Biodegradable ulva preparation, use and preparation thereof

Abstract

An ulva-based article (e.g., an ulva-based film, an ulva-based package, or the like) obtained by hot melt processing such as extrusion or hot press molding is provided. The ulva preparation is optionally characterized by a moisture content of between about 1 and about 25%. In addition, methods of making or shaping ulva-based articles from ulva extract by hot melt processing (e.g., extrusion, hot press molding, etc.

Description

[0001] Cross-reference to related applications This application claims priority to Israeli Patent Application No. 300493, filed on February 7, 2023, entitled “BIODEGRADABLE ULVAN ARTICLES, USES AND PREPARATION THEREOF”, the entire contents of which are incorporated herein by reference. Technical Field

[0002] Generally speaking, the present invention relates to the field of polymer hydrogels and articles comprising polymer hydrogels. Background Technology

[0003] The plastics industry generates a massive amount of plastic waste, especially from packaging. More than 8 million tons of plastic waste end up in the ocean each year, causing global environmental pollution and damaging ecosystems. Furthermore, since petrochemical-based plastics are primarily used for food packaging, it is necessary to reduce the use of these products by adopting new raw materials with similar properties to plastics but which are biodegradable and harmless.

[0004] Therefore, there is an urgent need for alternative sources of packaging materials. Ulva, a green seaweed, also known as sea lettuce, can achieve high productivity and growth rates under a variety of geographical and climatic conditions, and it does not require chemical fertilizers, pesticides, or farmland, which increases its potential for large-scale production. The main bioproduct produced from Ulva is ulvanan, a sulfated polysaccharide.

[0005] Ulva polysaccharide is a polysaccharide found in the cell wall and accounts for 9-36% of the dry weight of Ulva. It is mainly composed of uronic acids such as sulfated rhamnose (45.0 mol%), glucuronic acid (22.5 mol%), and iduronic acid (22.5 mol%), as well as xylose (9.6 mol%).

[0006] Ulva polysaccharide products are non-toxic and environmentally friendly. Furthermore, ulva polysaccharide has been reported to possess antioxidant activity, which may be important for food packaging. However, to date, there is no industrially applicable method for processing unpurified ulva polysaccharide that reduces production costs. Therefore, there is an urgent need to develop industrially available methods for processing ulva polysaccharide to obtain shaped ulva polysaccharide products as an alternative source of packaging materials. Summary of the Invention

[0007] The following embodiments and aspects thereof are described and illustrated in conjunction with systems, tools and methods, which are intended to be exemplary and illustrative, and not to limit the scope.

[0008] In one aspect of the invention, a ulva polysaccharide product is provided, wherein the ulva polysaccharide product is characterized by a water content between about 1% and about 25%; and wherein the ulva polysaccharide product is obtained by hot melt processing.

[0009] In one embodiment, the ursanthemum polysaccharide product further includes a plasticizer.

[0010] In another aspect of the invention, a ulva-based product is provided, which is a composite comprising ulva-based material and a plasticizer; wherein the w / w concentration of the plasticizer in the ulva-based product is between 0.5% and 30%, and wherein the ulva-based product is obtained by hot melt processing.

[0011] In one embodiment, the plasticizer includes a water-soluble polymer, a glycol, a triol, a monosaccharide, a disaccharide, or any combination thereof.

[0012] In one implementation, the plasticizer is glycerin.

[0013] In one embodiment, the ulva in the ulva product is a non-crosslinked ulva; and the ulva product is substantially free of crosslinking agents.

[0014] In one embodiment, the ulva polysaccharide product is flowable at a temperature between 89°C and 120°C and a pressure of 1 bar.

[0015] In one embodiment, the ulva polysaccharide product is in the form of a film, characterized by at least one of the following: strain under maximum load is higher than 25%; and stress under maximum load is higher than 12 MPa.

[0016] In another aspect of the invention, a ulva-based product is provided, wherein the ulva is a cross-linked ulva, wherein the w / w concentration of the cross-linking agent in the cross-linked ulva is between 5% and 25%; and wherein the ulva-based product is obtained by hot melt processing.

[0017] In one embodiment, the crosslinking agent is a multifunctional covalent crosslinking agent.

[0018] In one embodiment, the multifunctional covalent crosslinking agent is a dicyclooxyalkylene oxide.

[0019] In one embodiment, the w / w percentage of ulva in the ulva product is between 60% and 98% based on the dry weight of the ulva product.

[0020] In one embodiment, the ulva polysaccharide product is compostable, biodegradable, biodegradable, or any combination thereof.

[0021] In one embodiment, the ulva polysaccharide article is in the form of a film, sheet, tape, mesh, nonwoven material, granules, or a container comprising any combination thereof.

[0022] In one embodiment, the ulva polysaccharide article is (i) a thermoformed article, wherein the thermoforming is carried out at a temperature between 89°C and 120°C; or (ii) an extruded article, wherein the extrusion is carried out at a temperature between 79°C and 85°C.

[0023] In another aspect of the invention, a method for manufacturing the ulva polysaccharide article of the invention is provided, comprising contacting ulva polysaccharide with water under suitable conditions to obtain a hydrated powder; and shaping the hydrated powder under conditions suitable for hot-melt processing; wherein the hydrated powder is flowable under conditions suitable for hot-melt processing; and wherein the proportion of water in the hydrated powder is between 20% w / w and 60% w / w.

[0024] In one embodiment, contact includes mixing; and suitable conditions include a temperature between 30°C and 70°C and a time period between 1 minute and 10 hours.

[0025] In one embodiment, uranyl polysaccharide is the dry matter of an aqueous extract of an algae species of the genus Ulva; and wherein the aqueous extract is a whole plant extract.

[0026] In one embodiment, the whole plant extract comprises chlorophyll and is characterized by a first UV peak having a maximum value at a wavelength between 400 nm and 440 nm, and a second UV peak having a maximum value at a wavelength between 640 nm and 680 nm.

[0027] In one embodiment, the contact further includes the addition of a plasticizer.

[0028] In one embodiment, the concentration of plasticizer in the hydrated powder is between about 5% w / v and about 20% w / v.

[0029] In one embodiment, hot melt processing includes any injection molding, hot blown film molding, hot pressing, or any combination thereof; and the conditions suitable for hot melt processing include temperatures between about 89°C and about 120°C.

[0030] In one embodiment, suitable conditions for hot melt processing include temperatures between about 90°C and about 95°C.

[0031] In one embodiment, hot melt processing is extrusion; wherein the forming step includes feeding a plurality of granules into an extruder; and wherein suitable conditions for hot melt processing include a temperature between 78°C and 85°C.

