may be any known in the art. The cellulose ester that can be used in the present invention generally contains repeating units of the following structure.

[0013] [ka]

[0014] In the formula, R 1 , R 2 , and R 3It is independently selected from the group consisting of hydrogen, acetyl, propyl or butyl. The substitution level of the cellulose ester is usually expressed in terms of the degree of substitution (DS), which is the average number of non-OH substituents per anhydroglucose unit (AGU). Generally, conventional cellulose contains three hydroxyl groups that can be substituted in each AGU unit, and thus the DS can have a value between zero and three. Natural cellulose is a large polysaccharide with a degree of polymerization of 250 to 5,000 even after pulping and purification, and thus the assumption that the maximum DS is 3.0 is approximately correct. Since the DS is a statistical average value, a value of 1 does not guarantee that any AGU has a single substitution. In some cases, there may be unsubstituted anhydroglucose units, some have two, and some have three substituents, and typically the value is non-integer. The total DS is defined as the average total number of substituents per anhydroglucose unit. The degree of substitution per AGU can also refer to a specific substituent, such as hydroxyl or acetyl, etc. In embodiments, n is an integer within the range of 25 to 250, or 25 to 200, or 25 to 150, or 25 to 100, or 25 to 75.

[0015] In embodiments of the present invention, the cellulose ester has at least two anhydroglucose rings and can have at least 50 to a maximum of 5,000 anhydroglucose rings, or at least 50 to less than 150 anhydroglucose rings. The number of anhydroglucose units per molecule is defined as the degree of polymerization (DP) of the cellulose ester. In embodiments, the cellulose ester can have an intrinsic viscosity (IV) of about 0.2 to about 3.0, or about 0.5 to about 1.8, or about 1 to about 1.5 deciliters / gram when measured at a temperature of 25 °C for a 0.25 gram sample in a 100 ml 60 / 40 weight ratio phenol / tetrachloroethane solution. In embodiments, the cellulose ester useful herein can have a DS / AGU of about 1 to about 2.5, or less than 1 to 2.2, or less than 1 to 1.5, and the substituted ester is acetyl.

[0016] Cellulose esters can be produced by any method known in the art. Examples of processes for producing cellulose esters are taught in Kirk-Othmer, Encyclopedia of Chemical Technology, 5th Edition, Volume 5, Wiley-Interscience, New York (2004), pages 394-444. Cellulose, the starting material for producing cellulose esters, can be obtained in different grades and from different sources, such as cotton linters, softwood pulp, hardwood pulp, corn fibers and other agricultural sources, and especially bacterial cellulose.

[0017] One way to produce cellulose esters is the esterification of cellulose by mixing cellulose with a suitable organic acid, acid anhydride, and catalyst. The cellulose is then converted to cellulose triester. Ester hydrolysis is then carried out by adding a water-acid mixture to the cellulose triester, which can then be filtered to remove any gel particles or fibers. Water is then added to the mixture and the cellulose ester precipitates. The cellulose ester can then be washed with water to remove reaction by-products, followed by dehydration and drying.

[0018] The cellulose triester to be hydrolyzed can have three acetyl substituents. These cellulose esters can be prepared by several methods known to those skilled in the art. For example, cellulose esters can be prepared by the heterogeneous acylation of cellulose in a mixture of carboxylic acids and anhydrides in the presence of a catalyst such as H2SO4. Cellulose triester can also be prepared by the homogeneous acylation of cellulose dissolved in a suitable solvent such as LiCl / DMAc or LiCl / NMP.

[0019] Those skilled in the art will understand that the commercial term cellulose triesters also includes cellulose esters that are not fully substituted with acyl groups. For example, cellulose triacetate, commercially available from Eastman Chemical Company, Kingsport, TN, USA, typically has a DS of about 2.85 to about 2.99.

[0020] Following the esterification of cellulose to triester, some of the acyl substituents may be removed by hydrolysis or alcohol decomposition to produce secondary cellulose esters. As previously mentioned, depending on the specific method used, the distribution of acyl substituents may be random or non-random. Secondary cellulose esters can also be prepared directly without hydrolysis by using a limited amount of acylation reagent. This process is particularly useful when the reaction is carried out in a solvent that dissolves cellulose. All of these methods result in cellulose esters useful in the present invention.

[0021] In one embodiment, or in combination with any of the embodiments mentioned, or in combination with any of the embodiments mentioned, the cellulose acetate is dicellulose acetate having a polystyrene-equivalent number-average molecular weight (Mn) of about 10,000 to about 100,000, as measured by gel permeation chromatography (GPC) using NMP as a solvent and polystyrene-equivalent number-average molecular weight (Mn) according to ASTM D6474. In embodiments, the cellulose acetate composition uses NMP as a solvent and ASTM Measured by gel permeation chromatography (GPC) according to D6474, 10,000-90,000; or 10,000-80,000; or 10,000-70,000; or 10,000-60,000; or less than 10,000-60,000; or less than 10,000-55,000; or 10,000-50,000; or less than 10,000-50,000; or less than 10,000-45,000; or 10,000-40,000; or 10,000-30,000; or less than 20,000-60,000; or less than 20,000-55,000; It contains cellulose diacetate having a polystyrene-equivalent number-average molecular weight (Mn) of 20,000 to 50,000; or less than 20,000 to 50,000; or less than 20,000 to 45,000; or 20,000 to 40,000; or 20,000 to 35,000; or 20,000 to 30,000; or less than 30,000 to 60,000; or less than 30,000 to 55,000; or less than 30,000 to 50,000; or less than 30,000 to 45,000; or 30,000 to 40,000; or 30,000 to 35,000.

[0022] The most common commercial secondary cellulose esters are prepared by forming cellulose triesters by the initial acid-catalyzed heterogeneous acylation of cellulose. After obtaining a homogeneous solution of the cellulose triester in the corresponding carboxylic acid, the cellulose triester is then subjected to hydrolysis until the desired degree of substitution is obtained. After isolation, random secondary cellulose esters are obtained, i.e., the relative degree of substitution (RDS) at each hydroxyl is approximately equal.

[0023] Cellulose esters useful in the present invention can be prepared using techniques known in the art and can be selected from various types of cellulose esters, such as those available from Eastman Chemical Company, Kingsport, TN, USA, for example, Eastman® Cellulose Acetate CA 398-30 and Eastman® Cellulose Acetate CA 398-10, Eastman® CAP 485-20 (acetic acid / propionic acid) cellulose, Eastman® CAB 381-2 (acetic acid / butyric acid) cellulose, etc.

[0024] In embodiments of the present invention, cellulose esters can be prepared by converting cellulose to cellulose esters using a reactant obtained from recycled materials, such as recycled plastic contents syngas sources. In embodiments, such a reactant may be a cellulose reactant comprising organic acids and / or acid anhydrides used in cellulose esterification or acylation reactions, as discussed herein.

[0025] In one embodiment of the present invention, or in combination with any of the embodiments mentioned, or in combination with any of the embodiments mentioned, a cellulose ester composition is provided comprising at least one recycled cellulose ester, wherein the cellulose ester has at least one substituent on an anhydroglucose unit (AU) derived from recycled contents material, such as recycled plastic contents syngas.

[0026] plasticizer In one embodiment, or in combination with any other embodiment, a melt-processable biodegradable cellulose ester composition may contain at least one plasticizer. The plasticizer reduces the melt temperature, Tg, and / or melt viscosity of the cellulose ester. Plasticizers for cellulose esters include glycerol triacetate (triacetin), glycerol diacetate, dibutyl terephthalate, dimethyl phthalate, diethyl phthalate, poly(ethylene glycol) MW200-600, triethylene glycol dipropionate, 1,2-epoxypropylphenylethylene glycol, 1,2-epoxypropyl(m-cresyl)ethylene glycol, 1,2-epoxypropyl(o-cresyl)ethylene glycol, β-oxyethylcyclohexene carboxylate, bis(cyclohexanate)diethylene glycol, triethyl citrate, polyethylene glycol, Benzoflex, propylene glycol, polysorbate, sucrose octaacetate, acetylated triethyl citrate, acetyl tributyl citrate, Admex, trippropionine, Scandiflex, and poloxamer copolymer. This may include polyethylene glycol succinate, diisobutyl adipate, polyvinylpyrrolidone and glycol tribenzoate, triethyl citrate, acetyl triethyl citrate, polyethylene glycol, benzoate-containing plasticizers, e.g., the Benzoflex® plasticizer series, poly(alkyl succinate), e.g., poly(butyl succinate), polyethersulfone, adipate-based plasticizer, soybean oil epoxide, e.g., the Paraplex® plasticizer series, sucrose-based plasticizer, dibutyl sebacate, tributylin, tripionine, sucrose acetate isobutyrate, plasticizers in the Resolflex® series, triphenyl phosphate, glycolate, methoxypolyethylene glycol, 2,2,4-trimethylpentane-1,3-diyrbis(2-methylpropanoate), and polycaprolactone.

[0027] In one embodiment or in combination with any other embodiment, the plasticizer is a food-compatible plasticizer. Food compatibility means that the plasticizer is in compliance with applicable food additive and / or food contact regulations, and is authorized for use or deemed safe by at least one (national or regional) food safety regulatory body (or organization), for example, listed in the 21 CFR Food Additives Regulations, or otherwise generally recognized as safe (GRAS) by the US FDA. In one embodiment or in combination with any other embodiment, the food-compatible plasticizer is triacetin or polyethylene glycol (PEG) having a molecular weight of about 200 to about 600. Examples of food-compatible plasticizers that may be considered in embodiments include triacetin, triethyl citrate, polyethylene glycol, Benzoflex, propylene glycol, polysorbate, sucrose octaacetate, acetylated triethyl citrate, acetyl tributyl citrate, Admex, trippropionine, Scandiflex, poloxamer copolymer, polyethylene glycol succinate, diisobutyl adipate, polyvinylpyrrolidone, and glycol tribenzoate.

[0028] In one embodiment, or in combination with any other embodiment, the plasticizer may be present in an amount sufficient to allow the cellulose ester composition to be melt-processed (or thermoformed) into articles useful in conventional melt-processing equipment, for example, into disposable plastic articles. In one embodiment, or in combination with any other embodiment, the plasticizer may be present in an amount of 1 to 40 wt%; or 5 to 25 wt%, or 10 to 25 wt%, or 12 to 20 wt%, based on the weight of the cellulose ester composition, for most thermoplastic resin processing. In embodiments, morph extrusion, sheet extrusion, thermoforming, and injection molding may be achieved with plasticizer levels in the range of 10 to 30 wt%, or 12 to 25 wt%, or 15 to 20 wt%, or 10 to 25 wt%, based on the weight of the cellulose ester composition.

[0029] In one embodiment or in combination with any other embodiment, the plasticizer is a biodegradable plasticizer. Some examples of biodegradable plasticizers include triacetin, triethyl citrate, acetyl triethyl citrate, polyethylene glycol, benzoate-containing plasticizers, e.g., the Benzoflex® plasticizer series, poly(alkyl succinates), e.g., poly(butyl succinates), polyethersulfone, adipate-based plasticizers, soybean oil epoxides, e.g., the Paraplex® plasticizer series, sucrose-based plasticizers, dibutyl sebacate, tributylin, plasticizers in the Resoflex® series, triphenyl phosphate, glycolate, polyethylene glycol, 2,2,4-trimethylpentane-1,3-diirbis(2-methylpropanoate), and polycaprolactone.

[0030] PEG / MPEG specific compositions In one embodiment, or in combination with any other embodiment, the cellulose ester composition may contain a plasticizer selected from the group consisting of PEG and MPEG (methoxyPEG). The composition is a polyethylene glycol or methoxy polyethylene glycol composition having an average molecular weight of 200 to 600 daltons, and the composition is melt-processable, biodegradable, and disintegrable.

[0031] In one embodiment, or in combination with any other embodiment, the composition comprises polyethylene glycol or methoxyPEG having an average molecular weight of 300 to 550 daltons.

[0032] In one embodiment, or in combination with any other embodiment, the composition comprises polyethylene glycol having an average molecular weight of 300 to 500 daltons. In one embodiment, or in combination with any other embodiment, the cellulose ester composition is, based on the total weight of the cellulose ester composition, 1 wt% to 40 wt%, or 5 wt% to 40 wt%, or 10 wt% to 40 wt%, or 12 wt% to 40 wt%, 13 wt% to 40 wt%, or 15 wt% to 40 wt%, or more than 15 wt% to 40 wt%, or 17 wt% to 40 wt%, or 20 wt% %~40wt%, or 25wt%~40wt%, or 5wt%~35wt%, or 10wt%~35wt%, or 13wt%~35wt%, or 15wt%~35wt%, or over 15wt%~35wt%, or 17wt%~35wt%, or 20wt%~35wt%, or 5wt%~30wt%, or 10wt%~30wt%, or 13wt%~30wt%, or 15wt%~30wt%, and This refers to a range of values ​​including over 15 wt% to 30 wt%, or 17 wt% to 30 wt%, or 5 wt% to 25 wt%, or 10 wt% to 25 wt%, or 13 wt% to 25 wt%, or 15 wt% to 25 wt%, or over 15 wt% to 25 wt%, or 17 wt% to 25 wt%, or 5 wt% to 20 wt%, or 10 wt% to 20 wt%, or 13 wt% to 20 wt%, or 15 wt% to 20 wt%, or over 15 wt% to 2 The material contains at least one plasticizer (as specified herein) in an amount of 0 wt%, or 17 wt% to 20 wt%, or 5 wt% to 17 wt%, or 10 wt% to 17 wt%, or 13 wt% to 17 wt%, or 15 wt% to 17 wt%, or more than 15 wt% to 17 wt%, or 5 wt% to less than 17 wt%, or 10 wt% to less than 17 wt%, or 13 wt% to less than 17 wt%, or 15 wt% to less than 17 wt%.

[0033] In one embodiment or in combination with any other embodiment, at least one plasticizer comprises or is a food-compatible plasticizer. In one embodiment or in combination with any other embodiment, the food-compatible plasticizer comprises or is triacetin or PEG MW300-500.

[0034] In one embodiment, or in combination with any other embodiment, the cellulose ester composition comprises a biodegradable cellulose ester (BCE) component comprising at least one BCE, and a biodegradable polymer component comprising at least one other biodegradable polymer (other than BCE). In one embodiment, or in combination with any other embodiment, the other biodegradable polymer may be selected from polyhydroxyalkanoates (PHA and PHB), polylactic acid (PLA), polycaprolactone polymer (PCL), polybutylene adipate terephthalate (PBAT), polyethylene succinate (PES), polyvinyl acetate (PVA), polybutylene succinate (PBS) and copolymers (e.g., polybutylene succinate-co-adipate (PBSA)), cellulose esters, cellulose ethers, starch, proteins, their derivatives, and combinations thereof. In one embodiment, or in combination with any other embodiment, the cellulose ester composition comprises two or more biodegradable polymers. In one embodiment, or in combination with any other embodiment, the cellulose ester composition contains a biodegradable polymer (other than BCE) in an amount of 0.1 wt% to less than 50 wt%, or 1 wt% to 40 wt%, or 1 wt% to 30 wt%, or 1 wt% to 25 wt%, or 1 wt% to 20 wt%, based on the cellulose ester composition. In one embodiment, or in combination with any other embodiment, the cellulose ester composition contains a biodegradable polymer (other than BCE) in an amount of 0.1 wt% to less than 50 wt%, or 1 wt% to 40 wt%, or 1 wt% to 30 wt%, or 1 wt% to 25 wt%, or 1 wt% to 20 wt%, based on the total amount of BCE and biodegradable polymer.In one embodiment, or in combination with any other embodiment, at least one biodegradable polymer is measured using gel permeation chromatography (GPC) with methylene chloride as a solvent, a refractive index detector and a polystyrene standard, with values ​​ranging from 10,000 to 1,000,000, or 50,000 to 1,000,000, or 100,000 to 1,000,000, or 250,000 to 1 The PHA comprises a weight-average molecular weight (Mw) of 1,000,000, or 500,000 to 1,000,000, or 600,000 to 1,000,000, or 600,000 to 900,000, or 700,000 to 800,000, or 10,000 to 500,000, or 10,000 to 250,000, or 10,000 to 100,000, or 10,000 to 50,000. In one embodiment, or in combination with any other embodiment, the PHA may comprise polyhydroxybutyrate-co-hydroxyhexanoate.

[0035] Alkaline filler A suitable alkaline filler for the present invention is at least one selected from the group consisting of metal oxides, metal hydroxides, metal carbonates, and mixtures thereof. A blend of alkaline fillers may be used in a cellulose ester composition. In one embodiment, or in combination with any other embodiment, the alkaline filler is at least one selected from the group consisting of alkaline earth metal oxides, alkaline earth metal hydroxides, and alkaline earth carbonates.

[0036] Alkaline fillers have specific physical properties. For this application to be suitable, the water solubility of alkaline fillers at 20-25°C is useful only within a certain range. If the water solubility is too high, moisture in the molten article may prematurely initiate the chemical reaction of disintegration. If the water solubility is too low, basic ions (OH) may cause disintegration. -1 or CO3 -2) cannot be released from the filler. Furthermore, the pH of a 1 wt% solution or suspension of the alkaline filler should be pH 8 or higher, which is related to water solubility. If the pH is not 8 or higher, the conditions are not suitable for promoting the chemical reaction of decay. In one embodiment, or in combination with any other embodiment, the pH of a 1 wt% solution or suspension of the alkaline filler is pH 8.5 or higher. In one embodiment, or in combination with any other embodiment, the pH of a 1 wt% solution or suspension of the alkaline filler may be in the range of about 8 to about 12, about 8 to about 11.5, about 8 to about 11, about 8 to about 10.5, about 8 to about 10, 8.5 to about 12, about 8.5 to about 11.5, about 8.5 to about 11, about 8.5 to about 10.5, about 8.5 to about 10, about 9 to about 12, about 9 to about 11.5, about 9 to about 11, and about 9 to about 10.5. Not all metal oxides, hydroxides, and carbonates are suitable for use in this invention. For example, aluminum oxide (Al2O3) and titanium dioxide (TiO2) are insoluble in water, do not react with water to form corresponding hydroxides, and do not change the pH of water.