[0032] In another aspect of the invention, a method for manufacturing the ulva-based product of the invention is provided, the method comprising contacting non-crosslinked ulva with water at a water:ulva ratio between 1:5 and 1:2, and contacting it with a crosslinking agent under conditions suitable for crosslinking, thereby obtaining crosslinked ulva; adding an amount of polar organic solvent sufficient to precipitate the crosslinked ulva, thereby obtaining a plurality of particles; and providing the plurality of particles under conditions suitable for hot-melt processing, thereby obtaining the product.

[0033] In one embodiment, the method further includes separating multiple particles.

[0034] In one embodiment, suitable conditions for crosslinking include a crosslinking agent concentration ranging from about 3% w / v to about 20% w / v, and optionally include any of the following: a pH value of the hydrated powder between 8 and 14; and a temperature between 30°C and 70°C.

[0035] In one embodiment, the cross-linked ulnar polysaccharide is characterized by a degree of cross-linking between 5% and 25%.

[0036] In one embodiment, the method further includes a preparatory step of processing Ulva biomass to obtain Ulva polysaccharide.

[0037] In one embodiment, the processing includes water extraction of Ulva prostrata biomass to obtain a whole plant extract, and drying the whole plant extract to obtain dry matter.

[0038] In one embodiment, the *Ulva* biomass comprises algal species of the genus *Ulva*. In one embodiment, water extraction further comprises any of the following: sedimentation, precipitation, or any other technique suitable for inducing sedimentation or phase separation to obtain a solid sediment and an aqueous composition containing a water-soluble or water-dispersible fraction derived from the *Ulva* biomass. In one embodiment, water extraction further comprises separating the water-soluble or water-dispersible fraction from the solid sediment. In one embodiment, separation is performed by any of the following: filtration, decantation, centrifugation, or any combination thereof.

[0039] In one embodiment, the dry matter is partially purified uranium that further contains chlorophyll.

[0040] In one embodiment, hot melt processing includes any one of extrusion, injection, hot blown film, molding, or any combination thereof.

[0041] In one embodiment, hot melt processing is extrusion; wherein the provided steps include feeding a plurality of granules into an extruder; and wherein suitable conditions for hot melt processing include a temperature between 78°C and 85°C.

[0042] In one aspect, there is a Ulva polysaccharide product, wherein the Ulva polysaccharide product is characterized by a water content between about 1% and about 25%; and wherein the Ulva polysaccharide product is obtained by hot melt processing.

[0043] In some embodiments, the ulva polysaccharide product further includes a plasticizer.

[0044] In some embodiments, the ulva in the ulva product is cross-linked ulva.

[0045] In another aspect, there is a Ulva propolis product that is a complex comprising Ulva propolis and a plasticizer; wherein the w / w concentration of the plasticizer in the Ulva propolis product is between 0.5% and 30%, and wherein the Ulva propolis product is obtained by hot melt processing.

[0046] In some embodiments, the plasticizer includes water-soluble polymers, glycols, triols, monosaccharides, disaccharides, and any combination thereof.

[0047] In some implementations, the plasticizer is glycerin.

[0048] In another aspect, there is a ulva product in which the ulva is a cross-linked ulva, wherein the w / w concentration of the cross-linking agent in the cross-linked ulva is between 5% and 25%; and wherein the ulva product is obtained by hot melting.

[0049] In some implementations, the crosslinking agent is a multifunctional covalent crosslinking agent.

[0050] In some embodiments, the multifunctional covalent crosslinking agent is a dicyclooxyalkylene oxide.

[0051] In some embodiments, the w / w percentage of ulva in the ulva product is between 60% and 98%.

[0052] In some embodiments, the ulva polysaccharide products of the present invention are degradable or biodegradable.

[0053] In some embodiments, the ulva polysaccharide articles of the present invention are in the form of films, sheets, tapes, nets, nonwoven materials, or containers comprising any combination thereof.

[0054] In some embodiments, the ulva polysaccharide products of the present invention are formed by pressure molding or extrusion molding.

[0055] In another aspect, the method of manufacturing a ulva-based product according to the present invention includes contacting ulva with water under suitable conditions to obtain a hydrated powder; and shaping the hydrated powder under conditions suitable for hot-melt processing; wherein the hydrated powder is flowable under conditions suitable for hot-melt processing; and wherein the proportion of water in the hydrated powder is between 20% w / w and 60% w / w.

[0056] In some implementations, suitable conditions include a temperature between 30°C and 70°C, and optionally a time period from 1 minute to 10 hours.

[0057] In some implementations, contact is achieved through mixing.

[0058] In some implementations, the contact further includes the addition of a plasticizer.

[0059] In some embodiments, the concentration of plasticizer in the hydrated powder is between about 5% w / v and about 20% w / v.

[0060] In some implementations, suitable conditions for hot melt processing include temperatures between about 85°C and about 95°C.

[0061] In some embodiments, the method includes: contacting non-crosslinked ulva with water at a water:ulva ratio of 1:5 to 1:2, and contacting it with a crosslinking agent under conditions suitable for crosslinking, thereby obtaining crosslinked ulva; adding an amount of polar organic solvent sufficient to precipitate the crosslinked ulva, thereby obtaining a plurality of particles; and providing the plurality of particles under conditions suitable for hot melt processing, thereby obtaining an article.

[0062] In some implementations, the method further includes separating multiple particles.

[0063] In some embodiments, suitable conditions for crosslinking include a crosslinking agent concentration ranging from about 3% w / v to about 20% w / v, and optionally include any of the following: a pH value of the hydrated powder between 8 and 14; and a temperature between 30°C and 70°C.

[0064] In some embodiments, the cross-linked ulnar polysaccharide is characterized by a degree of cross-linking between 5% and 25%.

[0065] In some embodiments, hot melt processing includes extrusion, injection molding, hot blown film molding, molding, or any combination thereof.

[0066] In some embodiments, the method further includes a preparatory step of processing Ulva biomass to obtain Ulva polysaccharide.

[0067] In some embodiments, the uranium is a partially purified uranium.

[0068] In addition to the exemplary aspects and implementations described above, further aspects and implementations will become apparent from the following detailed description.

[0069] Unless otherwise defined, all technical and / or scientific terms used herein have the same meaning as commonly understood by one of ordinary skill in the art to which this invention pertains. While similar or equivalent methods and materials may be used in the practice or testing of embodiments of the invention, exemplary methods and / or materials are described below. In case of conflict, the patent specification (including definitions) shall prevail. Furthermore, materials, methods, and examples are illustrative only and are not necessarily intended to be limiting.

[0070] Further embodiments and the full scope of the invention will become apparent from the specific embodiments described below. However, it should be understood that while indicating preferred embodiments of the invention, the specific embodiments and examples are given only by way of description, because, based on these specific embodiments, those skilled in the art will understand various changes and modifications within the spirit and scope of the invention. Detailed Implementation

[0071] According to one aspect, a Ulva propolis article is provided, wherein the Ulva propolis article is manufactured (or shaped) by a hot melt process, and wherein the Ulva propolis article is characterized by a water content between 1% and 25%, 2% and 15%, 2% and 5%, 6% and 15%, 3% and 5%, 6% and 13%, 10% and 15%, 10% and 13%, 10% and 25%, 15% and 25% w / w, and any range therein.