[0037] "Alkaline efficiency" is defined as the number of moles of base divided by the number of kilograms of alkaline filler. The alkaline efficiency of an alkaline filler also determines its ability to promote decay through chemical reactions. Alkaline efficiency is the number of moles of basic ions relative to a particular mass of filler in the presence of water. For example, CaO and MgO react with water to form 2 moles of hydroxide ions (OH). -1 ) is formed. Alkaline fillers with higher alkaline efficiency can accelerate the chemical reactions underlying the disintegration at lower filler addition amounts based on wt% in the formulation. A stoichiometric amount of alkaline catalyst is required for the base-catalyzed hydrolysis of esters because the final acid formed neutralizes and inactivates the base catalyst.

[0038] For the purposes of this application, the water solubility of the alkaline filler at 20-25°C should be greater than 1 ppm but less than 1,000 ppm. In other embodiments of the present invention, the water solubility of the alkaline filler at 20-25°C should be about 2 ppm to about 1,000 ppm, about 2 ppm to about 950 ppm, about 2 ppm to about 900 ppm, about 2 ppm to about 850 ppm, about 2 ppm to about 800 ppm, about 2 ppm to about 750 ppm, about 2 ppm to about 700 ppm, about 2 ppm to about 650 ppm, about 2 ppm to about 600 ppm, about 2 ppm to about 550 ppm, about 2 ppm to about 500 ppm, about 2 ppm to about 450 ppm, and about 2 ppm to about 400 ppm. m, about 2ppm to about 350ppm, about 2ppm to about 300ppm, 3ppm to about 1,000ppm, about 3ppm to about 950ppm, about 3ppm to about 900ppm, about 3ppm to about 850ppm, about 3ppm to about 800ppm, about 3ppm to about 750 ppm, about 3ppm to about 700ppm, about 3ppm to about 650ppm, about 3ppm to about 600ppm, about 3ppm to about 550ppm, about 3ppm to about 500ppm, about 3ppm to about 450ppm, about 3ppm to about 400ppm, about 3ppm to about 350 ppm, approximately 3ppm to approximately 300ppm, 4ppm to approximately 1,000ppm, approximately 4ppm to approximately 950ppm, approximately 4ppm to approximately 900ppm, approximately 4ppm to approximately 850ppm, approximately 4ppm to approximately 800ppm, approximately 4ppm to approximately 750ppm, approximately 4ppm to approximately 7 00ppm, about 4ppm to about 650ppm, about 4ppm to about 600ppm, about 4ppm to about 550ppm, about 4ppm to about 500ppm, about 4ppm to about 450ppm, about 4ppm to about 400ppm, about 4ppm to about 350ppm, about 4ppm to about 3 The concentrations are 00 ppm, 5 ppm to approximately 1,000 ppm, approximately 5 ppm to approximately 950 ppm, approximately 5 ppm to approximately 900 ppm, approximately 5 ppm to approximately 850 ppm, approximately 5 ppm to approximately 800 ppm, approximately 5 ppm to approximately 750 ppm, approximately 5 ppm to approximately 700 ppm, approximately 5 ppm to approximately 650 ppm, approximately 5 ppm to approximately 600 ppm, approximately 5 ppm to approximately 550 ppm, approximately 5 ppm to approximately 500 ppm, approximately 5 ppm to approximately 450 ppm, approximately 5 ppm to approximately 400 ppm, approximately 5 ppm to approximately 350 ppm, and approximately 5 ppm to approximately 300 ppm.

[0039] In one embodiment, or in combination with any other embodiment, the pH of a 1 wt% suspension of the alkaline filler should be 8 or higher, and the alkaline efficiency should be at least 5. In one embodiment, or in combination with any other embodiment, the alkaline efficiency is at least 6, at least 7, at least 8, at least 9, or at least 10. The following table shows the comparative properties of selected alkaline fillers, only some of which satisfy all the criteria of the present invention. Examples of alkaline fillers that satisfy the criteria include calcium carbonate (CaCO3), magnesium oxide (MgO), magnesium hydroxide (Mg(OH)2), magnesium carbonate (MgCO3), and barium carbonate (BaCO3). Effective and readily available alkaline fillers are calcium carbonate (CaCO3), magnesium oxide (MgO), magnesium hydroxide (Mg(OH)2), and magnesium carbonate (MgCO3). Furthermore, these alkaline fillers are particularly suitable for food contact applications.

[0040] In one embodiment, or in combination with any other embodiment, the alkaline filler is a mixture of calcium carbonate and at least one of magnesium oxide, magnesium hydroxide, or magnesium carbonate, where, based on the total weight of the cellulose ester composition, calcium carbonate is present in an amount of 5 to 25% by weight, and at least one of magnesium oxide, magnesium hydroxide, or magnesium carbonate is present in an amount of 1 to 20% by weight. In one embodiment, or in combination with any other embodiment, the alkaline filler is a mixture of calcium carbonate and at least one of magnesium oxide, magnesium hydroxide, or magnesium carbonate, where calcium carbonate is present in an amount of 5 to 15% by weight, based on the total weight of the cellulose ester composition, and at least one of magnesium oxide, magnesium hydroxide, or magnesium carbonate is present in an amount of 1 to 20% by weight. In one embodiment, or in combination with any other embodiment, the alkaline filler is a mixture of calcium carbonate and at least one of magnesium oxide, magnesium hydroxide, or magnesium carbonate, where, based on the total weight of the cellulose ester composition, calcium carbonate is present in an amount of 5 to 10% by weight, and at least one of magnesium oxide, magnesium hydroxide, or magnesium carbonate is present in an amount of 1 to 20% by weight.

[0041] Alkaline packing materials may be hydrated. Blends of alkaline packing materials are also an option for creating alkaline conditions to promote disintegration. Alkaline packing materials, hydrates, or blends may be natural or synthetic blends, compounds, or minerals. For example, magnesium carbonate may be mined as a magnesite mineral or prepared in the laboratory by reacting a soluble magnesium salt with sodium bicarbonate. Examples of mineral hydrates and blends include basic magnesium carbonate (BMC, typically hydrated with 3-5 water molecules), artiniite (4MgCO3·Mg(OH)2·3H2O), hydromagnesite (Mg5(CO3)4(OH)2·4H2O), dipingite (4MgCO3·Mg(OH)2·5H2O), and dolomite (CaCO3·MgCO3). When a soluble magnesium salt (e.g., magnesium chloride or magnesium sulfate) is treated with sodium carbonate or sodium bicarbonate, the resulting precipitate may, depending on the reaction temperature and CO2 partial pressure, contain hydrated complexes of magnesium carbonate and / or magnesium hydroxide, e.g., [MgCO3·3H2O] or [4MgCO3·Mg(OH)2·4H2O]. Blends can also be prepared by combining the anhydrous or hydrated forms of MgO, Mg(OH)2, and / or MgCO3 with each other or with other minerals within the same water solubility range (e.g., CaCO3 or BaCO3).

[0042] [Table 1]

[0043] While not essential, it is beneficial for alkaline fillers to have the ability to cause volume expansion. For example, hydration of MgO to magnesium hydroxide (Mg(OH)2) results in an increase in volume. During hydration, the weight of 1 mole of MgO increases from 40.3 g to 58.3 g (i.e., a 44.7% increase), and the filler volume can increase 2.2 times after complete hydration. Localized volume expansion can create tensile stress in the molten workpiece, leading to the formation of cracks and fissures that contribute to collapse. Similarly, MgCO3 can be hydrated, which alters the filler density and significantly increases its molar volume. MgCO3 also reacts with acidic aqueous solutions to release CO2 and water, simultaneously causing volume expansion within the thermoformed workpiece, which leads to tensile stress, physical deformation, and / or fracture.

[0044] [Table 2]

[0045] For the present invention to be useful, the amount of alkaline filler in the formulation is limited to a specific range. The amount should be high enough to accelerate the disintegration chemical reaction without causing premature decomposition of the formulation. If the alkaline filler is present in amounts greater than 35 wt%, the alkalinity or free alkali, combined with the heat of processing, may cause premature decomposition of the formulation. If the alkaline filler is present in excessively low amounts, it may be ineffective in accelerating the disintegration chemical reaction. In one embodiment, or in combination with any other embodiment, the alkaline filler is present in the cellulose ester composition in an amount of about 0.1 wt% to about 30 wt%, or about 0.1 wt% to about 25 wt%, or about 0.1 wt% to about 20 wt%, or about 0.1 wt% to about 15 wt%, or about 1 wt% to about 35 wt%, or about 1 wt% to about 30 wt%, or about 1 wt% to about 25 wt%, or about 1 wt% to about 20 wt%. wt%, or approximately 1 wt% to approximately 15 wt%, or approximately 1 wt% to approximately 10 wt%, or approximately 1 wt% to approximately 5 wt%, or approximately 5 wt% to approximately 35 wt%, or approximately 5 wt% to approximately 30 wt%, or approximately 5 wt% to approximately 25 wt%, or approximately 5 wt% to approximately 20 wt%, or approximately 5 wt% to approximately 15 wt%, or approximately 5 wt% to approximately 10 wt%, or approximately 10 wt% to approximately 35 wt%, or approximately 10 wt% to approximately 30 wt%, or Approximately 10 wt% to approximately 25 wt%, or approximately 10 wt% to approximately 20 wt%, or approximately 10 wt% to approximately 15 wt%, or approximately 15 wt% to approximately 35 wt%, or approximately 15 wt% to approximately 30 wt%, or approximately 15 wt% to approximately 25 wt%, or approximately 15 wt% to approximately 20 wt%, or approximately 15 wt% to approximately 20 wt%, or approximately 20 wt% to approximately 35 wt%, or approximately 20 wt% to approximately 30 wt%, or approximately 20 wt% to approximately 25 wt%, Alternatively, it may be present in amounts of approximately 25 wt% to 35 wt%, or approximately 25 wt% to 30 wt%, or approximately 0.1 wt% to 10 wt%, and in the cellulose ester composition, it may be present in amounts of approximately 0.5 wt% to 10 wt%, or approximately 1 wt% to 10 wt%, or approximately 1.5 wt% and 10 wt%, or approximately 2 wt% and 10 wt%, or approximately 2.5 wt% and 10 wt%, or approximately 3 wt% and 10 wt%, or approximately 3.It is present in amounts of 5 wt% and about 10 wt%, or about 4 wt% to about 10 wt%, or about 4.5 wt% to about 10 wt%, or about 5 wt% to about 10 wt%, or 0.1 wt% and about 9.5 wt%, and in the cellulose ester composition, it is present in amounts of about 0.5 wt% to about 9.5 wt%, or about 1 wt% to about 9.5 wt%, or about 1.5 wt% and about 9.5 wt%, or about 2 wt% and about 9.5 wt%, or about 2.5 wt% and about 9.5 wt%, or about 3 wt% and about 9.5 wt%, or about 3.5 wt% and about 9. It is present in amounts of 5 wt%, or about 4 wt% and about 9.5 wt%, or about 4.5 wt% and about 9.5 wt%, or about 5 wt% and about 9.5 wt%, or 0.1 wt% and about 9 wt%, or in amounts of about 0.5 wt% to about 9 wt%, or about 1 wt% to about 9 wt%, or about 1.5 wt% and about 9 wt%, or about 2 wt% and about 9 wt%, or about 2.5 wt% and about 9 wt%, or about 3 wt% and about 9 wt%, or about 3.5 wt% and about 9 wt%, or about 4 wt% It is present in amounts of % and about 9 wt%, or about 4.5 wt% and about 9 wt%, or about 5 wt% and about 9 wt%, or 0.1 wt% and about 8.5 wt%, or in amounts of about 0.5 wt% to about 8.5 wt%, or about 1 wt% to about 8.5 wt%, or about 1.5 wt% and about 8.5 wt%, or about 2 wt% and about 8.5 wt%, or about 2.5 wt% and about 8.5 wt%, or about 3 wt% and about 8.5 wt%, or about 3.5 wt% and about 8.5 wt%, or about 4 wt% It is present in amounts of approximately 8.5 wt%, or approximately 4.5 wt% and approximately 8.5 wt%, or approximately 5 wt% and approximately 8.5 wt%, or 0.1 wt% and approximately 8 wt%, and based on the cellulose ester composition, it is present in amounts of approximately 0.5 wt% to approximately 8 wt%, or approximately 1 wt% to approximately 8 wt%, or approximately 1.5 wt% to approximately 8 wt%, or approximately 2 wt% to approximately 8 wt%, or approximately 2.5% to approximately 8%, or approximately 3% to approximately 8%, or approximately 3.5% to approximately 8 wt%, or approximately 4 wt% to approximately 8%, or approximately 4.5% to approximately 8%, or approximately 5% to approximately 8% by weight.

[0046] Neutralizing agent Melt-processable cellulose ester compositions also contain at least one neutralizing agent. A neutralizing agent is also required in the formulation to control alkalinity or free alkali as a source of color. The neutralizing agent is a carboxylic acid having a first pKa in the range of about 2 to about 7 or about 2 to about 6. Examples of neutralizing agents, but not limited to these, include citric acid, malic acid, succinic acid, adipic acid, fumaric acid, formic acid, lactic acid, maleic acid, tartaric acid, malonic acid, glutamic acid, glutaric acid, gluconic acid, isophthalic acid, terephthalic acid, glycolic acid, itaconic acid, ferulic acid, mandelic acid, aconitic acid, benzoic acid, aspartic acid, and vanillic acid.

[0047] In one embodiment, or in combination with any other embodiment, the neutralizing agent is selected from the group consisting of citric acid, malic acid, succinic acid, adipic acid, and fumaric acid, particularly for use in cellulose ester compositions in food contact applications. In one embodiment, or in combination with any other embodiment, the neutralizing agent is selected from the group consisting of citric acid, adipic acid, or fumaric acid.

[0048] The minimum amount of the neutralizing agent is an amount sufficient to neutralize the free alkali in the cellulose ester composition. However, an excessive amount may be added. In one embodiment, or in combination with any other embodiment, about 0.5 wt% to about 5 wt% of the neutralizing agent is added based on the weight of the cellulose ester composition. In one embodiment, or in combination with any other embodiment, the neutralizing agent is present at about 0.5 wt% to about 5 wt%, or about 0.5 wt% to about 4.5 wt%, or about 0.5 wt% to about 4 wt%, or about 0.5 wt% to about 3.5 wt%, or about 0.5 wt% to about 3 wt%, or about 0.5 wt% to about 2.5 wt%, or about 0.5 wt% to about 2 wt%, or about 0.5 wt% to about 1 wt%, or about 1.5 wt% to about 5 wt%, or about 1.5 wt% to about 4.5 wt%, or 1 wt% to about 5 wt%, or about 1 wt% to about 4.5 wt%, or about 1 wt% to about 4 wt%, or about 1 wt% to about 3.5 wt%, or about 1 wt% to about 3 wt%, or about 1 wt% to about 2.5 wt%, or about 1.5 wt% to about 5 wt%, or about 1.5 wt% to about 4.5 wt%, or about 1.5 wt% to about 4 wt%, or about 1.5 wt% to about 3.5 wt%, or about 1.5 wt% to about 3 wt%, or about 1.5 wt% to about 2.5 wt%, or about 2 wt% to about 5 wt%, or about 2 wt% to about 4.5 wt%, or about 2 wt% to about 4 wt%, or about 2 wt% to about 3.5 wt%, or about 2 wt% to about 3 wt% based on the weight of the cellulose ester composition, and the neutralizing agent is added.

[0049] Appearance The appearance of an article containing a melt-processable cellulose ester composition is important for its acceptability in many applications. For example, bright colors and transparency are desirable properties for many melt-processed articles such as packaging, bags, films, bottles, food containers, straws, stirrers, cups, dishes, bowls, take-out trays and lids, and cutlery.

[0050] CIE L * a * b * In the color space, L * value is a measure of lightness, L* =0 is black, L * =100 is white. Therefore, the color of the item is L * The value is in the upper half of that range, or L * If >50, it may be considered bright. In one embodiment, or in combination with any other embodiment, the L of the cellulose ester composition * This can range from 50-100, 50-95, 50-90, 50-85, 50-80, 50-75, 55-100, 55-95, 55-90, 55-85, 55-80, 55-75, 60-100, 60-95, 60-90, 60-85, 60-80, 60-75, 65-100, 65-95, 65-90, 65-85, 65-80, or 65-75.

[0051] Opacity is a measure of light transmission through a film or article. Transparency refers to the optical clarity through which an object can be observed when viewed through a film or sheet. Perceived opacity and transparency depend on the thickness of the sample. In the application examples above, the thickness of the article can range from about 1 mil for packaging film to over 60 mils for injection-molded blades. Transparency can be particularly important for viewing the contents of a container, for example, through the side of a bottle or through the lid of a container. The thickness of melt-processed containers, cups, and lids varies from about 10 mils to about 30 mils, while bottles are about 20 mils thick.

[0052] The boundary between transparent, translucent, and opaque is often highly subjective. In this study, opacity was measured as the percentage transmittance of 600 nm light through a 30 mil thick film. In one embodiment, or in combination with any other embodiment, the percentage transmittance of the cellulose ester composition of the present invention may range from about 1% to about 100%, about 1% to about 90%, about 1% to about 80%, about 1% to about 70%, about 1% to about 60%, about 1% to about 50%, about 1% to about 40%, about 1% to about 30%, about 1% to about 20%, about 1% to about 10%, and about 1%.

[0053] Transparency was quantified as color difference, or Delta E (CIE76). On a typical scale, Delta E values ​​range from 0 to 100. The human eye's ability to distinguish between two colors is related to Delta E; colors with Delta E < 1 cannot be perceived as different. Conversely, colors with Delta E > 10 are perceived as different at a glance. We used a Delta E cutoff of 20 to specify the easily recognizable difference between black and white when observed through a 30 mil extruded film. The formula for Delta E (CIE76) is:

[0054]

number

[0055] In one embodiment, or in combination with any other embodiment, the delta E of the cellulose ester composition may be in the range of about 20 to about 100. Other elements of the composition In one embodiment, or in combination with any other embodiment, a melt-processable cellulose ester composition may further include at least one selected from the group consisting of non-alkaline fillers, additives, biopolymers, stabilizers, and / or odor modifiers. Examples of additives include waxes, compatibilizers, biodegradation accelerators, dyes, pigments, colorants, fragrances, gloss modifiers, lubricants, antioxidants, viscosity modifiers, antifungal agents, antifogging agents, flame retardants, heat stabilizers, impact modifiers, antimicrobial agents, softeners, mold release agents, and combinations thereof. It should be noted that multiple categories of components in a cellulose ester composition may identify or contain the same type of compound or material. For example, polyethylene glycol (PEG) may function as a plasticizer or as an additive that does not function as a plasticizer, such as a hydrophilic polymer or a biodegradation accelerator. For example, PEG with a lower molecular weight has a plasticizing effect, while PEG with a higher molecular weight functions as a hydrophilic polymer but does not have a plasticizing effect.

[0056] In one embodiment, or in combination with any other embodiment, the cellulose ester composition comprises at least one stabilizer. While the cellulose ester composition is preferably constructible and / or biodegradable, certain amounts of stabilizers may be added to provide selected lifespan or stability, such as stability to light exposure, oxidative stability, or hydrolysis stability. In various embodiments, the stabilizer may include UV absorbers, antioxidants (such as ascorbic acid, BHT, BHA), other acids and radical scavengers, epoxidized oils, such as epoxidized soybean oil, or combinations thereof.

[0057] Antioxidants can be classified into several classes, including primary and secondary antioxidants. Primary antioxidants are generally known to function essentially as free radical terminators (scavengers). Secondary antioxidants are generally known to decompose hydroperoxides (ROOHs) into non-reactive products before they decompose into alkoxy and hydroxyl radicals. Secondary antioxidants are often used in combination with free radical scavengers (primary antioxidants) to achieve synergistic inhibitory effects, and secondary AOs are used to extend the lifetime of phenolic primary AOs.

[0058] A "primary antioxidant" is an antioxidant that acts by reacting with peroxide radicals via hydrogen transfer, thereby quenching the radicals. Primary antioxidants generally contain reactive hydroxyl or amino groups, such as hindered phenols and secondary aromatic amines. Examples of primary antioxidants include BHT, Irganox® 1010, 1076, 1726, 245, 1098, 259 and 1425; Ethanox® 310, 376, 314 and 330; Evernox® 10, 76, 1335, 1330, 3114, MD1024, 1098, 1726, 120, 2246 and 565; Anox® 20, 29, 330, 70, IC-14 and 1315; Lowinox™ 520, 1790, 22IB46, 22M46, 44B25, AH25, GP45, CA22, CPL, HD98, TBM-6 and WSP; Naugard™ 431, PS48, SP and 445; Songnox™ 1010, 1024, 1035, 1076CP, 1135LQ, 1290PW, 1330FF, 1330PW, 2590PW and 3114FF; and ADK Stab AO-20, AO-30, AO-40, AO-50, AO-60, AO-80 and AO-330.

[0059] Secondary antioxidants are often called hydroperoxide decomposers. They act by reacting with hydroperoxides and breaking them down into non-radical, non-reactive, and thermally stable products. Secondary antioxidants are often used in conjunction with primary antioxidants. Examples of secondary antioxidants include compounds of the organophosphorus (e.g., phosphites, phosphonites) and organosulfur classes. The phosphorus and sulfur atoms in these compounds react with peroxides to convert them into alcohols. Examples of secondary antioxidants include Ultranox 626, Ethanox (trademark) 368, 326 and 327; Doverphos (trademark) LPG11, LPG12, DP S-680, 4, 10, S480, S-9228, S-9228T; Evernox (trademark) 168 and 626; Irgafos (trademark) 126 and 168; Weston (trademark) DPDP, DPP, EHDP, PDDP, TDP, TLP and TPP; Mark (trademark) CH302, CH55, TNPP, CH66, CH300, CH301, CH302, CH304 and CH305; ADK Stab2112, HP-10, PEP-8, PEP-36, 1178, 135A, 1500, 3010, C and TPP; Weston439, DHOP, DPDP, DPP, DPTDP, EHDP, PDDP, PNPG, PTP, PTP, TDP, TLP, TPP, 398, 399, 430, 705, 705T, TLTTP and TNPP; Alkanox240, 626, 626A, 627AV, 618F and 619F; and Songnox(trademark) 1680FF, 1680PW and 6280FF.

[0060] In one embodiment, or in combination with any other embodiment, the cellulose ester composition comprises at least one stabilizer, the stabilizer comprising one or more secondary antioxidants. In one embodiment, or in combination with any other embodiment, the stabilizer comprises a first stabilizer component selected from one or more secondary antioxidants, and a second stabilizer component selected from one or more primary antioxidants, or a combination thereof.

[0061] In one embodiment, or in combination with any other embodiment, the stabilizer is present in a weight percentage of the total amount of secondary antioxidants, based on the total weight of the composition, of 0.01 to 0.8, or 0.01 to 0.7, or 0.01 to 0.5, or 0.01 to 0.4, or 0.01 to 0.3, or 0.01 to 0.25, or 0.01 to 0.2, or 0.05 to 0.8, or 0.05 to 0.7 , or includes one or more secondary antioxidants in amounts within the range of 0.05-0.5, 0.05-0.4, 0.05-0.3, 0.05-0.25, 0.05-0.2, 0.08-0.8, 0.08-0.7, 0.08-0.5, 0.08-0.4, 0.08-0.3, 0.08-0.25, or 0.08-0.2. In one class of this embodiment, the stabilizer includes a secondary antioxidant that is a phosphite compound. In one class of this embodiment, the stabilizer includes a secondary antioxidant that is a phosphite compound and another secondary antioxidant that is DLTDP.

[0062] In one subclass of this class, the stabilizer further comprises a second stabilizer component containing one or more primary antioxidants in an amount ranging from 0.05 to 0.7, or 0.05 to 0.6, or 0.05 to 0.5, or 0.05 to 0.4, or 0.05 to 0.3, or 0.1 to 0.6, or 0.1 to 0.5, or 0.1 to 0.4, or 0.1 to 0.3, based on the total weight of the composition. In another subclass of this class, the stabilizer further comprises a second stabilizer component containing citric acid in an amount ranging from 0.05 to 0.2, or 0.05 to 0.15, or 0.05 to 0.1, based on the total weight of the composition. In yet another subclass of this class, the stabilizer further comprises a second stabilizer component containing one or more primary antioxidants and citric acid in amounts discussed herein. In one subclass of this class, the stabilizer contains less than 0.1 wt% of a primary antioxidant based on the total weight of the composition, or does not contain a primary antioxidant. In one subclass of this class, the stabilizer contains less than 0.05 wt% of a primary antioxidant based on the total weight of the composition, or does not contain a primary antioxidant.

[0063] In one embodiment, or in combination with any other embodiment, the cellulose ester composition comprises at least one non-alkaline filler. In one embodiment, or in combination with any other embodiment, the other filler is at least one selected from the group consisting of carbohydrates (sugars and salts), cellulose and organic fillers (ground nut shells, cork powder, cereal by-products [e.g., rice husks, oat bran], wood flour, wood fiber, hemp, carbon, coal particles, graphite and starch), mineral and inorganic fillers (talc, silica, silicate, titanium dioxide, glass fiber, glass spheres, borindite, aluminum trihydrate, alumina and clay), food waste or by-products (egg shells, distilled grains and coffee powder), desiccants (e.g., calcium sulfate, magnesium sulfate), alkaline fillers other than those defined in the claims (e.g., CaO, Na2CO3), or combinations of these fillers (e.g., mixtures). In one embodiment, or in combination with any other embodiment, the cellulose ester composition may also comprise at least one filler that functions as a coloring additive. In one embodiment, or in combination with any other embodiment, the color-adding filler may be selected from carbon, graphite, titanium dioxide, opacifiers, dyes, pigments, toners, and combinations thereof. In one embodiment, or in combination with any other embodiment, the cellulose ester composition may include at least one filler that also functions as a stabilizer or flame retardant.

[0064] In one embodiment, or in combination with any other embodiment, the cellulose ester composition is, based on the total weight of the cellulose ester composition, in amounts of 1-60 wt%, or 5-55 wt%, or 5-50 wt%, or 5-45 wt%, or 5-40 wt%, or 5-35 wt%, or 5-30 wt%, or 5-25 wt%, or 10-55 wt%, or 10-50 wt%, or 10-45 wt%, or 10-40 wt%, or 10-35 wt%, or The further comprises at least one non-alkaline filler (as described herein) in an amount of 10-30 wt%, or 10-25 wt%, or 15-55 wt%, or 15-50 wt%, or 15-45 wt%, or 15-40 wt%, or 15-35 wt%, or 15-30 wt%, or 15-25 wt%, or 20-55 wt%, or 20-50 wt%, or 20-45 wt%, or 20-40 wt%, or 20-35 wt%, or 20-30 wt%.

[0065] In one embodiment, or in combination with any other embodiment, depending on the application, for example in disposable food contact applications, the cellulose ester composition may contain at least one odor-modifying additive. In one embodiment, or in combination with any other embodiment, depending on the application and the components used in the cellulose ester composition, suitable odor-modifying additives may be selected from vanillin, Pennyroyal M-1178, almond, cinnamyl, spices, spice extracts, volatile organic compounds or small molecules, and Plastidor. In one embodiment, or in combination with any other embodiment, the odor-modifying additive may be vanillin. In one embodiment, or in combination with any other embodiment, the cellulose ester composition may contain an amount of odor-modifying additive of 0.01 to 1 wt%, or 0.1 to 0.5 wt%, or 0.1 to 0.2 wt%, or 0.1 to 0.2 wt%, based on the total weight of the composition. The mechanism of the odor-modifying additive may include masking, capture, capture, or a combination thereof.

[0066] As discussed above, the cellulose ester composition may contain other additives. In one embodiment, or in combination with any other embodiment, the cellulose ester composition may contain at least one compatibilizer. In one embodiment, or in combination with any other embodiment, the compatibilizer may be either a non-reactive or reactive compatibilizer. The compatibilizer may improve the ability of the cellulose ester or another component to reach a desired small particle size in order to improve the dispersion of selected components in the composition. In such embodiments, depending on the desired formulation, the biodegradable cellulose ester may be in either a continuous or discontinuous phase of the dispersion. In one embodiment, or in combination with any other embodiment, the compatibilizer used may improve the mechanical and / or physical properties of the composition by modulating the interfacial interactions / bonding between the biodegradable cellulose ester and another component, such as other biodegradable polymers.

[0067] In one embodiment, or in combination with any other embodiment, the cellulose ester composition contains a compatibilizer in an amount of about 1 to about 40 wt%, or about 1 to about 30 wt%, or about 1 to about 20 wt%, or about 1 to about 10 wt%, or about 5 to about 20 wt%, or about 5 to about 10 wt%, or about 10 to about 30 wt%, or about 10 to about 20 wt%, based on the weight of the cellulose ester composition.

[0068] In one embodiment, or in combination with any other embodiment, the cellulose ester composition may optionally contain biodegradable and / or degrading agents, such as hydrolysis aids or any intentional degradation-promoting additives, which are added to or contained in the cellulose ester composition during or after the production of biodegradable cellulose ester (BCE) and melted or solvent-blended with the BCE to form the cellulose ester composition. In one embodiment, or in combination with any other embodiment, the additives may promote hydrolysis by releasing acidic or basic residues, and / or accelerate photocatalytic (UV) or oxidative degradation, and / or promote the growth of selective microbial colonies in compost and soil media to aid in disintegration and biodegradation. In addition to promoting degradation, these additives may have additional functions such as improving the processability of the article or improving desired mechanical properties.

[0069] An example of a possible set of decomposing agents includes inorganic carbonates, synthetic carbonates, nephrite syenite, talc, aluminum hydroxide, diatomaceous earth, natural or synthetic silica, calcined clay, etc. In embodiments, it may be desirable that these additives be well dispersed in the cellulose ester composition matrix. The additives may be used individually or in combination of two or more.

[0070] Another example of a possible set of decomposition agents is aromatic ketones used as oxidative decomposition agents, including benzophenone, anthraquinone, anthrone, acetylbenzophenone, 4-octylbenzophenone, etc. These aromatic ketones may be used individually or in combination of two or more.

[0071] Other examples include transition metal compounds used as oxidative decomposition agents, such as salts of cobalt or magnesium, such as aliphatic carboxylic acid (C12-C20) salts of cobalt or magnesium, or cobalt stearate, cobalt oleate, magnesium stearate, and magnesium oleate; or anatase-type titanium dioxide or titanium dioxide may be used. Mixed-phase titanium dioxide particles may be used, in which both rutile and anatase crystal structures are present within the same particle. The photoactivator particles may have a relatively high surface area of ​​about 10 to about 300 sq.m / g, or 20 to 200 sq.m / g, as measured, for example, by the BET surface area method. The photoactivator may be added to the plasticizer if desired. These transition metal compounds may be used alone or in combination of two or more.

[0072] Examples of rare earth compounds that can be used as oxidative decomposition agents include rare earth elements belonging to Group 3A of the periodic table and their oxides. Specific examples include cerium (Ce), yttrium (Y), neodymium (Nd), rare earth oxides, hydroxides, rare earth sulfates, rare earth nitrates, rare earth acetates, rare earth chlorides, rare earth carboxylates, etc. More specific examples include cerium oxide, cerium sulfate, cerium ammonium sulfate, cerium ammonium nitrate, cerium acetate, lanthanum nitrate, cerium chloride, cerium nitrate, cerium hydroxide, cerium octolate, lanthanum oxide, yttrium oxide, scandium oxide, etc. These rare earth compounds may be used alone or in combination of two or more.

[0073] In one embodiment, or in combination with any other embodiment, the melt-processable cellulose ester composition includes additives having biodegradability-enhancing properties, such as enzymes, bacterial cultures, sugars, glycerol, or other energy sources. The additives may also include hydroxylamine esters and thio compounds.

[0074] In certain embodiments, other possible biodegradable and / or degrading agents may include swelling agents and disintegrants. Swelling agents may be hydrophilic materials that increase in volume after absorbing water and exert pressure on the surrounding matrix. Disintegrants may be additives that facilitate the breakdown of the matrix into smaller fragments in an aqueous environment. Examples include minerals and polymers containing crosslinked or modified polymers and swellable hydrogels. In embodiments, the BCE composition may include water-swellable minerals or clays and their salts, e.g., laponite and bentonite; hydrophilic polymers, e.g., poly(acrylic acid) and salts, poly(acrylamide), poly(ethylene glycol) and poly(vinyl alcohol); polysaccharides and gums, e.g., starch, alginate, pectin, chitosan, psyllium, xanthan gum; guar gum, locust bean gum; and modified polymers, e.g., crosslinked PVP, sodium starch glycolate, carboxymethylcellulose, gelatinized starch, croscarmellose sodium; or combinations of these additives.

[0075] Other examples of hydrophilic polymers or biodegradation accelerators may include glycols, polyglycols, polyethers and polyhydric alcohols, or other biodegradable polymers, such as poly(glycolic acid), poly(lactic acid), polyethylene glycol, polypropylene glycol, polydioxane, polyoxalate, poly(α-ester), polycarbonate, polyanhydride, polyacetal, polycaprolactone, poly(orthoester), polyamino acid, poly(hydroxyalkanoate), aliphatic polyesters, such as poly(butylene) succinate, poly(ethylene) succinate, starch, regenerated cellulose, or aliphatic-aromatic polyesters, such as PBAT, and co-polyesters of any of these.

[0076] In one embodiment, or in combination with any other embodiment, examples of colorants include carbon black, iron oxides, e.g., red or blue iron oxide, titanium dioxide, silicon dioxide, cadmium red, calcium carbonate, kaolin clay, aluminum hydroxide, barium sulfate, zinc oxide, aluminum oxide; and organic pigments, e.g., azo, diazo, and triazo pigments, condensed azo, azo lake, naphthol pigment, anthrapyrimidine, benzimidazolone, carbazole, diketopyrrolopyrrole, flavantron, indigoid pigment, isoindolinone, isoindoline, isobiolantron, and metals. This may include complex pigments, oxazines, perylenes, perinones, pyrantrons, pyrazoloquinazolones, quinophthalones, triarylcarbonium pigments, triphendioxazines, xanthenes, thioindigos, indanthrons, isoindanthrons, anthantrons, anthraquinones, isodibenzantrons, triphendioxazines, quinacridones, and phthalocyanine series, particularly copper phthalocyanines and their nuclear halogenated derivatives, as well as lakes of acids, bases, and mordant dyes, as well as isoindolinone pigments, as well as plant and vegetable dyes, and any other available colorants or dyes.

[0077] In one embodiment, or in combination with any other embodiment, gloss control agents and fillers for adjusting gloss may include silica, talc, clay, barium sulfate, barium carbonate, calcium sulfate, calcium carbonate, magnesium carbonate, and the like.

[0078] Suitable flame retardants may include silica, metal oxides, phosphates, catechol phosphates, resorcinol phosphates, borates, inorganic hydrates, and aromatic polyhalides.