[0072] In some embodiments, the Ulva polysaccharide product is characterized by a water content between 1% and 7%, 2% and 4%, 2% and 7%, 2% and 5%, 2% and 6%, 2.5% and 3%, 3% and 3.5% and 3.5% w / w, and any range therein.

[0073] In some embodiments, the Ulva polysaccharide product is an extruded product characterized by a substantially unidirectional orientation. In some embodiments, the extruded product is characterized by the unidirectional orientation of the polysaccharide molecules. The unidirectional orientation of the polymer in the extruded product can be observed using an electron microscope.

[0074] In some embodiments, the extruded article is characterized by a unidirectional orientation of at least 50%, at least 70%, at least 80%, or between 50% and 90%, or between 50% and 100% of the entire polysaccharide molecule, including any range therein.

[0075] In some embodiments, the extruded article is characterized by orientation (or directionality) in one direction (e.g., the extrusion direction). In some embodiments, the ulva-based article is characterized by non-uniform tensile strength along its longitudinal and transverse axes. In some embodiments, the ulva-based article is characterized by a first tensile strength along the extrusion direction and a second tensile strength along a second direction. In some embodiments, the first tensile strength is substantially greater than the second tensile strength (e.g., 20%, 50%, or more).

[0076] In some embodiments, the extruded article is characterized by a water content between 1% and 25%, 2% and 15%, 2% and 5%, 6% and 15%, 3% and 5%, 6% and 13%, 10% and 15%, 10% and 13%, 10% and 25%, 15% and 25% w / w, 1% and 10%, 1% and 7%, 2% and 4%, 2% and 7%, 2% and 5%, 2% and 6%, 2.5% and 3%, 3% and 3.5% and 3.5% and 4% w / w, and any range therein.

[0077] In some implementations, water binds to uranium through physical interactions (e.g., hydrogen bonds, dipole-dipole interactions, electrostatic interactions, etc.).

[0078] In some embodiments, the Ulva protopanax product is primarily composed of Ulva protopanax and water, wherein the water content is as described above. In some embodiments, the Ulva protopanax product is primarily composed of Ulva protopanax, water, and optionally at least one of a plasticizer and a crosslinking agent; wherein the water content is as described above. In some embodiments, the Ulva protopanax in the Ulva protopanax product is crosslinked Ulva protopanax or substantially non-crosslinked Ulva protopanax.

[0079] The term “uranium polysaccharide” includes one or more naturally occurring sulfated polysaccharides derived from natural products, i.e., algal biomass, which includes or is mainly composed of at least one species of Ulva algae (e.g., U. arasakii, U. armoricana, U. clathrata, U. compressa, U. conglobate, U. fasciata, U. flexusa, U. gigantea, U. intestinalis and / or U. lactuca).

[0080] The term "ulnaranone" further includes an aqueous extract of Ulva biomass, which comprises or is primarily composed of natural sulfated polysaccharides. In some embodiments, the aqueous extract is a whole-plant extract. In some embodiments, the aqueous extract is a dry matter obtained by substantially removing water (drying) from the aqueous extract (e.g., a whole-plant aqueous extract). In some embodiments, ulnaranone is obtained by filtering and subsequently drying a whole-plant aqueous extract of Ulva biomass. The terms "ulnaranone" and "partially purified ulnaranone" are used interchangeably herein.

[0081] In some embodiments, as disclosed below, ulva polysaccharide is primarily composed of natural sulfated polysaccharides and one or more impurities. In some embodiments, the w / w content of the natural sulfated polysaccharides (including any salts thereof) in the ulva polysaccharide is between 99.5% and 80%, 99% and 80%, 98% and 80%, 95% and 80%, 92% and 80%, or any range therein.

[0082] In some embodiments, Ulva protopanax comprises one or more sulfated polysaccharide species. In some embodiments, the one or more sulfated polysaccharide species are characterized by an average molecular weight (Mw) between 10 and 2000 kDa, 50 and 2000 kDa, 50 and 500 kDa, 100 and 2000 kDa, and 150 and 2000 kDa, in any range therebetween, and are further characterized by a degree of sulfatedness between 1 and 40%, 5 and 40%, and 10 and 35%, in any range therebetween.

[0083] In some embodiments, the sulfated polysaccharide species in the Ulva polysaccharide of the present invention are characterized by an average molecular weight (Mw) between 300 and 350 kDa, or between 310 and 340 kDa, and by Mn between 80 and 150 kDa, or between 90 and 120 kDa.

[0084] The backbone of sulfated polysaccharides consists of repeating units selected from rhamnose, glucuronic acid, xylose, and iduronic acid, wherein any repeating unit is optionally coated with sulfate (SO4). 2- Instead of the hydroxyl groups in unmodified sugars, sulfated polysaccharides may have the following types: A 3s B 3s U 3s and U 2’s、3s .

[0085] In some embodiments, the term "derived from" includes any industrial processing, such as extraction, purification, separation, fractionation, chemical modification, etc. In some embodiments, the partially purified ulva polysaccharide is further composed of impurities (i.e., impurities that are not ulva polysaccharide), wherein the w / w concentration of the impurities in the partially purified ulva polysaccharide is up to 20%, up to 15%, up to 10%, up to 5%, up to 1%, and between 0 and 20%, 0 and 5%, 5 and 10%, 5 and 15%, 5 and 20%, 10 and 20%, 15 and 20%, or any range therein.

[0086] In some embodiments, the impurities include any of the following: polysaccharides (e.g., water-insoluble fiber, cellulose, xyloglucan, glucuronan), fatty acids (and / or their esters), lipids, salts, pigments (e.g., chlorophyll, carotenoids), and polynucleotides.

[0087] In some embodiments, the impurities include one or more chlorophyll species (e.g., natural chlorophyll such as chlorophyll a, chlorophyll b, chlorophyll c, chlorophyll d, and / or chlorophyll f). In some embodiments, the w / w concentration of one or more chlorophyll species in the partially purified ulva polysaccharide is up to 0.5%, up to 1%, up to 3%, up to 5%, and between 0.05% and 5%, 0.1% and 5%, 0.05% and 1%, 0.1% and 1%, 0.1% and 2%, 1% and 3%, 0.1% and 5%, and any range therein. In some embodiments, the impurities are protein-free (e.g., determined by Coomassie staining assay).

[0088] In some embodiments, the partially purified ulva polysaccharide of the present invention is characterized by a UV absorbance profile indicating one or more chlorophyll species. In some embodiments, the partially purified ulva polysaccharide of the present invention is characterized by a first UV peak having a maximum value at a wavelength between 400 and 440 nm or between 410 and 430 nm; and a second UV peak having a maximum value at a wavelength between 640 and 680 nm or between 650 and 670 nm.

[0089] In some embodiments, the partially purified ulva mannan of the present invention is characterized by a chemical purity of up to 95%, up to 90%, up to 88%, up to 85%, up to 80%, up to 70%, up to 60%, up to 50%, between 60 and 95%, between 60 and 90%, between 60 and 85%, between 70 and 90%, between 70 and 85%, between 70 and 80%, and any value in between. The term "chemical purity" refers to the dry weight content of SP (ulva mannan SP) in the partially purified ulva mannan.

[0090] In some embodiments, the Ulva protopanax product does not contain additional polymers, such as additional polysaccharides—which are not Ulva protopanax. In some embodiments, the Ulva protopanax product does not contain synthetic polymers. In some embodiments, the Ulva protopanax product does not contain additional natural polymers or polymers derived therefrom. In some embodiments, Ulva protopanax is the only polysaccharide present in the Ulva protopanax product. In some embodiments, the Ulva protopanax product does not contain particulate matter. In some embodiments, the Ulva protopanax product does not contain crosslinking agents (e.g., boric acid, polycationic crosslinking agents, etc.).

[0091] In some embodiments, the Ulva protopanax article is in a solid state. The term "solid" or "solid" includes a non-flowable material / article that retains at least 90%, at least 95%, at least 97%, or between 80% and 100%, 85% and 100%, 90% and 100%, 90% and 100%, 90% and 97% or 85% of its original shape within any temperature range up to 85°C, up to 86°C, up to 87°C, up to 88°C, up to 88°C, up to 89°C, or between 85% and 89°C, and in any range thereof. The term "original shape" refers to at least one dimension (e.g., width, length, cross-section, height, or overall shape of the article) measured at a temperature of 25°C.

[0092] In some embodiments, the ulva in the ulva product is in the form of a hydrogel. The term "hydrogel" refers to a semi-solid (non-flowing substance) comprising a supramolecular structure of self-assembled polymer molecules (i.e., sulfated polysaccharides) and water. In some embodiments, the supramolecular structure is in the form of a three-dimensional network of polymer molecules. In some embodiments, the polymer molecules are uniformly distributed (e.g., dispersed) within the hydrogel, and there are substantially no aggregates and / or precipitation. In some embodiments, the hydrogel is in the form of a polymer matrix (i.e., a matrix formed of polysaccharide chains) stably bound to water molecules.

[0093] In some embodiments, the hydrogel is essentially composed of ulva polysaccharide and water, wherein the w / w ratio of ulva polysaccharide to water is between 10:1 and 100:1, between 10:1 and 20:1, between 10.1 and 40:1, between 10:1 and 60:1, between 10:1 and 80:1, and between 80:1 and 100:1, including any range therebetween. In some embodiments, the hydrogel is essentially composed of sulfated polysaccharide (SP) and water, wherein the w / w ratio of SP to water is between 10:1 and 100:1, between 10:1 and 20:1, between 10:1 and 40:1, between 10:1 and 60:1, between 10.1 and 80:1, and between 80:1 and 100:1, including any range therebetween.

[0094] In some embodiments, the articles of the present invention are substantially biocompatible or biodegradable, and / or biocorrosive. In some embodiments, the term "biodegradable" describes a substance that can decompose into its decomposition products under environmental conditions. In some embodiments, the term "biodegradable" as used in the context of embodiments of the present invention also includes the term "biocorrosive," which describes a material / composition / article that decomposes under environmental conditions. Such environmental conditions include, for example, exposure to moisture, hydrolytic enzyme activity, microorganisms, or any combination thereof; wherein exposure includes temperatures of 10 to 40°C in a moist environment (such as soil and / or compost), wherein the moisture content of the moist environment is at least 5%, at least 10%, at least 20%, at least 50%, or between 5 and 60%, between 5 and 50%, between 10 and 50%, and any range therein. In some embodiments, the term "soil" includes any naturally occurring soil type (e.g., loam, coarse sand, fine sand, sandy loam, sandy loam, sandy clay loam, silty loam, clay loam, silty clay loam, clay, peat, etc.). Soil includes soil microbiome and various chemically active molecules such as enzymes, which can induce or enhance the degradation of the articles of the present invention.

[0095] As used herein, the term "soil microbiome" refers to microorganisms living in a specific environment, including microorganisms living in the soil surrounding plant roots and / or interacting with plant roots. Optionally, the term "soil microbiome" refers to microorganisms located in the rhizosphere. Microorganisms include bacteria, archaea, fungi, or combinations thereof.

[0096] The term "compost" refers to any compost known to those skilled in the art. In some embodiments, compost refers to any organic material that undergoes aerobic degradation. In some embodiments, compost is the result of Grub composting. In another embodiment, compost is Bokashi compost. In another embodiment, compost includes EM1 (lactic acid bacteria, yeast, and photosynthetic (PNSB) bacteria). In another embodiment, compost is Hügelkultur (a type of compost). In another embodiment, compost includes human excrement compost. In yet another embodiment, compost is vermicompost (a type of earthworm compost).

[0097] The term "biodegradable" refers to a material that degrades, decomposes, or is subjected to erosion under environmental conditions within any timeframe, including but not limited to 2 years (y), 1 year, 0.5 years, or 1 month. The term "decomposition," including any of its grammatical derivatives, encompasses (i) the physical breakdown of a material (or article) into smaller parts, resulting in a substantial loss of its structure and / or mechanical properties; and (ii) chemical decomposition, including a reduction in mass, volume, or both, due to the chemical conversion of the material into gases (e.g., CO2, N2, O2, NOx, SO2, etc.) and / or water. The term "biodegradable" further includes the breakdown of a material / article into compounds that can be metabolized or digested by microorganisms (e.g., soil and / or aquatic microorganisms).

[0098] The term “decomposition”, including any of its grammatical derivatives, refers to the breakdown of a material (or article) by at least 80%, at least 90%, at least 95%, at least 97%, or between 80 and 99% of its initial weight and / or volume.

[0099] In some embodiments, the terms "biodegradable" and "compostable" are used interchangeably herein. Biodegradable materials according to some embodiments of the invention conform to one or more of the following standards: EN13432, D6400, D5338, D6691, or any other suitable standard.

[0100] In some embodiments, the ulva polysaccharide product further includes a plasticizer. In some embodiments, the plasticizer is selected from polyols, monosaccharides, disaccharides, and oligosaccharides (e.g., PEG 200, glycerol, sorbitol, and sucrose), including any salts and copolymers thereof.

[0101] In some embodiments, the plasticizer is a small molecule or a salt thereof. The term "small molecule" refers to a molecule that is up to 1 kDa, or up to 500 Da, or between 50 and 500 Da, between 60 and 300 Da, or between 50 and 200 Da, including any range therein.