[0079] Antifungal and / or antimicrobial agents include polyene antifungal agents (e.g., natamycin, rimocidine, philipin, nystatin, amphotericin B, candicin, and hamycin), imidazole antifungal agents (e.g., miconazole (available from WellSpring Pharmaceutical Corporation as MICATIN®), ketoconazole (marketed from McNeil Consumer Healthcare as NIZORAL®), and clotrimazole (LOTRAMIN® and LOTRAMIN from Merck). Triazole antifungals (marketed as AF® and also available from Bayer as CANESTEN®), econazole, omoconazole, bifonazole, butoconazole, fenticonazole, isoconazole, oxiconazole, sertaconazole (marketed from OrthoDematologics as ERTACZO®), sulconazole, and ticonazole; triazole antifungals, e.g., fluconazole, itraconazole, isabconazole, rabconazole, posaconazole, voriconazole, terconazole, and albaconazole); thiazole antifungals (e.g., abafungin); allylamine antifungals (e.g., terbinafine (marketed from Novartis Consumer Health, Inc. as LAMISIL®), naftifine (marketed from Merz Pharmaceuticals as NAFTIN®), and butenafine (from Merck as LOTRAMIN) This includes echinocandin antifungal agents (e.g., anidurafungin, caspofungin, and micafungin), polygodial, benzoic acid, cyclopirox, tolnaphthate (e.g., TINACTIN® from MDS Consumer Care, Inc.), undecylenic acid, flucytosine, 5-fluorocytosine, griseofulvin, haloprogin, caprylic acid, and any combination thereof.

[0080] Viscosity modifiers that can be used for the purpose of adjusting the melt flow index or viscosity of biodegradable cellulose ester compositions include polyethylene glycol and polypropylene glycol, as well as glycerin.

[0081] In one embodiment, or in combination with any other embodiment, other components that may be included in the melt-workable cellulose ester composition may function as release agents or lubricants (e.g., fatty acids, ethylene glycol distearate), anti-blocking or slip agents (e.g., fatty acid esters, metal stearates (e.g., zinc stearate) and waxes), anti-fogging agents (e.g., surfactants), heat stabilizers (e.g., epoxy stabilizers, epoxidized soybean oil (ESBO), linseed oil and sunflower oil derivatives), antistatic agents, foaming agents, biocides, impact modifiers, or reinforcing fibers. Two or more components may be present in the BCE composition. Note that additional components may perform two or more functions in the melt-workable cellulose ester composition. The different (or specific) functionality of any particular additive (or component) to the melt-workable cellulose ester composition may depend on its physical properties (e.g., molecular weight, solubility, melting temperature, Tg, etc.) and / or the amount of such additive / component in the composition as a whole. For example, polyethylene glycol can function as a plasticizer at one molecular weight, or as a hydrophilic agent (having little to no plasticizing effect) at another molecular weight.

[0082] In embodiments, fragrances may be added as desired. Examples of fragrances include spices, spice extracts, herb extracts, essential oils, stimulants, volatile organic compounds, volatile small molecules, methyl formate, methyl acetate, methyl butyrate, ethyl acetate, ethyl butyrate, isoamyl acetate, pentyl butyrate, pentyl valerate, octyl acetate, myrcene, geraniol, nerol, citral, citronellal, citronellol, linalool, nerolidol, limonene, camphor, terpineol, alpha-ionone, thujone, benzaldehyde, eugenol, isoeugenol, cinnamaldehyde, ethyl maltol, Vanilla, vanillin, cinnamyl alcohol, anisole, anethole, estragole, thymol, furaneol, methanol, rosemary, lavender, citrus, freesia, apricot blossom, green vegetables, peach, jasmine, rosewood, pine, thyme, oakmoss, musk, vetiver, myrrh, blackcurrant, bergamot, grapefruit, acacia, passionflower, sandalwood, tonka bean, mandarin, neroli, violet leaves, gardenia, red berries, ylang-ylang, king oak, mimosa, tonka bean, wood, ambergris, trumpet Daffodil, hyacinth, narcissus, blackcurrant buds, iris, raspberry, lily of the valley, sandalwood, vetiver, cedarwood, neroli, strawberry, carnation, oregano, honey, musk, heliotrope, caramel, coumarin, patchouli, dewberry, helonial, coriander, pimentoberry, labdanum, king oak, aldehyde, orchid, amber, orris, night-blooming jasmine, palmarosa, cinnamon, nutmeg, moss, styrax, pineapple, foxglove, tulip, wisteria, clematis, anne Bergliss, gum, resin, musk, plum, beaver, musk, myrrh, geranium, rose violet, daffodil, spicy carnation, galbanum, petitgrain, iris, honeysuckle, pepper, raspberry, benzoin, mango, coconut, hesperides, beaver, osmanthus, oakmoss, nectarine, mint, anise, cinnamon, orris, apricot, plumeria, marigold, rose oil, daffodil, tolu balsam, frankincense, amber, orange blossom, bourbon vetiver, opopanax,White musk, papaya, sugar candy, jackfruit, honey, lotus flower, lily of the valley, mulberry, wormwood, ginger, juniper berry, scented benzoin, peony, violet, lemon, lime, hibiscus, white rum, basil, lavender, balsamics, fo-ti-tieng, osmanthus, karo karunde, white orchid, calla lily, white rose, royal lily, mandarin orange, ambergris, ivy, lawn, rubber tree, spearmint, clary sage, poplar, grape, brimbelle, lotus, cyclamen, orchid, glycine, tiare flower, Hepatica nobilis, green osmanthus, passionflower, blue rose, bellflower, goldenrod, African mandarin orange, Anatolian rose Rose, Auvergne narcissus, British broom, British broom chocolate, Bulgarian rose, Chinese patchouli, Chinese gardenia, Calabrian mandarin, Comoros Island tuberose, Ceylonese cardamom, Caribbean passion fruit, Rosa damascena, Georgia peach, white lily, Egyptian jasmine, Egyptian marigold, Ethiopian musk, Farnesian cassie, Florentine iris, French jasmine, French daffodil, French hyacinth, Guinea oranges, Guyana wacapua, Grasse petitgrain Petitgrain, Grasse rose, Grasse tuberose, Haitian vetiver, Hawaiian pineapple, Israeli basil, Indian sandalwood, Indian Ocean vanilla, Italian bergamot, Italian iris, Jamaican pepper, May rose, Madagascar ylang-ylang, Madagascar vanilla,This may include Moroccan jasmine, Moroccan rose, Moroccan oakmoss, Moroccan orange blossoms, Mysore sandalwood, Oriental rose, Russian leather, Russian coriander, Sicilian mandarin, South African marigold, South American tonka bean, Singapore patchouli, Spanish orange blossoms, Sicilian lime, Réunion vetiver, Turkish rose, Thai benzoin, Tunisian orange blossoms, Yugoslav oakmoss, Virginian cedarwood, Utah yarrow, West Indian rosewood, etc., and any combination thereof.

[0083] In one embodiment, or in combination with any other embodiment, a cellulose ester composition and any article made from or containing such a composition comprises a biodegradable cellulose ester (BCE) containing several recycled contents. In an embodiment, the recycled contents are provided by a reactant derived from recycled material, which is a source of one or more acetyl groups on the BCE. In an embodiment, the reactant is derived from recycled plastic. In an embodiment, the reactant is derived from recycled plastic contents syngas. "Recycled plastic contents syngas" means syngas obtained from a synthesis gas operation using raw materials containing at least some content of recycled plastic, which are more fully described below in various embodiments. In an embodiment, recycled plastic contents syngas may be made according to any of the processes for producing syngas described herein; may include or consist of any of the syngas compositions or syngas composition streams described herein; or may be made from any of the raw material compositions described herein.

[0084] In one embodiment, or in combination with any other embodiment, the raw materials (for the synthesis gas operation) may be in the form of a combination of one or more particulate fossil fuel sources and particulate recycled plastics. In one embodiment, or in any of the embodiments mentioned, the solid fossil fuel source may include coal. In one embodiment, or in combination with any other embodiment, the raw materials are supplied to a gasifier together with an oxidizing gas, and the raw materials are converted into syngas.

[0085] In one embodiment, or in combination with any other embodiment, recycled plastic contents syngas is used to produce at least one chemical intermediate in a reaction scheme for producing recycled cellulose esters. In one embodiment, or in combination with any other embodiment, recycled plastic contents syngas may be a component of the raw materials, including other syngas sources, hydrogen, carbon monoxide, or a combination thereof (used to produce at least one CA intermediate). In one embodiment, or in any of the embodiments mentioned, recycled plastic contents syngas is the sole syngas source used to produce the CA intermediate.

[0086] In one embodiment, or in combination with any other embodiment, the CA intermediate prepared using recycled contents syngas, e.g., recycled plastic contents syngas, may be selected from methanol, acetic acid, methyl acetate, acetic anhydride, and combinations thereof. In one embodiment, or in combination with any other embodiment, the CA intermediate may be at least one reactant or at least one product in one or more of the following reactions: (1) syngas conversion to methanol; (2) syngas conversion to acetic acid; (3) methanol conversion to acetic acid, e.g., carbonylation of methanol to produce acetic acid; (4) production of methyl acetate from methanol and acetic acid; and (5) conversion of methyl acetate to acetic anhydride, e.g., carbonylation of methyl acetate and methanol to acetic acid and acetic anhydride.

[0087] In one embodiment, or in combination with any other embodiment, recycled plastic contents syngas is used to produce at least one cellulose reactant. In an embodiment, recycled plastic contents syngas is used to produce at least one recycled cellulose ester.

[0088] In one embodiment, or in combination with any other embodiment, recycled plastic contents syngas is used to produce acetic anhydride. In one embodiment, or in combination with any other embodiment, syngas containing recycled plastic contents syngas is first converted to methanol, which is then used in a reaction scheme for producing acetic anhydride. "RPS acetic anhydride" refers to acetic anhydride derived from recycled plastic contents syngas. "Derived from" means that at least a portion of the raw materials (used in any reaction scheme for producing the CA intermediate) contains a certain amount of recycled plastic contents syngas.

[0089] In one embodiment, or in combination with any other embodiment, RPS acetic anhydride is used as a CA intermediate reactant for esterification of cellulose to prepare recycled BCE, as discussed more thoroughly above. In one embodiment, or in combination with any other embodiment, RPS acetic acid is used as a reactant for preparing cellulose esters or cellulose diacetate.

[0090] In one embodiment, or in combination with any other embodiment, recycled CA is prepared from a cellulose reactant containing anhydride acetate derived from recycled plastic contents syngas.

[0091] In one embodiment, or in combination with any other embodiment, the recycled plastic contents syngas includes a gasification product from a gasification raw material. In one embodiment, or in combination with any other embodiment, the gasification product is produced by a gasification process using a gasification raw material that includes recycled plastic. In the embodiment, the gasification raw material includes coal.

[0092] In the embodiment, the gasification raw material comprises a liquid slurry containing coal and recycled plastic. In the embodiment, the gasification process comprises gasifying the gasification raw material in the presence of oxygen.

[0093] In one embodiment, or in combination with any other embodiment, a recycled cellulose ester composition is provided comprising at least one biodegradable cellulose ester having at least one substituent derived from one or more chemical intermediates on an anhydroglucose unit (AGU), wherein at least one of the chemical intermediates is obtained at least in part from recycled plastic contents syngas.

[0094] In one embodiment, or in combination with any other embodiment, the recycled cellulose ester is biodegradable and contains contents derived from renewable sources, such as wood or cotton linters, and contents derived from recycled material sources, such as recycled plastics. Thus, in embodiments, a melt-workable material is provided that is biodegradable and contains both renewable and recycled contents, i.e., is made from renewable and recycled sources.

[0095] In one embodiment, or in combination with any other embodiment, a cellulose ester composition is provided comprising a recycled cellulose ester prepared by an integrated process comprising the following processing steps: (1) preparing a recycled plastic contents syngas in a synthesis gas operation using a solid fossil fuel source and a raw material containing at least some content of recycled plastic; (2) preparing at least one chemical intermediate from the syngas; (3) reacting the chemical intermediate in a reaction scheme to prepare at least one cellulose reactant for preparing a recycled cellulose ester, and / or selecting the chemical intermediate to be at least one cellulose reactant for preparing a recycled cellulose ester; and (4) reacting at least one cellulose reactant to prepare a recycled cellulose ester, wherein the recycled cellulose ester comprises at least one substituent derived from the recycled plastic contents syngas on an anhydroglucose unit (AGU).

[0096] In one embodiment, or in combination with any other embodiment, processing steps (1) to (4) are carried out in a fluid and / or gas-connected system (i.e., including the possibility of a combination of fluid and gas connections). In one or more reaction schemes for producing recycled cellulose esters starting from recycled plastic contents syngas, it should be understood that chemical intermediates may be temporarily stored in storage containers and then reintroduced into the integrated process system.

[0097] In one embodiment, or in combination with any other embodiment, at least one chemical intermediate is selected from methanol, methyl acetate, acetic anhydride, acetic acid, or a combination thereof. In one embodiment, one chemical intermediate is methanol, which is used in a reaction scheme to produce a second chemical intermediate, which is acetic anhydride. In another embodiment, the cellulose reactant is acetic anhydride.

[0098] Biodegradable cellulose esters useful in embodiments of the present invention may have a degree of substitution in the range of 1.0 to 2.5. In some cases, the cellulose esters described herein may have an average degree of substitution of at least about 1.0, 1.05, 1.1, 1.15, 1.2, 1.25, 1.3, 1.35, 1.4, 1.45 or 1.5, and / or an average degree of substitution of about 2.5, 2.45, 2.4, 2.35, 2.3, 2.25, 2.2, 2.15, 2.1, 2.05, 2.0, 1.95, 1.9, 1.85, 1.8 or 1.75 or less.

[0099] In one embodiment, or in combination with any other embodiment, the biodegradable cellulose ester may have a number-average molecular weight (Mn) of 100,000 or less, or 90,000 or less, as measured using gel permeation chromatography on a polystyrene basis and using N-methyl-2-pyrrolidone (NMP) as the solvent. In some cases, the biodegradable cellulose ester may have an Mn of at least about 10,000, at least about 20,000, 25,000, 30,000, 35,000, 40,000 or 45,000, and / or about 100,000, 95,000, 90,000, 85,000, 80,000, 75,000, 70,000, 65,000, 60,000 or 50,000 or less.

[0100] Biodegradation and decay In embodiments, cellulose ester-containing articles may be biodegradable and may have a certain degree of decay. Biodegradation refers to the mineralization of a substance through the action of microbial metabolism, or its conversion into biomass, CO2, and water. Decay, on the other hand, refers to the visible destruction of a material, often through a combination of physical, chemical, and biological mechanisms.

[0101] In one embodiment, or in combination with any other embodiment, a melt-processable cellulose ester composition exhibits improved disintegration compared to formulations without alkaline fillers. The improvement may be measured as the disintegration of thicker portions over the same period, or it may be referred to as a faster rate of disintegration. The degree of disintegration may be characterized by the weight loss of a sample over a given period of exposure to certain environmental conditions. In some cases, a melt-processable cellulose ester composition may exhibit a weight loss of at least about 5, 10, 15, or 20 percent after 60 days of burial in soil, and / or a weight loss of at least about 15, 20, 25, 30, or 35 percent after 15 days of exposure to a typical municipal waste composting system. However, the rate of disintegration may vary depending on the specific end-use of the article, the composition of the article, and the specific test. Exemplary test conditions are described in U.S. Patents 5,970,988 and 6,571,802.

[0102] In some embodiments, the melt-processable cellulose ester composition may be in the form of biodegradable disposable (molded / pre-formed) articles. The melt-processable cellulose ester compositions described herein may exhibit enhanced levels of environmental non-sustainability, characterized by greater-than-expected degradation under a variety of environmental conditions. The cellulose ester-containing articles described herein may meet or exceed the acceptance criteria set by international testing methods and authorities for industrial compostability, household compostability, and / or soil biodegradability.

[0103] Disintegration refers to the physical breakdown of a material. Disintegration of a material can be influenced by biological, chemical, and / or physical processes. Methods for monitoring disintegration during composting can be performed in synthetic compost under standardized laboratory conditions, or as field tests in reliable industrial or home composting systems. Standardized methods for monitoring disintegration in industrial compost are defined in ISO-20200 and ISO-16929. Qualitative screening tests can also be based on these standardized tests.

[0104] Home composting can be simulated under laboratory conditions, for example, by performing ISO-16929 or ISO-20200 at lower temperatures, or by monitoring the disintegration of test materials in a home composting container. Home composting can also be carried out under similar conditions to those described in the standardized methods, but on a larger scale in outdoor home composting bins.

[0105] To be considered "compostable," a material must meet the following four criteria: (1) The material should pass the biodegradation requirements in tests conducted under controlled composting conditions at high temperature (58°C) in accordance with ISO 14855-1 (2012), which corresponds to 90% absolute biodegradation or 90% relative biodegradation to a control polymer; (2) Materials tested under aerobic composting conditions in accordance with ISO 16929 (2013) or ISO 20200 must reach 90% disintegration; (3) Test materials must meet all requirements regarding volatile solids, heavy metals, and fluorine as specified in ASTM D6400 (2012), EN 13432 (2000), and ISO 17088 (2012); and (4) The material should not adversely affect plant growth. As used herein, the term "biodegradable" generally refers to the biological transformation and consumption of organic molecules. Biodegradability is an inherent property of a material itself, and a material may exhibit different degrees of biodegradability depending on the specific conditions to which it is exposed. The term "collapsible" refers to the tendency of a material to break down into smaller physical fragments when exposed to certain conditions. Collapsibility depends on both the material itself and the physical size and composition of the article being tested. Ecotoxicity is a measure of a material's impact on vegetation, and the heavy metal content of a material is determined according to the procedures presented in standard test methods.

[0106] Cellulose ester compositions (or articles containing them) may exhibit at least 70 percent biodegradation within a period of 50 days or less when tested under aerobic composting conditions at ambient temperature (28°C ± 2°C) in accordance with ISO 14855-1 (2012). In some cases, cellulose ester compositions (or articles containing them) may exhibit at least 70 percent biodegradation within a period of 49, 48, 47, 46, 45, 44, 43, 42, 41, 40, 39, 38, or 37 days when tested under these conditions, also known as “household composting conditions.” These conditions may not be aqueous or anaerobic. In some cases, cellulose ester compositions (or articles containing them) may exhibit total biodegradation of at least about 71, 72, 73, 74, 75, 76, 77, 78, 79, 80, 81, 82, 83, 84, 85, 86, 87, or 88 percent when tested for a period of 50 days under household composting conditions in accordance with ISO 14855-1 (2012). This may represent relative biodegradation of at least about 95, 97, 99, 100, 101, 102, or 103 percent compared to cellulose subjected to the same test conditions.