[0102] In some embodiments, the plasticizer is a water-soluble polymer or copolymer. In some embodiments, the plasticizer is compatible with a flowable ulva-based composition, wherein the flowable composition is as described herein. In some embodiments, the plasticizer is configured to lower the melt temperature of the ulva-based composition. In some embodiments, the plasticizer is configured to provide sufficient elasticity to the ulva-based articles of the present invention. In some embodiments, the plasticizer is glycerol.

[0103] In some embodiments, the ulva polysaccharide product is a thermoplastic material. In some embodiments, the ulva polysaccharide product is suitable for hot-melt processing, i.e., it does not decompose within any range of hot-melt processing temperatures, including 89 to 120°C, 89 to 110°C, 89 to 100°C, 90 to 120°C, 90 to 110°C, 88 to 120°C, and 87 to 120°C.

[0104] In some embodiments, the ulva in the ulva product is a cross-linked ulva comprising cross-linked SP molecules.

[0105] In some embodiments, the ulva polysaccharide content of the ulva polysaccharide product of the present invention is between 60% and 100%, 60% and 70%, 70% and 80%, 80% and 90%, 90% and 100%, 85% and 90%, and 90% and 95%, including any range therebetween. In some embodiments, the ulva polysaccharide content of the ulva polysaccharide product of the present invention is between 99% and 70% w / w, 99% and 80% w / w, and 99% and 90% w / w, including any range therebetween.

[0106] In some embodiments, the Ulva protopanax product further includes an active agent. In some embodiments, the w / w concentration of the active agent in the Ulva protopanax product is between 0.01 and 20%, 0.01 and 10%, 0.01 and 5%, 0.01 and 10%, 0.1 and 20%, 0.1 and 10%, 1 and 5%, 5 and 20%, 5 and 10%, 10 and 20%, 0.01% and 1%, 10 and 20% w / w, and any range or value therein.

[0107] In some embodiments, the activator binds to and / or incorporates into ursulphur sugar through physical interactions.

[0108] In some embodiments, the active agent is a pharmaceutical, pesticide (e.g., biocide, pesticide, insecticide, fungicide, etc.), or both. In some embodiments, the active agent is a small molecule.

[0109] In some embodiments, the active agent is a volatile compound. Various volatile compounds having high vapor pressures under ambient conditions and at temperatures between 20 and 30°C are well known in the art.

[0110] In some embodiments, the active agent has antibacterial activity (e.g., biocide), phytostimulatory activity (e.g., plant hormone, fertilizer, etc.), pest control activity (e.g., pesticide, fungicide, herbicide, insecticide) or any combination thereof. In some embodiments, the active agent includes hydrogen peroxide (HP), urea, HP precursors (e.g., urea hydrogen peroxide adduct, percarbonate, etc.), hypochlorite, hypobromite, trisodium phosphate-Cl (TSP-Cl), metal ions, ammonium phosphite, methyl orange, cibacron blue, trichloroacetic acid, dichloroacetic acid, monochloroacetic acid, trifluoroacetic acid, and / or water-insoluble substances, such as plant hormones, essential oils like thymol, pheromones like dodecylaldehyde or dodecyl alcohol, pesticides like fluazinam, benzoyl peroxide, or biological pest control agents, antibacterial metal ions, or any one of chlorine (Cl), bromine (Br), and iodine (I) in elemental or halide salt or halide ion form, or any combination thereof.

[0111] In some embodiments, the hydrogen peroxide source is selected from liquid hydrogen peroxide sources (i.e., aqueous solutions of hydrogen peroxide) and solid hydrogen peroxide sources (i.e., solid compounds that release hydrogen peroxide upon heating or exposure to water). Examples of solid hydrogen peroxide sources are, for example, hydrogen peroxide bound to chemical compounds (e.g., solid compounds of hydrogen peroxide bound to polyvinylpyrrolidone (PVP)) and compounds with the potential to generate hydrogen peroxide—e.g., through reaction with water, such as perborates (e.g., sodium perborate), percarbonates (e.g., sodium percarbonate), peroxyphosphates (e.g., sodium peroxyphosphate), sodium persulfate (e.g., potassium persulfate), peroxymonosulfate, peroxydisulfate, urea peroxide, etc. It should be understood that the hydrogen peroxide source referred to herein may consist of one or more source types, or may consist of a solid source in combination with a liquid hydrogen peroxide source. In some embodiments, the hydrogen peroxide source is selected from sodium peroxide, calcium peroxide, sodium percarbonate, sodium periodate, sodium persulfate, ammonium persulfate, sodium perborate, silver(II) oxide, chlorine dioxide, benzoyl peroxide, ketone peroxide, peroxydicarbonate, peroxide ester, dialkyl peroxide, hydroperoxide, peroxyketal, or any combination thereof.

[0112] In some embodiments, the active agent (e.g., a biocide) includes percarboxylic acids (e.g., peracetic acid, peroctanoic acid, perlactic acid, perpropionic acid, percitric acid and persalicylic acid, performic acid, including any mixture or derivative thereof), hydrogen peroxide, urea peroxide, sodium peroxide, calcium peroxide, silver, silver salts and hydrogen peroxide (HP), sodium percarbonate, sodium periodate, sodium persulfate, ammonium persulfate, perchloric acid, sodium perborate, silver oxide (II), chlorine dioxide, benzoyl peroxide, ketone peroxide, peroxydicarbonate, peroxyester, dialkyl peroxide, hydroperoxide and peroxyketal or any combination or salt thereof.

[0113] As used herein, the term "essential oil (EO)" refers to a product obtained from a natural source of plant origin by steam distillation, mechanical processing of the outer peel of citrus fruits, or dry distillation—after physical processing to separate the aqueous phase (if any). EOs are known and documented in the art and will be apparent to those skilled in the art. The essential oil applicable according to the invention is any essential oil characterized by biocidal activity against microorganisms such as bacteria, yeasts, and / or molds. In some embodiments, the essential oil is selected from thymol, limonene, cinnamon oil, oregano oil, sage oil, tea tree oil, carvacrol oil, or any combination thereof. In some embodiments, the metal ion is any antibacterial metal ion.

[0114] In some embodiments, the metal ion is any biocidal metal ion. As used herein, "biocidal metal ion" refers to a metal ion characterized by biocidal activity. In some embodiments, the metal ion is selected from Zn. 2+ Cu 2+ or Ag + .

[0115] In some embodiments, "biocide" refers to a combination of two or more biocides. In some embodiments, a biocide refers to a combination of two biocides. In some embodiments, the coating includes two or more biocides.

[0116] In some embodiments, the ulva polysaccharide product further includes one or more additives (e.g., colorants, UV blockers, stabilizers, antioxidants, preservatives, etc.).