[0107] To be considered "biodegradable" under home composting conditions according to French standard NF T51-800 and Australian standard AS5810, the material must exhibit at least 90 percent biodegradation overall (compared to, for example, an initial sample), or at least 90 percent of the maximum degradation of a suitable reference material after reaching a plateau in both the reference and test samples. The maximum test period for biodegradation under home composting conditions is one year. The cellulose ester compositions described herein may exhibit at least 90 percent biodegradation within one year, as measured according to 14855-1 (2012), under home composting conditions. In some cases, a cellulose ester composition (or an article containing the same) may exhibit at least about 91, 92, 93, 94, 95, 96, 97, 98, 99, or 99.5 percent biodegradation within one year, as measured according to 14855-1 (2012) under household composting conditions, or a cellulose ester composition (or an article containing the same) may exhibit 100 percent biodegradation within one year.

[0108] Furthermore, or alternatively, the cellulose ester compositions (or articles containing the same) described herein may exhibit at least 90 percent biodegradability within approximately 350, 325, 300, 275, 250, 225, 220, 210, 200, 190, 180, 170, 160, 150, 140, 130, 120, 110, 100, 90, 80, 70, 60, or 50 days, as measured under household composting conditions according to ISO 14855-1 (2012). In some cases, the cellulose ester compositions (or articles containing the same) may be at least approximately 97, 98, 99, or 99.5 percent biodegradable within approximately 70, 65, 60, or 50 test days according to ISO 14855-1 (2012), as measured under household composting conditions. As a result, cellulose ester compositions (or articles containing them) may be considered biodegradable when tested under household composting conditions, for example, according to French standard NF T51-800 and Australian standard AS5810.

[0109] Cellulose ester compositions (or articles containing them) may exhibit at least 60 percent biodegradation within 45 days when tested under aerobic composting conditions at a temperature of 58°C (±2°C) in accordance with ISO 14855-1 (2012). In some cases, cellulose ester compositions (or articles containing them) may exhibit at least 60 percent biodegradation within 44, 43, 42, 41, 40, 39, 38, 37, 36, 35, 34, 33, 32, 31, 30, 29, 28, or 27 days when tested under these conditions, also known as “industrial composting conditions.” These conditions do not necessarily have to be aqueous or anaerobic. In some cases, a cellulose ester composition (or article containing the same) may exhibit total biodegradation of at least about 65, 70, 75, 80, 85, 87, 88, 89, 90, 91, 92, 93, 94, or 95 percent when tested in accordance with ISO 14855-1 (2012) for a period of 45 days under industrial composting conditions. This may represent relative biodegradation of at least about 95, 97, 99, 100, 102, 105, 107, 110, 112, 115, 117, or 119 percent compared to the same cellulose ester composition (or article containing the same) subjected to the same test conditions.

[0110] To be considered "biodegradable" under industrial composting conditions in accordance with ASTM D6400 and ISO 17088, at least 90 percent of the organic carbon in the whole article (or for each component present in more than 1% by dry mass) must be converted to carbon dioxide by the end of the test period, either in comparison to a control or in absolute terms. According to European standard ED13432 (2000), the material must exhibit at least 90 percent biodegradation overall, or at least 90 percent of the maximum biodegradation of a suitable reference material after both the reference and test articles have reached a plateau. The maximum test period for biodegradability under industrial composting conditions is 180 days. The cellulose ester compositions (or articles containing them) described herein may exhibit at least 90 percent biodegradation within 180 days, as measured in accordance with ISO 14855-1 (2012), under industrial composting conditions. In some cases, a cellulose ester composition (or an article containing the same) may exhibit at least about 91, 92, 93, 94, 95, 96, 97, 98, 99, or 99.5 percent biodegradation within 180 days, as measured in accordance with ISO 14855-1 (2012) under industrial composting conditions, or a cellulose ester composition (or an article containing the same) may exhibit 100 percent biodegradation within 180 days.

[0111] Furthermore, or alternatively, the cellulose ester compositions (or articles containing the same) described herein may exhibit at least 90 percent biodegradability within approximately 175, 170, 165, 160, 155, 150, 145, 140, 135, 130, 125, 120, 115, 110, 105, 100, 95, 90, 85, 80, 75, 70, 65, 60, 55, 50, or 45 days under industrial composting conditions, as measured in accordance with ISO 14855-1 (2012). In some cases, the cellulose ester compositions (or articles containing the same) may be at least approximately 97, 98, 99, or 99.5 percent biodegradable within approximately 65, 60, 55, 50, or 45 test days under industrial composting conditions, as measured in accordance with ISO 14855-1 (2012). As a result, the cellulose ester compositions (or articles containing them) described herein may be considered biodegradable in accordance with ASTM D6400 and ISO 17088 when tested under industrial composting conditions.

[0112] Cellulose ester compositions (or articles containing them) may exhibit at least 60 percent biodegradation in soil within 130 days, as measured according to ISO 17556 (2012) under aerobic conditions at ambient temperature. In some cases, cellulose ester compositions (or articles containing them) may exhibit at least 60 percent biodegradation within 130, 120, 110, 100, 90, 80, or 75 days when tested under these conditions, also known as “soil composting conditions.” These conditions do not have to be aqueous or anaerobic. In some cases, cellulose ester compositions (or articles containing them) may exhibit at least about 65, 70, 72, 75, 77, 80, 82, or 85 percent total biodegradation when tested according to ISO 17556 (2012) over a period of 195 days under soil composting conditions. This may represent a relative biodegradation of at least about 70, 75, 80, 85, 90, or 95 percent compared to the same cellulose ester composition (or article containing it) subjected to the same test conditions.

[0113] To be considered "biodegradable" under soil composting conditions according to Vincotte's OK Biodegradable Soil Certificate and DIN CERTCO's DIN Gepruft Soil Biodegradability Certification Scheme, the material must exhibit at least 90 percent biodegradation overall (compared to, for example, an initial sample), or at least 90 percent of the maximum degradation of a suitable reference material after both the reference and test samples have reached a plateau. The maximum test period for biodegradability under soil composting conditions is two years.

[0114] The cellulose ester compositions (or articles containing the same) described herein may exhibit at least 90 percent biodegradation within 2 years, 1.75 years, 1 year, 9 months, or 6 months, as measured under soil composting conditions in accordance with ISO 17556 (2012). In some cases, the cellulose ester compositions (or articles containing the same) may exhibit at least about 91, 92, 93, 94, 95, 96, 97, 98, 99, or 99.5 percent biodegradation within 2 years, as measured under soil composting conditions in accordance with ISO 17556 (2012), or the cellulose ester compositions (or articles containing the same) may exhibit 100 percent biodegradation within 2 years.

[0115] Furthermore, or alternatively, the cellulose ester compositions (or articles containing the same) described herein may exhibit at least 90 percent biodegradability within approximately 700, 650, 600, 550, 500, 450, 400, 350, 300, 275, 250, 240, 230, 220, 210, 200, or 195 days under soil composting conditions, as measured according to ISO 17556 (2012). In some cases, the cellulose ester compositions (or articles containing the same) may be at least approximately 97, 98, 99, or 99.5 percent biodegradable within approximately 225, 220, 215, 210, 205, 200, or 195 days under soil composting conditions, as measured according to ISO 17556 (2012). As a result, the cellulose ester compositions (or articles containing them) described herein may meet the requirements for obtaining Vincotte's OK Biodegradable Soil Conformity Certificate and the requirements for conforming to the standards of DIN CERTCO's DIN Gepruft Soil Biodegradability Certification Scheme.

[0116] In some embodiments, the cellulose ester composition (or article containing the same) of the present invention may contain an unknown biodegradable component in an amount less than 1, 0.75, 0.50, or 0.25 weight percent. In some cases, the cellulose ester composition (or article containing the same) described herein may not contain an unknown biodegradable component.

[0117] To monitor the biodegradation of polymer materials, the water biodegradation test - O2 consumption (OECD 301F) can be used. OECD 301F is an aerobic water biodegradation test that determines the biodegradability of a material by measuring its oxygen consumption. OECD 301F is most frequently used for insoluble and volatile materials. The purity or proportion of the main components of the test material is important in calculating the theoretical oxygen demand (ThOD). As with other 301 test methods, the standard test period for OECD 301F is a minimum of 28 days. A solution or suspension of the test substance in an inorganic culture medium is seeded and incubated under aerobic conditions in the dark or under diffuse light. Cellulose is tested in parallel as a positive control to check the procedure.

[0118] Biodegradation in water is another measure of the biodegradability of a blend of materials. Biological oxygen demand [BOD] was measured over time using the OxiTop® Control OC110 respiratory system. This is achieved by measuring the negative pressure generated when oxygen is consumed in a closed bottle system. NaOH tablets are added to the system to collect the CO2 generated when O2 is consumed. CO2 and NaOH react to form Na2CO3, which draws CO2 from the gas phase, resulting in a measurable negative pressure. The OxiTop measuring head records this negative pressure value and relays the information wirelessly to the controller, which converts the generated CO2 into BOD at a 1:1 ratio. The measured biological oxygen demand can be compared to the theoretical oxygen demand of each test material to determine the percentage of biodegradation. In one embodiment of the present invention, if an alkaline filler is included in the blend, the biodegradation rate in water may be the same or different.

[0119] In addition to being biodegradable under industrial and / or household composting conditions, the cellulose ester compositions (or articles containing them) described herein may also be compostable under household and / or industrial conditions. As previously stated, a material is considered compostable if it meets or exceeds the requirements set forth in EN13432 regarding biodegradability, disintegration capacity, heavy metal content, and ecotoxicity. The cellulose ester compositions (or articles containing them) described herein may exhibit sufficient compostability under household and / or industrial composting conditions to meet the requirements for receiving OK Compost and OK Compost HOME conformity certificates from Vincotte.

[0120] In some cases, the cellulose ester compositions (or articles containing them) described herein may have volatile solid concentrations, heavy metal and fluorine content that meet all the requirements presented in EN13432(2000). Furthermore, the cellulose ester compositions (or articles containing them) may not adversely affect compost quality (including chemical parameters and ecotoxicity tests).

[0121] In some cases, a cellulose ester composition (or an article containing the same) may exhibit at least 90 percent disintegration within 26 weeks under industrial composting conditions, as measured according to ISO 16929 (2013) or ISO 20200. In some cases, a cellulose ester composition (or an article containing the same) may exhibit at least about 91, 92, 93, 94, 95, 96, 97, 98, 99, or 99.5 percent disintegration within 26 weeks under industrial composting conditions, or a cellulose ester composition (or an article containing the same) may exhibit 100 percent disintegration within 26 weeks under industrial composting conditions. Alternatively, or further, a cellulose ester composition (or article containing the same) may exhibit at least 90 percent decay within approximately 26, 25, 24, 23, 22, 21, 20, 19, 18, 17, 16, 15, 14, 13, 12, 11, or 10 weeks under industrial composting conditions, as measured according to ISO 16929 (2013) or ISO 20200. In some cases, the cellulose ester compositions (or articles containing the same) described herein may exhibit at least 97, 98, 99, or 99.5 percent decay within approximately 12, 11, 10, 9, or 8 weeks under industrial composting conditions, as measured according to ISO 16929 (2013) or ISO 20200.

[0122] In some cases, a cellulose ester composition (or an article containing the same) may exhibit at least 90 percent disintegration within 26 weeks under home composting conditions, as measured according to ISO 16929 (2013) or ISO 20200. In some cases, a cellulose ester composition (or an article containing the same) may exhibit at least approximately 91, 92, 93, 94, 95, 96, 97, 98, 99, or 99.5 percent disintegration within 26 weeks under home composting conditions, or a cellulose ester composition (or an article containing the same) may exhibit 100 percent disintegration within 26 weeks under home composting conditions. Alternatively, or further, a cellulose ester composition (or article containing the same) may exhibit at least 90 percent disintegration within approximately 26, 25, 24, 23, 22, 21, 20, 19, 18, 17, 16, or 15 weeks, as measured according to ISO 16929 (2013) or ISO 20200 under home composting conditions. In some cases, the cellulose ester compositions (or articles containing the same) described herein may exhibit at least 97, 98, 99, or 99.5 percent disintegration within 20, 19, 18, 17, 16, 15, 14, 13, or 12 weeks, as measured according to ISO 16929 (2013) or ISO 20200 under home composting conditions.

[0123] In one embodiment, or in combination with any other embodiment, if the cellulose ester composition is formed into a film having a maximum thickness of 0.02, 0.05, 0.07, 0.10, 0.13, 0.25, 0.38, 0.51, 0.64, 0.76, 0.89, 1.02, 1.14, 1.27, 1.40, 1.52, 1.78, 2.0, 2.3, 2.5, 3.0, 3.3, or 3.8 mm, or injection-molded into an article having such a maximum thickness, the film or article will exhibit more than 90% disintegration after 12 weeks according to the disintegration test protocol described herein, or alternatively according to ISO 16929 (2013) or ISO 20200. In certain embodiments, when a cellulose ester composition is formed into a film having a maximum thickness of 0.02, 0.05, 0.07, 0.10, 0.13, 0.25, 0.38, 0.51, 0.64, 0.76, 0.89, 1.02, 1.14, 1.27, 1.40, 1.52, 1.78, 2.0, 2.3, 2.5, 3.0, 3.3, or 3.8 mm, or injection-molded into an article having such a maximum thickness, the film or article exhibits more than 90% disintegration after 12 weeks according to the disintegration test protocol described herein, or alternatively according to ISO (2013) or ISO 20200. In a particular embodiment, when the cellulose ester composition is formed into a film having a thickness of 0.13, 0.25, 0.38, 0.51, 0.64, 0.76, 0.89, 1.02, 1.14, 1.27, 1.40, or 1.52 mm, the film exhibits greater than 90, 95, 96, 97, 98, or 99% disintegration after 12 weeks, according to the disintegration test protocol described herein, or alternatively, according to ISO 16929 (2013) or ISO 20200.In one particular embodiment, the cellulose ester composition is 0.02, or 0.05, or 0.07, or 0.10, or 0.13, or 0.25, or 0.38, or 0.51, or 0.64, or 0.76, or 0.89, or 1.02, or 1.14, or 1.27, or 1.40, or 1.52, or 1.78, or 2.0, or 2.3, or 2.5, or 3.0, or 3.3, if If the film or article is formed to have a maximum thickness of 3.8 mm or is injection-molded to have such a maximum thickness, the film or article shall exhibit more than 90, 95, 96, 97, 98, or 99% disintegration after 8, 9, 10, 11, 12, 13, 14, 15, or 16 weeks, in accordance with the disintegration test protocol described herein, or alternatively, in accordance with ISO 16929 (2013) or ISO 20200.

[0124] In some embodiments, the cellulose ester compositions (or articles containing them) described herein may be substantially free of photodegrading agents. For example, the cellulose ester compositions (or articles containing them) may contain a photodegrading agent in an amount of about 1, 0.75, 0.50, 0.25, 0.10, 0.05, 0.025, 0.01, 0.005, 0.0025, or 0.001 weight percent or less, based on the total weight of the cellulose ester compositions (or articles containing them), or the cellulose ester compositions (or articles containing them) may not contain a photodegrading agent. Examples of such photodegrading agents include, but are not limited to, pigments that act as photo-oxidation catalysts and may be optionally enhanced by the presence of one or more metal salts, oxidizing polomotors, and combinations thereof. The pigments may include coated or uncoated anatase or rutile titanium dioxide, which may exist alone or in combination with one or more reinforcing components, such as various types of metals. Other examples of photodegrading agents include benzoin, benzoin alkyl ethers, benzophenone and its derivatives, acetophenone and its derivatives, quinones, thioxanthones, phthalocyanines and other photosensitizers, ethylene-carbon monoxide copolymers, aromatic ketone-metal salt sensitizers, and combinations thereof.

[0125] End use In one embodiment, or in combination with any other embodiment, a biodegradable, disintegrable, and / or compostable article comprising the cellulose ester composition described herein is provided. In embodiments, the cellulose ester composition may be extrudeable, moldable, castable, thermoformable, or 3D printable.

[0126] In one embodiment, or in combination with any other embodiment, the cellulose ester composition can be melt-processed and molded into useful molded articles, such as disposable food contact articles, which are biodegradable and / or compostable. In one embodiment, or in combination with any other embodiment, the articles are non-sustainable. Environmentally, "non-sustainable" means that when the biodegradable cellulose ester reaches an advanced level of decomposition, it is suitable for complete consumption by natural microbial communities. The decomposition of the biodegradable cellulose ester ultimately results in its conversion into carbon dioxide, water, and biomass. In one embodiment, or in combination with any other embodiment, an article is provided comprising a cellulose ester composition (discussed herein) having a maximum thickness of up to 150 mils, or 140 mils, or 130 mils, or 120 mils, or 110 mils, or 100 mils, or 90 mils, or 80 mils, or 70 mils, or 60 mils, or 50 mils, or 40 mils, or 30 mils, or 25 mils, or 20 mils, or 15 mils, or 10 mils, or 5 mils, or 2 mils, or 1 mil, and being biodegradable and compostable (i.e., passing the industrial or household compostability tests / criteria discussed herein). In one embodiment, or in combination with any other embodiment, an article is provided comprising a cellulose ester composition having a maximum thickness of up to 150 mils, or 140 mils, or 130 mils, or 120 mils, or 110 mils, up to 100 mils, or 90 mils, or 80 mils, or 70 mils, or 60 mils, or 50 mils, or 40 mils, or 30 mils, or 25 mils, or 20 mils, or 15 mils, or 10 mils, or 5 mils, or 2 mils, or 1 mil, and being environmentally non-sustainable (as discussed herein).