[0117] In some embodiments, surfactants and / or additives are incorporated into the Ulva protoplasm article. In some embodiments, surfactants and / or additives are embedded within the Ulva protoplasm article. In some embodiments, surfactants and / or additives are surrounded by the Ulva protoplasm article (e.g., the surfactant is located between layers of the Ulva protoplasm article). In some embodiments, surfactants and / or additives are uniformly distributed within the Ulva protoplasm article (e.g., assessed by testing the surfactant concentration at at least three different locations on a coated substrate).

[0118] In some embodiments, the additives include any one of the following: tackifiers, fillers (e.g., clay particles), plasmids, elastomers, pigments, dyes, antioxidants (such as free radical scavengers, anti-ozone agents), pH stabilizers, light stabilizers, UV stabilizers, heat stabilizers, flame retardants, or any combination thereof.

[0119] Non-limiting examples of additives include, but are not limited to, 2,4-dihydroxybenzophenone, 2-hydroxy-4-N-(octyl)benzophenone, derivatives of 2-hydroxyphenyl-s-triazine, hindered amine light stabilizers (HALS), benzotriazolyl UV absorbers (such as Tinuvin), or combinations thereof.

[0120] Non-limiting examples of fillers according to the invention include talc, calcium carbonate, clay, silica, mica, wollastonite, feldspar, aluminum silicate, alumina, hydrated alumina, glass microspheres, ceramic microspheres, thermoplastic microspheres, barite, and sawdust.

[0121] In some embodiments, UV stabilizers include shielding agents, absorbers, quenchers, free radical scavengers, and peroxide decomposers. Non-limiting examples of UV absorbers include benzophenone, benzotriazole, aryl esters, N,N'-oxalyldiphenylamine, acrylates, and formamidinium.

[0122] Non-limiting examples of antioxidants according to the present invention include phenols, aromatic amines, phosphates, phosphites, and BHT.

[0123] In some embodiments, the w / w concentration of the additive in the Ulva polysaccharide product is between 0.01 and 10%, between 0.01 and 1%, between 0.1 and 2%, between 1 and 2%, between 2 and 5%, between 5 and 10%, between 0.01 and 5%, between 0.1 and 5%, and any range therein.

[0124] In some embodiments, the ulva polysaccharide product is stable upon exposure to UV and / or visible light radiation. In some embodiments, the product is stable for at least 12 months, at least 15 months, at least 18 months, at least 20 months, or at least 24 months after exposure to 180 kronorleys (KLy pa) of UV radiation per year. In some embodiments, the UV stability of the product is measured according to ISO 4892-2.

[0125] As used herein, the term "stable" refers to the ability of an article to maintain its structural and / or mechanical integrity. In some embodiments, an article is called stable if it is characterized by sufficient mechanical integrity to be used as packaging material. In some embodiments, an article is called stable if it substantially maintains its structural and / or mechanical integrity under outdoor conditions (such as temperatures of -25°C and 75°C, rain, humidity, UV and / or visible light exposure for at least 12 months, as described above). In some embodiments, a stable article is rigid under outdoor conditions. In some embodiments, a stable article retains at least 50% of its initial tensile strength and / or elasticity. In some embodiments, the term "initial" refers to immediately after the article is manufactured, before exposure to storage conditions and / or outdoor conditions. In some embodiments, it is essentially as described below.

[0126] In some embodiments, the ulva-based articles of the present invention can have any three-dimensional shape. In some embodiments, the three-dimensional shape is any shape of the ulva-based article, which can be any shape obtainable by hot-melt processing. In some embodiments, the ulva-based articles of the present invention are in the form of a continuous layer, such as a film, or in the form of a container, wherein the film forms or defines at least one wall of the container. In some embodiments, the container is tableware. In some embodiments, the container is a tube (e.g., a hollow tube).

[0127] In some embodiments, the film is a single layer. In some embodiments, the film is a multilayer.

[0128] The term "continuous layer" or "layer" refers to a substantially homogeneous material of substantially uniform thickness that retains its physicochemical properties (e.g., mechanical strength, elasticity, Young's modulus, chemical composition, water content) throughout its entire dimensions (length and width dimensions). In some embodiments, each layer has a different physical structure and / or a different chemical composition. In some embodiments, each layer has the same physical structure and / or the same chemical composition. In some embodiments, the term "layer" refers to a layer of Ulva protopanax.

[0129] The term "thickness" refers to dry thickness. As used herein, the term "dry thickness" refers to the thickness of a dried film layer (e.g., after significant evaporation or removal of water). A dried film layer refers to a solid film layer (e.g., a non-flowing layer that substantially retains its shape and / or size when tilted).

[0130] In some embodiments, the article is an extruded article. In some embodiments, the article is an extruded film. In some embodiments, the film is a continuous film. In some embodiments, the film is in the form of a strip or tape. In some embodiments, the film is in the form of a mesh. In some embodiments, the film is in the form of interwoven yarns, threads, fibers, or strips.

[0131] In some embodiments, the film is characterized by a thickness between 0.1 and 1 mm, 0.1 and 0.5 mm, 0.5 and 2 mm, 1 and 10 mm, 2.5 and 5 mm, and 0.5 cm and 5 cm, including any range or value therebetween.

[0132] In some embodiments, the film is characterized by a thickness between 10µm and 1000µm, 200µm and 500µm, 100µm and 1000µm, 1mm and 10mm, 2mm and 5mm, 5µm and 200µm, 1mm and 5mm, or any range or value therein. Each possibility represents a separate embodiment of the invention.

[0133] In some embodiments, the article is in the form of a 2D film or a three-dimensionally shaped film (e.g., a container). In some embodiments, the film is characterized by (i) a strain at maximum load greater than 22%, greater than 25%, greater than 27%, greater than 30%, greater than 32%, between 22 and 45%, between 25 and 40%, between 25 and 35%, or any range therein; and (ii) a stress at maximum load greater than 12 MPa, greater than 15 MPa, greater than 20 MPa, greater than 25 MPa, greater than 30 MPa, between 12 and 35 MPa, between 15 and 35 MPa, or both (i) and (ii). The strain / stress at maximum load is measured according to ASTM D-882.

[0134] In some embodiments, the extruded film of the present invention is characterized in that the strain (SML) under maximum load is greater than that of the control, i.e., films having the same dimensions and made from the same ulnar polysaccharide extract by solvent casting; wherein, greater than the control is at least 10%, at least 15%, at least 20%, at least 50%, at least 70%, at least 100%, or between 10% and 80%, including any range therebetween.

[0135] In some embodiments, the extruded film of the present invention is characterized in that the stress under maximum load (STML) is greater than that of the control, i.e., films of the same size made from the same ulnar polysaccharide extract by solvent casting; wherein greater than the control is at least 20%, at least 50%, at least 100%, at least 200%, at least 300%, at least 400%, or between 50 and 500%, between 50 and 450%, or any range therein.