[0127] In one embodiment, or in combination with any other embodiment, articles comprising a cellulose ester composition are provided, which are used in food service and food products, horticulture, agriculture, recreation, coatings, textiles, nonwovens, and home / office applications. Examples of food service and food products, but not limited to, include straws, cup lids, composite lids, portion cups, beverage cups, trays, bowls, plates, food containers, container lids, clamshell containers, cutlery, cooking utensils, stirring rods, bottles, bottle caps, bottles, bottle caps, bags, flexible packaging, wraps, baskets for agricultural products, stickers for agricultural products, and twisted yarns. Examples of horticultural and / or agricultural applications, but not limited to, include flower pots, germination trays, transplanting pots, plant tags, buckets, bags for soil and mulch, trimmer strings, agricultural films, mulch films, greenhouse films, silage films, compostable bags, film supports, and twisted yarns for hay packing. Examples of recreational articles, but not limited to, include toys, sporting goods, fishing gear, golf equipment, and camping equipment. Toys may include, but are not limited to, beach toys, blocks, wheels, propellers, sippy cups, doll accessories, and pet toys. Sporting goods may include, but are not limited to, whistles, whiffle balls, paddles, nets, foam balls, and darts, as well as artificial turf. Fishing equipment may include, but are not limited to, floats, lures, nets, and traps. Golf equipment may include, but are not limited to, tees, practice balls, ball markers, and divot tools. Camping equipment may include, but are not limited to, tent stakes, tableware, and cords / ropes. Examples of household and office goods may include, but are not limited to, gift cards, credit cards, signs, labels, report covers, envelopes, tape, tool handles, toothbrush handles, writing instruments, combs, film containers, wire insulation, screw caps, and bottles.

[0128] In one embodiment, or in combination with any other embodiment, the article is made from a moldable thermoplastic material comprising the cellulose ester composition described herein. In one embodiment, or in combination with any other embodiment, the article is a disposable food contact article. Examples of such articles that can be made using a cellulose ester composition include cups, trays, trays with multiple compartments, clamshell packaging, candy sticks, films, sheets, trays and lids (e.g., thermoformed), straws, plates, bowls, portion cups, food packaging, liquid transport containers, solid or gel transport containers, and cutlery. In one embodiment, or in combination with any other embodiment, the cellulose ester may be a coating or layer of the article. The article may contain fibers. In one embodiment, or in combination with any other embodiment, the article may be a horticultural article. Examples of such articles that can be made using a cellulose ester composition include flower pots, plant tags, mulch films, and agricultural ground cover.

[0129] In one embodiment, or in combination with any other embodiment, the cellulose ester has a number-average molecular weight ("M") in the range of 10,000 to 90,000 daltons as measured by GPC. n In one embodiment, or in combination with any other embodiment, the cellulose ester has a number average molecular weight ("M") in the range of 30,000 to 90,000 daltons as measured by GPC. n In one embodiment, or in combination with any other embodiment, the cellulose ester has a number average molecular weight ("M") in the range of 40,000 to 90,000 daltons as measured by GPC. n It has ''.

[0130] In one embodiment, or in combination with any other embodiment, when the composition is formed into a film having a thickness of 0.38 mm, the film exhibits more than 5% disintegration after 6 weeks and more than 90% disintegration after 12 weeks, according to the disintegration test protocol described herein, or alternatively, according to ISO 16929 (2013) or ISO 20200. In one embodiment, or in combination with any other embodiment, when the composition is formed into a film having a thickness of 0.38 mm, the film exhibits more than 10% disintegration after 6 weeks and more than 90% disintegration after 12 weeks, according to the disintegration test protocol described herein, or alternatively, according to ISO 16929 (2013) or ISO 20200. In one embodiment, or in combination with any other embodiment, when the composition is formed into a film having a thickness of 0.38 mm, the film exhibits more than 20% disintegration after 6 weeks and more than 90% disintegration after 12 weeks, according to the disintegration test protocol described herein, or alternatively, according to ISO 16929 (2013) or ISO 20200. In one embodiment, or in combination with any other embodiment, when the composition is formed into a film having a thickness of 0.38 mm, the film exhibits more than 30% disintegration after 6 weeks and more than 90% disintegration after 12 weeks, according to the disintegration test protocol described herein, or alternatively, according to ISO 16929 (2013) or ISO 20200. In one embodiment, or in combination with any other embodiment, when the composition is formed into a film having a thickness of 0.38 mm, the film exhibits more than 50% disintegration after 6 weeks and more than 90% disintegration after 12 weeks, according to the disintegration test protocol described herein, or alternatively, according to ISO 16929 (2013). In one embodiment, or in combination with any other embodiment, when the composition is formed into a film having a thickness of 0.38 mm, the film exhibits more than 70% disintegration after 6 weeks and more than 90% disintegration after 12 weeks, according to the disintegration test protocol described herein, or alternatively, according to ISO 16929 (2013) or ISO 20200.

[0131] In one embodiment, or in combination with any other embodiment, when the composition is formed into a film having a thickness of 0.76 mm, the film exhibits more than 30% disintegration after 12 weeks according to the disintegration test protocol described herein, or alternatively according to ISO 16929 (2013) or ISO 20200. In one embodiment, or in combination with any other embodiment, when the composition is formed into a film having a thickness of 0.76 mm, the film exhibits more than 50% disintegration after 12 weeks according to the disintegration test protocol described herein, or alternatively according to ISO 16929 (2013) or ISO 20200. In one embodiment, or in combination with any other embodiment, when the composition is formed into a film having a thickness of 0.76 mm, the film exhibits more than 70% disintegration after 12 weeks according to the disintegration test protocol described herein, or alternatively according to ISO 16929 (2013) or ISO 20200. In one embodiment, or in combination with any other embodiment, when the composition is formed into a film having a thickness of 0.76 mm, the film exhibits more than 90% disintegration after 12 weeks according to the disintegration test protocol described herein, or alternatively according to ISO 16929 (2013) or ISO 20200. In one embodiment, or in combination with any other embodiment, when the composition is formed into a film having a thickness of 0.76 mm, the film exhibits more than 95% disintegration after 12 weeks according to the disintegration test protocol described herein, or alternatively according to ISO 16929 (2013) or ISO 20200.

[0132] In one embodiment, or in combination with any other embodiment, when the composition is molded into an article having a thickness of 3.7 mm or less, at least 90% of the article will disintegrate in 90 days at 58°C according to standard ISO20200, or when the composition is molded into an article having a thickness of 1.89 mm or less, at least 90% of the article will disintegrate in 90 days at a temperature of 20-30°C according to standard ISO20200.

[0133] In another embodiment, a cellulose acetate tow band is provided comprising a cellulose acetate composition, the cellulose acetate composition comprising at least one cellulose ester, at least one plasticizer, at least one alkaline additive, and at least one neutralizing agent, the cellulose acetate composition being biodegradable according to ASTM D6400 when tested under industrial composting conditions.

[0134] Typical cigarette filters are made from continuous filament tow bands of cellulose acetate-based fibers, called cellulose acetate tow or simply acetate tow. The use of acetate tow for making filters is described in various patents, and the tow may be plasticized. See, for example, U.S. Patent No. 2,794,239.

[0135] Instead of continuous fibers, shorter short fibers that can aid in the final decomposition of the filter may be used. See, for example, U.S. Patent No. 3,658,626, which discloses the manufacture of short fiber cigarette filter elements, etc., directly from continuous filament tow. These short fibers may also be plasticized.

[0136] Acetate tows for cigarette fibers are typically made of Y-shaped small filament denier fibers that are intentionally highly crimped and entangled, as described in U.S. Patent No. 2,953,838. The Y-shape allows for an optimal cigarette filter with the lowest weight for a given pressure drop compared to other fiber shapes. See U.S. Patent No. 2,829,027. Typically, small filament denier fibers in the range of 1.6 to 8 denier (dpf) per filament are used to produce efficient filters. When constructing the filter, the crimp of the fibers allows for improved filter stiffness and a reduction in tow weight for a given pressure drop.

[0137] The conversion of acetate tow to cigarette filters can be achieved using a tow preparation system and a plug maker, as described, for example, in U.S. Patent No. 3,017,309. The tow preparation system draws the tow from the bale, de-registers ("blooms") the fibers, and delivers the tow to the plug maker. The plug maker compresses the tow, wraps it in plug wrap paper, and cuts it into rods of the desired length. To further increase the stiffness of the filter, non-volatile solvents can be added to solvent-bond the fibers together. These solvent-bonding agents are commercially known as plasticizers and have historically included triacetin (glycerol triacetate), diethylene glycol diacetate, triethylene glycol diacetate, trippropionine, acetyl triethyl citrate, and triethyl citrate. Waxes have also been used to increase the stiffness of the filter; see, for example, U.S. Patent No. 2,904,050.

[0138] Conventional plasticizer interfiber binders are useful for binding and selective filtration. However, plasticizers are typically not water-soluble, and the fibers remain bound together for extended periods. In fact, conventional cigarette filters can take years to decompose and disintegrate when discarded, due to the highly entangled nature of the filter fibers, solvent bonding between fibers, and the inherently slow biodegradability of cellulose acetate polymer. Therefore, attempts are being made to develop cigarette filters with improved biodegradability.

[0139] Specific Embodiments Embodiment 1. An article comprising a melt-processable biodegradable cellulose ester composition, wherein the cellulose ester composition is A composition comprising at least one cellulose ester, at least one alkaline filler, and at least one neutralizing agent, wherein a 1% by weight suspension of the alkaline filler has a pH of 8 or higher, the water solubility of the alkaline filler at 20-25°C is greater than 1 ppm but less than 1,000 ppm, and the alkaline filler is present in an amount of about 0.1% to about 35% by weight based on the weight of the cellulose ester composition; or An article comprising at least one type of cellulose acetate, at least one type of plasticizer, at least one type of alkaline filler, and at least one type of neutralizing agent, wherein a 1% suspension of the alkaline filler has a pH of 8 or higher, the water solubility of the alkaline filler at 20-25°C is greater than 1 ppm but less than 1,000 ppm, and the alkaline filler is present in an amount of about 0.1% to about 35% by weight based on the weight of the cellulose ester composition.

[0140] Embodiment 2. The article according to Embodiment 1, wherein the alkaline filler is present in an amount of about 0.1% to about 10% by weight, based on the weight of the cellulose ester composition. Embodiment 3. The article according to Embodiment 1 or 2, wherein the cellulose ester is cellulose acetate.

[0141] Embodiment 4. The article according to any one of Embodiments 1 to 3, wherein the cellulose ester is prepared by converting cellulose to a cellulose ester using a reactant obtained from recycled material.

[0142] Embodiment 5. The plasticizer is glycerol triacetate (triacetin), glycerol diacetate, dibutyl terephthalate, dimethyl phthalate, diethyl phthalate, poly(ethylene glycol) MW200~600, triethylene glycol dipropionate, 1,2-epoxypropylphenylethylene glycol, 1,2-epoxypropyl(m-cresyl)ethylene glycol, 1,2-epoxypropyl(o-cresyl)ethylene glycol, β-oxyethylcyclohexene carboxylate, bis(cyclohexanate)diethylene glycol, triethyl citrate, polyethylene glycol, Benzoflex, propylene glycol, polysorbate, sucrose octaacetate, acetylated triethyl citrate, acetyl tributyl citrate, Admex, trippropionine, Scandiflex, poloxamer copolymer, polyethylene glycol succinate, A An article according to any one of Embodiments 1 to 4, wherein the plasticizer is at least one selected from the group consisting of diisobutyl dipicate, polyvinylpyrrolidone and glycol tribenzoate, triethyl citrate, acetyl triethyl citrate, polyethylene glycol, benzoate-containing plasticizers, e.g., the Benzoflex® plasticizer series, poly(alkyl succinates), e.g., poly(butyl succinate), polyethersulfone, adipate-based plasticizer, soybean oil epoxide, e.g., the Paraplex® plasticizer series, sucrose-based plasticizer, dibutyl sebacate, tributylin, tripionine, sucrose acetate isobutyrate, plasticizers in the Resolflex® series, triphenyl phosphate, glycolate, methoxypolyethylene glycol, 2,2,4-trimethylpentane-1,3-diyrbis(2-methylpropanoate), and polycaprolactone.

[0143] Embodiment 6. An article according to any one of Embodiments 1 to 5, wherein the plasticizer is present in an amount of 1 to 40% by weight. Embodiment 7. The article according to any one of Embodiments 1 to 6, wherein the pH of a 1% by weight solution or suspension of the alkaline filler is in the range of about 8 to about 12.

[0144] Embodiment 8. An article according to any one of Embodiments 1 to 7, wherein the water solubility of the alkaline filler at 20 to 25°C is about 2 ppm to about 400 ppm. Embodiment 9. An article according to any one of Embodiments 1 to 9, wherein the pH of a 1% by weight suspension of an alkaline filler is 8 or higher and the alkaline efficiency is at least 5.

[0145] Embodiment 10. An article according to any one of Embodiments 1 to 9, wherein the alkaline filler is at least one selected from the group consisting of calcium carbonate (CaCO3), magnesium oxide (MgO), magnesium hydroxide (Mg(OH)2), magnesium carbonate (MgCO3), barium carbonate (BaCO3), and hydrated forms of these compounds.

[0146] Embodiment 11. The article according to any one of Embodiments 1 to 10, wherein the alkaline filler is a mixture of calcium carbonate and at least one of magnesium oxide, magnesium hydroxide, or magnesium carbonate, and based on the total weight of the cellulose ester composition, calcium carbonate is present in an amount of 5 to 25% by weight and at least one of magnesium oxide, magnesium hydroxide, or magnesium carbonate is present in an amount of 1 to 20% by weight.

[0147] Embodiment 12. The article according to any one of Embodiments 1 to 11, wherein the neutralizing agent is at least one selected from the group consisting of citric acid, malic acid, succinic acid, adipic acid, fumaric acid, formic acid, lactic acid, maleic acid, tartaric acid, malonic acid, glutamic acid, glutaric acid, gluconic acid, isophthalic acid, terephthalic acid, glycolic acid, itaconic acid, ferulic acid, mandelic acid, aconitic acid, benzoic acid, aspartic acid, and vanillic acid.

[0148] Embodiment 13. An article according to any one of Embodiments 1 to 12, wherein the neutralizing agent has a pKa of 4.5 or less and a boiling point or decomposition temperature of 170°C or higher. Embodiment 14. A melt-processable cellulose ester composition according to any one of Embodiments 1 to 13, wherein the neutralizing agent is citric acid, adipic acid, or fumaric acid.

[0149] Embodiment 15. An article according to any one of Embodiments 1 to 14, wherein about 0.5% to about 5% by weight of a neutralizing agent is present in the cellulose ester composition, based on the weight of the cellulose ester composition.

[0150] Embodiment 16. An article according to any one of Embodiments 1 to 15, selected from the group consisting of biodegradable and / or compostable molded articles. Embodiment 17. An article according to any one of Embodiments 1 to 16, wherein the maximum thickness is up to 150 mils.

[0151] Embodiment 18. An article according to any one of Embodiments 1 to 17, used in food service and groceries, horticulture, agriculture, recreation, coatings, textiles, nonwovens, and home / office applications.

[0152] Embodiment 19. An article according to any one of Embodiments 1 to 18, wherein the maximum thickness of the article is 3.7 mm or less, and at least 90% of the article decomposes in 90 days at 58°C according to the standard ISO 20200.

[0153] Embodiment 20. An article according to any one of Embodiments 1 to 18, wherein the maximum thickness of the article is 1.89 or less, and at least 90% of the article decomposes in 90 days at a temperature of 20°C to 30°C according to the standard ISO 20200. [Examples]

[0154] Abbreviation CA is cellulose acetate, mm is millimeters, TA is triacetin, wt is weight, wt% is weight percent, g is grams, °C is Celsius temperature, °F is Fahrenheit temperature, mL is milliliters, L is liters, ppm is parts per million, CAP is (acetic acid / propionic acid) cellulose (cellulose acetate propionate), h is time, TGA is thermogravimetric analysis, TDS is total evaporation residue, and EC is electrical conductivity.

[0155] Example 1 Free alkali content of inorganic fillers The free alkali content of the inorganic packing material was determined by titration. 2.0 g of the test material was boiled in 100 mL of water for 5 minutes in a covered beaker, and filtered while still hot. 50 mL of the cooled filtrate was titrated with 0.10 N sulfuric acid.

[0156] [Table 3]

[0157] Example 2 The CA-containing material was melt-processed. Formulated pellets: Pellets were extruded using an 18mm (Leistritz) twin-screw extruder with a single-hole die, and these were subsequently used for film extrusion. These pellets were prepared from raw materials consisting of powdered cellulose acetate CA-398-30 obtained from Eastman Chemical Company, liquid plasticizer (polyethylene glycol (PEG400) or TA), and additives. Any dry components were added to the base powder, dry-blended to produce a free-flowing powder, and added to a (Coperion) twin-screw weight-loss feeder. The plasticizer was supplied to zone 2 by a liquid injection unit with a (Witte) gear pump, Hardy 4060 controller, and an injector with a 0.020” bore. The formulated strands were passed through a water tank and pelletized (using a ConAir pelletizer).

[0158] Film Extrusion: Film was produced using a (Maddock) single-screw extruder (3.81 cm (1.5 inch) Killion) equipped with a mixer screw. Compounded cellulose acetate pellets were fed into a hopper, the material was passed through a barrel, and the mixer screw transferred the material toward the die. The barrel housing the screw was heated in three zones to allow for high shear and a high degree of dispersion mixing, as the pellets melted as they passed along the screw through a very narrow gap. It was observed that a homogeneous polymer mixture was formed as it approached the die, and the mixture was pushed through the die by the screw, resulting in extrusion. The extrusion formed a flat molten film as the film exited the die, and the film solidified on a temperature-controlled polished chrome roll (roll stack). Film samples after extrusion were taken intermittently to determine the film thickness. If the extruder produced the appropriate film thickness, the film was mounted on a receiving roller and the film was carefully wound until the final roll was complete.

[0159] Example 3 (counterexample) In formulations containing plasticizers and CA, 5 wt% MgO could not be prepared in the absence of a neutralizing agent.