[0136] In some embodiments, the ulva polysaccharide products of the present invention are in the form of sheets, films, packaging products, agricultural products, containers comprising one or more walls, or any combination thereof.

[0137] In some embodiments, the ulva polysaccharide product is a light-transparent product. In some embodiments, the ulva polysaccharide product is characterized by a visible light transparency between 30% and 70%, between 30% and 60%, between 30% and 50%, and any range therein.

[0138] Non-crosslinked ulmosan products In some embodiments, a non-crosslinked ulva-based article is provided, which is primarily composed of ulva-based material and optionally plasticizers, activators, and / or additives; wherein the non-crosslinked ulva-based article is characterized by a water content between 2% and 15%, 2% and 7%, 2% and 6%, 2% and 5%, 2% and 4%, 5% and 15%, 7% and 15%, 8% and 15%, 5% and 12%, 8% and 12%, 8% and 15%, or any range therein; and wherein the non-crosslinked ulva-based article is manufactured (or formed) by hot-melt processing. Those skilled in the art will understand that water content can affect the elasticity / rigidity of the article. Therefore, by changing the water content of the article, it is possible to obtain articles with elastic or plastic properties. In some embodiments, the non-crosslinked ulva products are substantially free of crosslinked ulva (i.e., the w / w content of crosslinked ulva in the total ulva content of the product is at most 5%, at most 3%, at most 1%, at most 0.5%, between 0.1 and 5%, between 0.1 and 1%, and any range therein).

[0139] In some embodiments, the non-crosslinked ulva polysaccharide article is in a solid state at temperatures up to 85°C, up to 86°C, as low as 87°C, up to 88°C, or up to 89°C. In some embodiments, the non-crosslinked ulva polysaccharide article / material is flowable within any temperature range between 89 and 120°C, 89 and 110°C, 89 and 100°C, 90 and 120°C, 90 and 110°C, 88 and 120°C, and 87 and 120°C, and in between.

[0140] In some embodiments, the non-crosslinked ulva polysaccharide product / material is a thermoplastic material. In some embodiments, the non-crosslinked ulva polysaccharide product / material is an elastic material.

[0141] In this document, the term "elasticity" refers to the tendency of a material (optionally in the form of layers) to return to its original shape after being deformed by stress (e.g., tensile stress and / or shear stress) at a temperature of 10 to 50°C.

[0142] Conversely, "rigid" materials do not return to their original shape after being deformed by stress; instead, they will fracture.

[0143] In some implementations, tensile properties (e.g., modulus of elasticity, elongation at break, recovery, and ultimate tensile strength) are determined according to ASTM International Standard D882-12 for testing the tensile properties of thin plastic sheets.

[0144] In some embodiments, the non-crosslinked ulva-based product further includes a plasticizer; wherein the w / w concentration of the plasticizer to the non-crosslinked ulva-based product is between 0.5% and 30%, 0.5% and 1%, 0.5% and 5%, 0.5% and 8%, 15% and 20%, 15% and 30%, 8% and 20%, 5% and 15%, 10% and 20%, 8% and 9%, 9% and 10%, 10% and 11%, 11% and 12%, and 8% and 12%, including any range therebetween. Those skilled in the art will understand that the concentration of the plasticizer is sufficient to provide elasticity to the non-crosslinked ulva-based product.

[0145] In some embodiments, a non-crosslinked composite ulva product is provided, primarily composed of non-crosslinked ulva, a plasticizer, and optionally an activator and / or additives; wherein the water content of the non-crosslinked composite ulva product is between 5% and 15%, 7% and 15%, 8% and 15%, 5% and 12%, 8% and 12%, or 8% and 15%, in any range therebetween. In some embodiments, the non-crosslinked composite ulva product is an elastic product.

[0146] As used herein, the term "composite / composite material" refers to a material (e.g., a solid or non-flowing material) in the form of a homogeneous mixture of two or more components (e.g., the ulva polysaccharide and plasticizer of the present invention), wherein the components are stably bonded together and cannot be separated by conventional methods. Composite materials are characterized by distinct physical properties (e.g., elasticity, elongation at break, mechanical strength, etc.) compared to the physical properties of individual components.

[0147] In some embodiments, the elastic article (e.g., film) of the present invention is stretched in at least one direction.

[0148] In some embodiments, the elastic article is characterized by an elongation at break of any range or value between 5% and 200%, 5% and 10%, 5% and 50%, 5% and 100%, 5% and 150%, 50% and 100%, 50% and 150%, and 150% and 200%. In some embodiments, the elastic article is characterized by a moisture content of any range between 5% and 30%, 7% and 15%, 8% and 15%, 5% and 12%, 8% and 20%, and 8% and 15%.

[0149] In some embodiments, the non-crosslinked Ulva protease product / material is a rigid product / material (e.g., in sheet form) characterized by a tensile strength between 5 and 200 MPa, 5 and 10 MPa, 5 and 50 MPa, 5 and 100 MPa, 10 and 50 MPa, 10 and 100 MPa, 50 and 100 MPa, 5 and 150 MPa, 50 and 200 MPa, or 150 and 200 MPa, including any range or value therebetween. In some embodiments, the rigid product is characterized by a moisture content between 1% and 8%, 1% and 7%, 2% and 7%, 2% and 5%, or 2% and 4%, including any range therebetween.

[0150] In some embodiments, the non-crosslinked ulva polysaccharide product is characterized by strain under maximum load and / or stress under maximum load as described above.

[0151] In some embodiments, the ulva polysaccharide products of the present invention are in the form of sheets, films, packaging products, agricultural products, or any combination thereof.

[0152] In some embodiments, the elastic article is in the form of a sheet, strip, thread, or film. In some embodiments, the elastic article (e.g., in the form of a sheet, strip, thread, or film) is characterized by its elasticity being sufficient for use as a packaging article. In some embodiments, the article is characterized by sufficient elasticity (e.g., a flexible, formable, and resilient film) to achieve any predetermined shape. In some embodiments, the elastic article is characterized by its elasticity (e.g., Young's modulus, elongation at break, etc.) being sufficient to achieve the shape of the packaged material (e.g., edible material, packaging, crop material, etc.).

[0153] In some embodiments, the rigid article is in the form of a container or a rigid film (e.g., a sheet). In some embodiments, the rigid article is characterized by an elongation at break of less than 100%, less than 50%, less than 30%, less than 20%, less than 10%, less than 5%, and any range therein.