[0160] Formulations containing only CA, a plasticizer, and 5 wt% alkaline filler failed to melt-process successfully. Cellulose acetate (CA-398-30) plasticized with 20 wt% triacetin (TA) or 20 wt% PEG400 and 5 wt% MgO were formulated according to Example 3. The pellets produced by formulations 4 and 6 were porous and brittle, had a strong odor and dark color, and it was not possible to extrude an intact film from these pellets.

[0161] [Table 4]

[0162] Example 4 Appearance of melt-processed compound of plasticized CA The appearance of the molten CA compound was characterized. After compounding the pellets, a 30 mil thick film was extruded as in Example 2, and a 60 mil plaque was injection molded. Some of the compoundings included alkaline fillers and neutralizing agents, and the appearance of the molten articles was evaluated.

[0163] Using the Konika Minolta Chroma Meter, CR-400, and SpectraMagic NX software, the color of a 60-mil plaque was measured against a white background using CIE L. * a * b * Measured in color space. L * The value is a measure of brightness, L * =0 is black, L * =100 is white. * If the value was >50, the plaque color was characterized as "light".

[0164] Opacity was measured as the percentage transmittance (%T, 600nm) of light passing through a 30 mil extruded film using a Beckman DU530 spectrophotometer. Transparency was evaluated as the color difference (delta E) between the white and black surfaces when measured through the 30 mil extruded film. The appearance of the test specimens is summarized in Table 5.

[0165] [Table 5]

[0166] [Table 6]

[0167] Example 5 Melt-processed articles having an MgO content of less than 5 wt% and citric acid or malic acid as a neutralizing agent. The appearance of the molten CA-398-30 formulation was evaluated according to Example 4. The appearance of the test formulation was evaluated as summarized in Table 7.

[0168] [Table 7]

[0169] Example 6 Melt-processed articles containing 2-5 wt% MgO Appearance of molten articles containing 2-5 wt% MgO, including the addition of an antioxidant (BHT), a chelating agent (EDA), and / or a whitening agent (TiO2). Molten-processed CA398-30 formulations were characterized for their appearance according to Example 4. The appearance of the test articles is summarized in Table 8 below. (BHT = butylated hydroxytoluene, EDA = etidronic acid)

[0170] [Table 8]

[0171] Example 7 Melt-worked articles having Mg(OH)2 as an alkaline additive When a neutralizing agent is added to a molten product containing Mg(OH)2, its color and transparency are improved. Mg(OH)2 can be included in the molten product formulation containing the neutralizing agent up to 5%.

[0172] The molten CA-398-30 formulation was characterized for its appearance according to Example 4. Table 9 below shows the evaluation of the test formulations for their appearance.

[0173] [Table 9]

[0174] Example 8 Biodegradation of CA resin containing 2 wt% MgO in water Screening tests for biodegradation in freshwater were based on the OECD 301F Manometric Respirometry Test. Biological oxygen demand [BOD] was measured over time using an OxiTop® Control OC110 respiratory system. Eastman sludge was used as wastewater inoculum, and solid particles were removed by vacuum filtration. The test was conducted for 56 days. Longer periods allow the test to be used to screen materials that can be classified as easily or intrinsically biodegradable.

[0175] CA resin (Eastman CA398-30) was formulated as a blend with a plasticizer (15 wt% PEG400) and optionally 2 wt% alkaline additive MgO. The components of the formulation were accurately weighed and thoroughly mixed. Good mixing of the components was verified by nearly identical results in three independent reproductions. The formulation was not melted or dissolved before the biodegradation test in water. The initial pH of the inorganic medium was 7.48. The 2 wt% MgO did not affect the rate of biodegradation of CA-398-30 with PEG400 in the blend.

[0176] [Table 10]

[0177] Example 9 Collapse in industrial compost (OWS SAW-27) Qualitative screening tests were conducted based on ISO 16929, and for monitoring purposes, the disintegration of the test material was evaluated during 12 weeks of composting, simulating industrial composting conditions. The 30-mil extruded film test materials from Examples 4-7 were added as 10cm x 10cm pieces, mixed with biological waste, and composted in 200-liter composting jars. The mixture in the jars was periodically stirred manually, and the disintegration of the test material was visually monitored during this time.

[0178] After 12 weeks of composting, only a small amount of microscopic specimen fragments were observed in test samples 9, 10, 16, 17, 28, and 29 (test codes NZ-46, NZ-47, NZ-49, NZ-50, NZ-52, and NZ-53). In contrast, larger fragments of test samples 18 and 30 (test codes NZ-51 and NZ-54) were recovered from the test bottles. A summary of the most significant visual observations and changes during the disintegration of the test samples is shown in Table 12.

[0179] [Table 11]

[0180] [Table 12]

[0181] [Table 13]

[0182] Example 10 Collapse of 60-mil injection-molded plaque inside a home compost jar. CA398-30 was compounded with triacetin (TA) or PEG400, and optionally with CaCO3 or MgO, according to Table 15. Plaques (10.16 cm (4 inch) square and 0.152 cm (0.060 inch) thick) were injection molded from the compounded pellets. The plaques were cut into 2.54 cm (1 inch) × 10.16 cm (4 inch) strips, labeled with colored duct tape, and weighed. Twelve pieces of each test specimen were then placed in a household outdoor compost bin.

[0183] The compost jar was a black plastic tumbler for outdoor use with a total capacity of 140 liters, sold for home use. The jar was placed outdoors and filled to the center axis (approximately 70 liters) with industrial-grade mature compost from a local supplier. Additional materials were added: approximately 24 liters of pine shavings and approximately 6 liters of alfalfa pellets (commercial adult rabbit feed). Water was added to approximately 60% using a squeeze test. The jar was rotated approximately once a week. After rotation, the jar was opened to ensure that all samples were immersed in the compost. Every 6 weeks, 0.5 L of alfalfa pellets were added to the compost. The pH of the compost fluctuated between 6 and 7.5, while the C:N ratio was between 7 and 17.

[0184] Three replicate samples of each test material were collected from an outdoor tumbler after 8, 14, 20, and 26 weeks. Surface residue was removed from the samples, they were dried, and weighed again. The presence of 5 wt% MgO or 15 wt% CaCO3 increased decomposition, which was measured as weight loss in a household compost bin.

[0185] [Table 14]

[0186] Example 11 Collapse of a 125 mil injection-molded tensile rod inside a home compost jar CA398-30 was compounded with PEG400 and, optionally, CaCO3 or MgO according to Table 16. From the compounded pellets, tensile rods (also known as dogbones, 21.59 cm (8.5 inches) long, 0.508–1.905 cm (1 / 5–3 / 4 inches) wide, and 0.318 cm (0.125 inches) thick) were injection molded. The tensile rods were cut in half, labeled with colored duct tape, and weighed. Twelve pieces of each test specimen were then placed in a household outdoor compost bin.

[0187] The compost jar was a black plastic tumbler for outdoor use with a total capacity of 140 liters, sold for home use. The jar was placed outdoors and filled to the center axis (approximately 70 liters) with industrial-grade mature compost from a local supplier. Additional materials were added: approximately 24 liters of pine shavings and approximately 6 liters of alfalfa pellets (commercial adult rabbit feed). Water was added to approximately 60% using a squeeze test. The jar was rotated approximately once a week. After rotation, the jar was opened to ensure that all samples were immersed in the compost. Every 6 weeks, 0.5 L of alfalfa pellets were added to the compost. The pH of the compost fluctuated between 6 and 7.5, while the C:N ratio was between 10 and 13.

[0188] Three replicate samples of each test material were collected from an outdoor tumbler after 8, 14, 20, and 26 weeks. Surface residue was removed from the samples, they were dried, and weighed again. The presence of CaCO3 (15 wt%) or MgO (5 wt%) increased decomposition, which was measured as weight loss in a household compost bin.

[0189] [Table 15]

[0190] Example 12 Collapse of 50-130 mill injection molded blades inside a home compost jar. CA-398-30 was prepared with PEG400 and, optionally, CaCO3 or MgO according to Table 16. Blades were injection molded from the prepared pellets. The knives were labeled with colored duct tape and weighed. Twelve pieces of each test item were then placed in a household outdoor compost bin.

[0191] The compost bin was a black plastic tumbler for outdoor use with a total capacity of 140 liters, sold for home use. The bin was placed outdoors and filled to the center axis (approximately 70 liters) with industrial-grade mature compost from a local supplier. Additional materials were added: approximately 24 liters of pine shavings and approximately 6 liters of alfalfa pellets (commercial adult rabbit feed). Water was added to approximately 60% using a squeeze test. The bin was rotated approximately once a week. After rotation, the bin was opened to ensure that all samples were immersed in the compost. Every 6 weeks, 0.5 L of alfalfa pellets were added to the compost. The pH of the compost fluctuated between 6 and 7.5, while the C:N ratio was between 10 and 13.

[0192] Samples of each test material were collected from an outdoor tumbler after 26 weeks. Surface residue was removed from the samples, they were dried, and weighed again. The presence of 2–5 wt% MgO or 2–5 wt% Mg(OH)2 increased decomposition, which was measured as weight loss in a household compost bin.

[0193] [Table 16]

[0194] Example 13 Collapse in industrial compost field trials Industrial composting field tests were conducted using a turned windrow system. Photographs of the test materials were taken, tagged, and placed in nylon mesh bags. Compost was filled into the mesh bags and placed in the windrow at the start of the composting activation phase. In the tests, the average C:N ratio of the starting materials was approximately 24. The average temperature in the windrow over the 90-day activation phase was approximately 71°C (160°F), and the moisture content varied between 50-60%. The piles were subjected to an additional 90-day maturation phase. After retrieving the test materials from the mesh bags, the percentage of disintegration was estimated from images of the partially disintegrated test materials.

[0195] [Table 17]

[0196] Example 14 Hydrated MgCO3, hydromagnesite, and basic magnesium carbonate as alkaline additives Hydromagnesite (hydrated MgCO3) was precipitated from a solution of its soluble salt. Precipitation was carried out at 90°C. The starting materials were USP-grade MgSO4·7H2O and food-grade sodium bicarbonate. For the precipitation reaction, a 0.5M Mg salt solution was heated to at least 70°C, then solid sodium bicarbonate was gradually added with stirring, and the reaction mixture was held overnight at 90°C. The resulting solid precipitate was washed with DI water until the TDS of the filtrate was measured to less than 120 ppm using a portable EC meter. The precipitate was dried to a fixed weight, and the aggregate was crushed by sieving. The reaction product was confirmed to be hydromagnesite by TGA and by the plate-like crystalline morphology using SEM. The molecular formula of hydromagnesite is 4MgCO3·Mg(OH)2·4H2O.

[0197] Basic magnesium carbonate (BMC320-FCC, Brenntag Specialty Ingredients) was estimated by TGA to have approximately three bound water molecules, suggesting an artiniite-like molecular formula of 4MgCO3·Mg(OH)2·3H2O.

[0198] The pH of 1% suspensions of different Mg-based alkaline minerals was estimated using colorimetric pH test strips, and the total evaporation residue (TDS) of the 1 wt% suspension was measured at 21°C using a portable electrical conductivity (EC) meter and reported in ppm.

[0199] [Table 18]

[0200] A dry blend of CA-398-30, 5 wt% MgCO3 (hydrate), and 15 wt% PEG400 was prepared by sieving the dry components together three times to disperse the mineral additives in the CA powder. Then, PEG400 was added, and the mixture was blended together with an electric grinder to disperse the plasticizer. Each dry blend was weighed into an aluminum pan and dried at 80°C for 24 hours. The upper and lower platens were preheated to 218°C (425°F) and the films (10 mil and 20 mil) were compressed for a total of 4 minutes in a heated press. All pre-dried CA / PEG400 / MgO / acid-dried blends were applied to the center of a 10.16 cm (4 inch) square, 10 mil thick frame between the upper and lower layers of aluminum foil, which were located between two steel plates. The assembly was placed in a press and heated at 0 pressure for 1 minute to dry and pre-melt the pack, then compressed at 12,000 PHI for 1 minute, increasing to higher pressure over approximately 30 seconds, and finally held at 20,000 PHI for 1.5 minutes (ram force in pounds).

[0201] The compressed compound was characterized for its appearance according to Example 4, and the results are summarized in Table 19 below.

[0202] [Table 19]

[0203] Example 15 Appearance of melt-processed compound of plasticized CA A formulation containing PEG400 as a plasticizer and 1 wt% to 5 wt% hydromagnesite as an alkaline additive was prepared, and a 30-mil film was extruded according to Example 2. The appearance of the 30-mil extruded film was characterized according to Example 4, and the results are summarized in Table 20.

[0204] [Table 20]

[0205] Example 16 Melt-processed articles of CAP containing alkaline additives Compression-molded CAP films: For control film samples without MgO, CE powder was used as is. For samples containing MgO, 95 g of Eastman CAP-485-20 powder was mixed with 5 g of MgO using a planetary mixer (Thinky mixer). The powder was then sieved to ensure that the mixture did not contain agglomerates. The powder was compressed into a 30 mil film using a compression molding machine. The CAP formulations with and without MgO were compressed at 232°C (450°F) for up to 4 minutes.

[0206] Example 17 Molten CAB articles containing alkaline additives Compression-molded CAB films: For control film samples without MgO, CE powder was used as is. For samples containing MgO, 95 g of Eastman CAB-381-2 powder was mixed with 5 g of MgO using a planetary mixer (Thinky mixer). The powder was then sieved to ensure that the mixture did not contain agglomerates. The powder was compressed into a 30 mil film using a compression molding machine. CAB formulations with and without MgO were compressed at 232°C (420°F) for up to 4 minutes.

[0207] Example 18 Investigation of metal oxides, hydroxides, and carbonates as alkaline additives Selected metal oxides, hydroxides, and carbonates were screened as alkaline additives to promote the degradation of CA films (Table 21). Films were cast from acetone-doped CA-394-60S containing 12 wt% PEG400 and the mineral combinations listed in Table 23. Environmental degradation of the films was estimated using the weight loss from the films after 12 weeks in deionized water at 50°C. Only ZnO, Mg(OH)2, and BMC were effective in increasing weight loss from the films when included as the sole additives. Only Mg(OH)2 and BMC were effective in increasing weight loss from the films when combined with 15 wt% CaCO3. The highest %wt loss in water at 50°C was measured when the film contained 15 wt% CaCO3 and 5 wt% MgO plus 5 wt% Mg(OH)2.

[0208] [Table 21]

[0209] [Table 22]

[0210] [Table 23]

[0211] Example 19 CaCO3 combined with MgO and / or Mg(OH)2 Films were cast from acetone-doped CA-394-60S containing 12 wt% PEG400 and the mineral combinations listed in Table 25. Weight loss from the film, a prediction of environmental degradation, was maximized with calcium carbonate (CaCO3) from multiple sources and combinations of 5 wt% MgO or 5 wt% MgO and 5 wt% Mg(OH)2. In contrast, film degradation, as measured by weight loss, was not improved by the inclusion of the neutral filler kaolin.

[0212] [Table 24-1]

[0213] [Table 24-2]

[0214] [Table 25]

[0215] Example 20 Change in the ratio of MgO to Mg(OH)2 in a mixture with CaCO3 Films were cast from acetone-doped CA-394-60S containing 12 wt% PEG400 and the mineral combinations listed in Table 26. The weight loss from the film after 12 weeks in deionized water at 50°C, which is a prediction of environmental degradation, is increased by combining the alkaline additive MgO and / or Mg(OH)2 with CaCO3.

[0216] [Table 26]

[0217] Example 21 Change in the ratio of MgO to Mg(OH)2 in a mixture with CaCO3 Films were cast from acetone-doped CA-394-60S containing 12 wt% PEG400 and the mineral combinations listed in Table 27. The weight loss from the film after 12 weeks in deionized water at 50°C, which is a prediction of environmental degradation, varied only slightly with different ratios of the alkaline additives MgO and Mg(OH)2 with CaCO3.

[0218] [Table 27]

[0219] Example 22 A preferred neutralizing agent is a heat-stable carboxylic acid. A dry blend was prepared for compression molding. First, CA398-30 and MgO (Marinco FCC) were pre-sieved separately to remove clumps, then combined in the required ratio (158g CA + 10g MgO) and sieved together three times to ensure thorough dispersion. To avoid variations in MgO content, this CA:MgO master blend was used for all subsequent blends. To incorporate acid, approximately 1 gram of solid was ground into a fine powder using a mortar and pestle. Each ground acid was pre-sieved separately, then 0.3 grams of acid was combined with the CA:MgO pre-blend and sieved together three times to disperse the acid. Finally, PEG400 was added to the powder, and the final blend was mixed in a coffee grinder to disperse the PEG400. Each fully dry blend was pre-weighed into aluminum pans (5.5g) and dried at 70°C for 16 hours. Each dry blend contained 79 wt% CA-398-30, 15 wt% PEG400, 5 wt% MgO, and 1 wt% acid (or none).

[0220] The film was compressed for a total of 4 minutes in a heated press with the upper and lower platens preheated to 218°C (425°F). The pre-dried CA / PEG400 / MgO / acid-dried blend was applied to the center of a 10.16 cm (4 inch) square, 10 mil thick frame between the upper and lower layers of aluminum foil, all between two steel plates. The assembly was placed in the press and heated at 0 pressure for 1 minute to dry and pre-melt the pack, then compressed at 12,000 PHI for 1 minute, increasing to higher pressure over approximately 30 seconds, and finally held at 20,000 PHI for 1.5 minutes (ram force in pounds).

[0221] Observation results regarding the appearance of compression molded films are included in Table 28. In thin films composed of CA, 15 wt% PEG400, and 5 wt% MgO molded at 425°F / 218°C, characteristic dark brown color and burnt odor are produced in the absence of neutralizing acid. When 1 wt% citric acid is included, the color is much brighter, but bubble-like defects appear, which are thought to be caused by water vapor formed during the thermal dehydration of citric acid. The citric acid used in the formulation is anhydrous. Other acids resulted in complex outcomes. Benzoic acid and aspartic acid were weak as neutralizing additives when combined with MgO within the compression molded film. The film formed a dark color during molding and produced a strong odor. In contrast, molded films with 1 wt% adipic acid or fumaric acid had a lighter color and no clear signs of thermal decomposition were observed.

[0222] [Table 28]

[0223] Disintegration in compost Example 23 Disintegration in a household compost bin Injection molded knives made from different formulations were added to a residential compost bin to monitor disintegration in household compost. The dimensions of the molded cutting tools that function as controls and test formulations of the present invention are detailed in Table 29.

[0224] [Table 29]

[0225] The compost bin is a 140 L black plastic household tumbler, initially filled with approximately 100 L of raw materials (70 L of mature compost, 24 L of pine shavings, 4 - 5 L of alfalfa pellets, 60% moisture). The initial C:N ratio is adjusted to >2 with alfalfa pellets and / or KNO₃. The side ventilation openings are fully opened. Raw materials are added to the empty bin. The starting raw material volume was approximately 100 L.

[0226] [Table 30]

[0227] Test materials were labeled with colored tape and added to a jar. The jar was rotated weekly, and a squeeze test was used to maintain moisture levels. At weeks 8, 14, 20, and 26, approximately 1 liter of alfalfa was added to the compost. Pine shavings were added to maintain the compost volume above the central axis. The collapse of materials in the home compost jar was monitored as weight loss from the dry material collected from the jar. After 26 weeks in the home compost jar, the final % weight loss was determined. Only materials with a combination of alkaline minerals CaCO3 and MgO reached the target of >90% weight loss after 26 weeks.

[0228] [Table 31]

[0229] Example 24 Collapse in accordance with ISO20200 at high temperatures The U.S. standard ASTM D6400, Standard Specification for Labeling of Plastics Designed to be Aerobically Composted in Municipal or Industrial Facilities (2021), stipulates that a minimum of 90% decomposition is required for certification.

[0230] The test specimen was a fork molded from a compound containing 66 wt% CA-394-60S, 12 wt% PEG400, 5 wt% MgO, 15 wt% CaCO3, and 1 wt% citric acid. The thickness of the test specimen varied from 1.5 mm at the tip of the handle to 3.7 mm at the thickest part of the handle. The test specimen was disintegrated in experimental compost according to ISO 20200. The synthetic compost contained rabbit feed, corn starch, sugar, corn oil, urea, sawdust, and wood chips. This raw material was seeded using mature compost from a local industrial composting facility. The initial C:N ratio of 30:1 was adjusted with urea, and water was added to adjust the moisture content to 55%. The test specimen (14.6 grams) was added to each reactor along with 1 kg of the synthetic compost mix. The reactor was run three times. The mixture was composted for 12 weeks, with the temperature controlled at 58°C + / - 2°C. The average percentage of disintegration across the three tanks was 99.4%.

[0231] Example 25 Degradation according to ISO20200 at ambient temperature The French standard specification NF T51-800, Plastics - Specifications for plastics suitable for home composting (2015), the Australian standard specification AS5810, Biodegradable plastics - Biodegradable plastics suitable for home composting (2010), and the TUV AUSTRIA Belgium OK Compost HOME certification scheme all state that, in quantitative tests conducted according to ISO20200 (2015) at ambient temperatures (20-30°C), if at least 90% of the test material was reduced to a size of less than 2 mm after 26 weeks of composting, the material showed sufficient decomposition for home composting.

[0232] A test formulation containing CA-394-60S (66 wt%), PEG400 (12 wt%), MgO (5 wt%), CaCO3 (15 wt%) and citric acid (1 wt%) was used to mold a fork having dimensions ranging from 0.84 mm at the thinnest part (center of the handle) to 1.89 mm at the thickest part (neck). The disintegration of the articles in home compost was tested in accordance with ISO 20200 "Plastics - Determination of the degree of disintegration of plastic materials under simulated composting conditions in a laboratory-scale test" (2015). The test was modified by incubating the test samples and compost at 28 °C ± 2 °C to simulate home composting conditions. The synthetic compost mixture contained 2 kg per reactor of a fraction of mature compost less than 10 mm plus freshly milled vegetable, garden and fruit waste. The disintegration of the articles was 90.1% after 26 weeks. The present invention includes the following embodiments. [1] An article comprising a melt-processable biodegradable cellulose ester composition, wherein the cellulose ester composition is A composition comprising at least one cellulose ester, at least one alkaline filler, and at least one neutralizing agent, wherein a 1% by weight suspension of the alkaline filler has a pH of 8 or higher, the water solubility of the alkaline filler at 20-25°C is greater than 1 ppm but less than 1,000 ppm, and the alkaline filler is present in an amount of about 0.1% to about 35% by weight based on the weight of the cellulose ester composition; or An article comprising at least one type of cellulose acetate, at least one type of plasticizer, at least one type of alkaline filler, and at least one type of neutralizing agent, wherein a 1% suspension of the alkaline filler has a pH of 8 or higher, the water solubility of the alkaline filler at 20-25°C is greater than 1 ppm but less than 1,000 ppm, and the alkaline filler is present in an amount of about 0.1% to about 35% by weight based on the weight of the cellulose ester composition. [2] The article according to [1], wherein the alkaline filler is present in an amount of about 0.1% to about 10% by weight, based on the weight of the cellulose ester composition. [3] The article according to [1] or [2], wherein the cellulose ester is cellulose acetate. [4] The article according to any one of [1] to [3], wherein the cellulose ester is prepared by converting cellulose to a cellulose ester with a reactant obtained from recycled material. [5] The plasticizers include glycerol triacetate (triacetin), glycerol diacetate, dibutyl terephthalate, dimethyl phthalate, diethyl phthalate, poly(ethylene glycol) MW200-600, triethylene glycol dipropionate, 1,2-epoxypropylphenylethylene glycol, 1,2-epoxypropyl(m-cresyl)ethylene glycol, 1,2-epoxypropyl(o-cresyl)ethylene glycol, β-oxyethylcyclohexene carboxylate, bis(cyclohexanate)diethylene glycol, triethyl citrate, polyethylene glycol, Benzoflex, propylene glycol, polysorbate, sucrose octaacetate, acetylated triethyl citrate, acetyl tributyl citrate, Admex, trippropionine, Scandiflex, poloxamer copolymer, polyethylene glycol succinate, and Aji. An article according to any one of [1] to [4], wherein the article is at least one selected from the group consisting of diisobutyl pitate, polyvinylpyrrolidone and glycol tribenzoate, triethyl citrate, acetyl triethyl citrate, polyethylene glycol, benzoate-containing plasticizers, e.g., the Benzoflex® plasticizer series, poly(alkyl succinates), e.g., poly(butyl succinates), polyethersulfone, adipate-based plasticizer, soybean oil epoxide, e.g., the Paraplex® plasticizer series, sucrose-based plasticizer, dibutyl sebacate, tributylin, tripionine, sucrose acetate isobutyrate, Resolflex® plasticizer series, triphenyl phosphate, glycolate, methoxypolyethylene glycol, 2,2,4-trimethylpentane-1,3-diyrbis(2-methylpropanoate), and polycaprolactone. [6] The article according to any one of [1] to [5], wherein the plasticizer is present in an amount of 1 to 40% by weight. [7] The article according to any one of [1] to [6], wherein the pH of a 1% by weight solution or suspension of the alkaline filler is in the range of about 8 to about 12. [8] The article according to any one of [1] to [7], wherein the water solubility of the alkaline filler at 20 to 25°C is approximately 2 ppm to approximately 400 ppm. [9] The article according to any one of [1] to [9], wherein the pH of a 1% by weight suspension of an alkaline filler is 8 or higher and the alkaline efficiency is at least 5.

[10] Alkaline fillers include calcium carbonate (CaCO3). 3 ), magnesium oxide (MgO), magnesium hydroxide (Mg(OH) 2 ), magnesium carbonate (MgCO3) 3 ), barium carbonate (BaCO2) 3 An article according to any one of [1] to [9], which is selected from the group consisting of ), and hydrated forms of these compounds.

[11] The article according to any one of [1] to

[10] , wherein the alkaline filler is a mixture of calcium carbonate and at least one of magnesium oxide, magnesium hydroxide, or magnesium carbonate, and based on the total weight of the cellulose ester composition, calcium carbonate is present in an amount of 5 to 25% by weight and at least one of magnesium oxide, magnesium hydroxide, or magnesium carbonate is present in an amount of 1 to 20% by weight.

[12] The article according to any one of [1] to

[11] , wherein the neutralizing agent is at least one selected from the group consisting of citric acid, malic acid, succinic acid, adipic acid, fumaric acid, formic acid, lactic acid, maleic acid, tartaric acid, malonic acid, glutamic acid, glutaric acid, gluconic acid, isophthalic acid, terephthalic acid, glycolic acid, itaconic acid, ferulic acid, mandelic acid, aconitic acid, benzoic acid, aspartic acid, and vanillic acid.

[13] An article according to any one of [1] to

[12] , wherein the neutralizing agent has a pKa of 4.5 or less and a boiling point or decomposition temperature of 170°C or higher.

[14] A melt-processable cellulose ester composition according to any one of [1] to

[13] , wherein the neutralizing agent is citric acid, adipic acid, or fumaric acid.

[15] The article according to any one of [1] to

[14] , wherein the cellulose ester composition contains a neutralizing agent in an amount of about 0.5% to about 5% by weight, based on the weight of the cellulose ester composition.

[16] Articles according to any one of [1] to

[15] , selected from the group consisting of biodegradable and / or compostable molded articles.

[17] Articles according to any one of [1] to

[16] , having a maximum thickness of up to 150 mils.

[18] Articles described in any of [1] to

[17] used in food service and food products, gardening, agriculture, recreation, coatings, textiles, nonwovens, and home / office use.

[19] An article as described in any of [1] to

[18] , wherein the maximum thickness of the article is 3.7 mm or less, and at least 90% of the article disintegrates in 90 days at 58°C in accordance with the standard ISO20200.

[20] An article according to any one of [1] to

[18] , wherein the maximum thickness of the article is 1.89 or less, and at least 90% of the article disintegrates in 90 days at a temperature of 20°C to 30°C in accordance with the standard ISO20200.

Claims

1. An article comprising a melt-processable biodegradable cellulose ester composition, wherein the cellulose ester composition is A composition comprising at least one cellulose ester, at least one alkaline filler, and at least one neutralizing agent, wherein a 1% by weight suspension of the alkaline filler has a pH of 8 or higher, the water solubility of the alkaline filler at 20-25°C is greater than 1 ppm but less than 1,000 ppm, and the alkaline filler is present in an amount of 6% to 35% by weight based on the weight of the cellulose ester composition; or The composition comprises at least one type of cellulose acetate, at least one type of plasticizer, at least one type of alkaline filler, and at least one type of neutralizing agent, wherein a 1% suspension of the alkaline filler has a pH of 8 or higher, the water solubility of the alkaline filler at 20-25°C is greater than 1 ppm but less than 1,000 ppm, and the alkaline filler is present in an amount of 6% to 35% by weight based on the weight of the cellulose ester composition. The alkaline filler is a mixture of calcium carbonate and at least one of magnesium oxide, magnesium hydroxide, or magnesium carbonate, wherein, based on the total weight of the cellulose ester composition, calcium carbonate is present in an amount of 5 to 25% by weight, and at least one of magnesium oxide, magnesium hydroxide, or magnesium carbonate is present in an amount of 1 to 20% by weight. An article wherein the neutralizing agent is at least one selected from the group consisting of citric acid, malic acid, succinic acid, adipic acid, fumaric acid, formic acid, lactic acid, maleic acid, tartaric acid, malonic acid, glutamic acid, glutaric acid, gluconic acid, isophthalic acid, terephthalic acid, glycolic acid, itaconic acid, ferulic acid, mandelic acid, aconitic acid, benzoic acid, aspartic acid, and vanillic acid.

2. An article comprising a melt-processable biodegradable cellulose ester composition, wherein the cellulose ester composition is: A composition comprising at least one cellulose ester, at least one alkaline filler, and at least one neutralizing agent, wherein a 1% by weight suspension of the alkaline filler has a pH of 8 or higher, the water solubility of the alkaline filler at 20-25°C is greater than 1 ppm but less than 1,000 ppm, and the alkaline filler is present in an amount of 6% to 35% by weight based on the weight of the cellulose ester composition; or The composition comprises at least one type of cellulose acetate, at least one type of plasticizer, at least one type of alkaline filler, and at least one type of neutralizing agent, wherein a 1% suspension of the alkaline filler has a pH of 8 or higher, the water solubility of the alkaline filler at 20-25°C is greater than 1 ppm but less than 1,000 ppm, and the alkaline filler is present in an amount of 6% to 35% by weight based on the weight of the cellulose ester composition. The alkaline filler is a mixture of calcium carbonate and at least one of magnesium oxide, magnesium hydroxide, or magnesium carbonate, wherein, based on the total weight of the cellulose ester composition, calcium carbonate is present in an amount of 5 to 25% by weight, and at least one of magnesium oxide, magnesium hydroxide, or magnesium carbonate is present in an amount of 1 to 20% by weight. An article having a neutralizing agent with a pKa of 4.5 or less and a boiling point or decomposition temperature of 170°C or higher.

3. An article comprising a melt-processable biodegradable cellulose ester composition, wherein the cellulose ester composition is: A composition comprising at least one cellulose ester, at least one alkaline filler, and at least one neutralizing agent, wherein a 1% by weight suspension of the alkaline filler has a pH of 8 or higher, the water solubility of the alkaline filler at 20-25°C is greater than 1 ppm but less than 1,000 ppm, and the alkaline filler is present in an amount of 6% to 35% by weight based on the weight of the cellulose ester composition; or The composition comprises at least one type of cellulose acetate, at least one type of plasticizer, at least one type of alkaline filler, and at least one type of neutralizing agent, wherein a 1% suspension of the alkaline filler has a pH of 8 or higher, the water solubility of the alkaline filler at 20-25°C is greater than 1 ppm but less than 1,000 ppm, and the alkaline filler is present in an amount of 6% to 35% by weight based on the weight of the cellulose ester composition. The alkaline filler is a mixture of calcium carbonate and at least one of magnesium oxide, magnesium hydroxide, or magnesium carbonate, wherein, based on the total weight of the cellulose ester composition, calcium carbonate is present in an amount of 5 to 25% by weight, and at least one of magnesium oxide, magnesium hydroxide, or magnesium carbonate is present in an amount of 1 to 20% by weight. An article in which a neutralizing agent is present in the cellulose ester composition at a concentration of 0.5% to 5% by weight, based on the weight of the cellulose ester composition.

4. The article according to any one of claims 1 to 3, wherein an alkaline filler is present in an amount of 6% to 10% by weight based on the weight of the cellulose ester composition.

5. The article according to any one of claims 1 to 3, wherein the cellulose ester is cellulose acetate.

6. The article according to any one of claims 1 to 3, wherein the cellulose ester is prepared by converting cellulose to a cellulose ester using a reactant obtained from recycled material.

7. The aforementioned plasticizers include glycerol triacetate (triacetin), glycerol diacetate, dibutyl terephthalate, dimethyl phthalate, diethyl phthalate, poly(ethylene glycol) MW200-600, triethylene glycol dipropionate, 1,2-epoxypropylphenylethylene glycol, 1,2-epoxypropyl (m-cresyl)ethylene glycol, 1,2-epoxypropyl (o-cresyl)ethylene glycol, β-oxyethylcyclohexene carboxylate, bis(cyclohexanate)diethylene glycol, triethyl citrate, polyethylene glycol, Benzoflex, propylene glycol, polysorbate, sucrose octaacetate, acetylated triethyl citrate, acetyl tributyl citrate, Admex, trippropionine, S The article according to any one of claims 1 to 3, wherein the material is at least one selected from the group consisting of candiflex, poloxamer copolymer, polyethylene glycol succinate, diisobutyl adipate, polyvinylpyrrolidone and glycol tribenzoate, triethyl citrate, acetyl triethyl citrate, polyethylene glycol, benzoate-containing plasticizer, poly(alkyl succinate), polyethersulfone, adipate-based plasticizer, soybean oil epoxide, sucrose-based plasticizer, dibutyl sebacate, tributylin, trippropionine, sucrose acetate isobutyrate, triphenyl phosphate, glycolate, methoxypolyethylene glycol, 2,2,4-trimethylpentane-1,3-diirbis(2-methylpropanoate), and polycaprolactone.

8. The article according to any one of claims 1 to 3, wherein the plasticizer is present in an amount of 1 to 40% by weight.

9. The article according to any one of claims 1 to 3, wherein the pH of a 1% by weight solution or suspension of the alkaline filler is in the range of 8 to 12.

10. The article according to any one of claims 1 to 3, wherein the water solubility of the alkaline filler at 20 to 25°C is 2 ppm to 400 ppm.

11. The article according to any one of claims 1 to 3, wherein the pH of a 1% by weight suspension of an alkaline filler is 8 or higher, and the alkaline efficiency is at least 5.

12. Alkaline fillers contain calcium carbonate (CaCO3). ３ ), magnesium oxide (MgO), magnesium hydroxide (Mg(OH) ２ ), magnesium carbonate (MgCO3) ３ ), barium carbonate (BaCO2) ３ The article according to any one of claims 1 to 3, which is at least one selected from the group consisting of ), and hydrated forms of these compounds.

13. The article according to claim 1, wherein the neutralizing agent is citric acid, adipic acid, or fumaric acid.

14. An article according to any one of claims 1 to 3, selected from the group consisting of biodegradable and / or compostable molded articles.

15. An article according to any one of claims 1 to 3, wherein the maximum thickness is up to 150 mils.

16. Articles according to any one of claims 1 to 3, used in food service and groceries, horticulture, agriculture, recreation, coatings, textiles, nonwovens, and home / office applications.

17. An article according to any one of claims 1 to 3, wherein the maximum thickness of the article is 3.7 mm or less, and at least 90% of the article disintegrates in 90 days at 58°C in accordance with the standard ISO 20200.

18. An article according to any one of claims 1 to 3, wherein the maximum thickness of the article is 1.89 mm or less, and at least 90% of the article decomposes in 90 days at a temperature of 20°C to 30°C in accordance with the standard ISO 20200.

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