[0154] Cross-linked Ulva protease products In some embodiments, a cross-linked ulva-based article / material is provided, which is essentially composed of cross-linked ulva and optionally plasticizers, activators, and / or additives; wherein the cross-linked ulva-based article / material is characterized by a water content between 2% and 15%, 2% and 7%, 2% and 6%, 2% and 5%, 2% and 4%, 5% and 15%, 7% and 15%, 8% and 15%, 5% and 12%, 8% and 12%, 8% and 15%, and any range therein. In some embodiments, the cross-linked ulva-based article / material is solid (i.e., non-flowing and retains its shape, as described above) at temperatures up to 85°C, up to 86°C, down to 87°C, up to 88°C, or up to 89°C.

[0155] In some embodiments, the cross-linked ulva polysaccharide articles / materials are flowable within any temperature range inclusive between 89 and 120°C, 89 and 110°C, 89 and 100°C, 90 and 120°C, 90 and 110°C, 88 and 120°C, and 87 and 120°C. In some embodiments, the cross-linked ulva polysaccharide articles / materials are thermoplastic materials.

[0156] In some embodiments, the w / w concentration of the crosslinking agent in the crosslinked ulva polysaccharide article / material, calculated on a dry weight basis, is between 3% and 40%, 5% and 35%, 5% and 30%, 5% and 10%, 3% and 10%, 3% and 15%, 5% and 20%, 20% and 30%, 20% and 40%, 5% and 15%, 10% and 25%, and 15% and 25%, 20% and 30%, 20% and 40%, 5% and 7%, 7% and 9%, 9% and 11%, 11% and 13%, 5% and 15%, 10% and 25%, and 15% and 25%, including any range therebetween.

[0157] In some embodiments, the crosslinking agent is a covalent crosslinking agent (e.g., a polyfunctional epoxy alkyl crosslinking agent). In some embodiments, the crosslinked ulva is a covalently crosslinked ulva.

[0158] As used herein, the term "crosslinking" refers to the formation of a chemical bond between two chemical moieties or groups. In some embodiments, crosslinking includes inter-crosslinking (e.g., where the chemical moieties are different SP chains). In some embodiments, crosslinking includes intra-crosslinking (e.g., where the chemical moieties are within the same SP chain).

[0159] In some embodiments, the covalent crosslinking agent is selected from: glutaraldehyde, diamine crosslinking agent, dithiol crosslinking agent, adipicoyl dichloride, alkyl diepoxide (e.g., 1,7-octane diepoxide), 1,4-butanediol diglycidyl ether, and methacrylic anhydride.

[0160] In some implementations, the crosslinking agent is dicyclooxyoctane.

[0161] In some embodiments, the cross-linked ulva polysaccharide product is light-transparent (i.e., visible light-transmitting), as described above.

[0162] In some embodiments, the crosslinked ulva polysaccharide product is characterized by a tensile strength between 5 and 300 MPa, 5 and 10 MPa, 5 and 50 MPa, 20 and 50 MPa, 20 and 100 MPa, 5 and 20 MPa, 50 and 100 MPa, 50 and 150 MPa, 150 and 300 MPa, 50 and 250 MPa, and 200 and 300 MPa, including any range or value therebetween.

[0163] In some embodiments, the cross-linked Ulva protopanax product is characterized by an elongation at break of 5% to 100%, 5% to 10%, 5% to 20%, 5% to 50%, 10% to 40%, 10% to 15%, 20% to 40%, 20% to 50%, 20% to 70%, 20% to 80%, 60% to 80%, 70% to 90%, or any range or value thereof.

[0164] In some embodiments, the cross-linked ulva polysaccharide product is in granular form. In some embodiments, the granules are suitable for hot-melt processing (i.e., they are flowable in a temperature range between 89 and 120°C, as described above).

[0165] In another aspect, a particulate composition is provided, wherein each particulate is substantially composed of cross-linked ulva, and optionally comprises at least one of a plasticizer, an activator, and / or an additive; wherein the cross-linked ulva article is characterized by a water content between 2% and 40%, 2% and 7%, 2% and 6%, 2% and 5%, 2% and 4%, 5% and 15%, 7% and 15%, 8% and 15%, 5% and 12%, 8% and 12%, 8% and 15%, 10% and 40%, about 30% and about 40%, about 10% and about 40% w / w, and any range therein.

[0166] In some embodiments, the moisture content of the particles is up to 40%, up to 38%, up to 35%, up to 30%, up to 25%, up to 20%, between 2 and 40%, between 2 and 7%, between 2 and 6%, between 2 and 5%, between 2 and 4%, between 5 and 15%, between 7 and 15%, between 8 and 15%, between 5 and 12%, between 8 and 12%, between 8 and 15%, between 10 and 40%, between about 30 and about 40%, between about 10 and 40% w / w, and any range therein.

[0167] In some embodiments, the particulate composition is characterized by an average particle size between 0.1 and 100 mm. In some embodiments, the particulate composition is suitable for hot-melt processing. In some embodiments, the particulate composition is extrudable or moldable. In some embodiments, as described above, the particulate composition is flowable under conditions suitable for hot-melt processing, i.e., in a temperature range of 89 to 120°C.

[0168] Manufacturing method In another aspect, a method for manufacturing any of the articles disclosed herein is provided, comprising contacting ulva-3 (e.g., cross-linked or non-cross-linked ulva-3) with water (or an aqueous solution) at a water:ulva-3 ratio between 1:5 and 1:2 to form a hydrated powder; and providing the hydrated powder under conditions suitable for hot-melt processing to shape the ulva-3 article. In some embodiments, the hydrated powder is flowable under conditions suitable for hot-melt processing. In some embodiments, the step includes mixing water with ulva-3 at a water:ulva-3 ratio between 1:5 and 1:2, 1:4 and 1:3, 1:3 and 1:2, 3:6.5 and 3:7.5, 3:7.2 and 3:6.8, 3:7.1 and 3:6.9, about 3:7, and any range thereof.

[0169] In some embodiments, forming the hydrated powder includes mixing water with (i) ulva-3 or (ii) cross-linked ulva-3 and optionally (iii) a plasticizer under suitable conditions. In some embodiments, suitable conditions include at least one of the following: (i) a temperature between 30 and 70°C, between 30 and 60°C, between 40 and 60°C, between 40 and 50°C, between 50 and 60°C, between 40 and 70°C, between 40 and 45°C, between 45 and 50°C, between 50 and 55°C, between 50 and 60°C, and between 60 and 70°C, any range thereof; and (ii) a time period between 1 minute and 1 hour, at least 0.5 hours, at least 0.1 hours, at least 1 hour, at least 1.5 hours, at least 2 hours, at least 2.5 hours, at least 3 hours, at least 4 hours, and at least 5 hours, any range thereof. In some embodiments, suitable conditions further include mixing water with (i) ulva and (ii) cross-linked ulva and optionally (iii) a plasticizer.

[0170] In some embodiments, the dried ulva polysaccharide is in powder form, characterized by an average particle size between 10 μm and 5 mm, between 100 μm and 5 mm, between 100 μm and 1 mm, between 100 μm and 2 mm, and any range therein.

[0171] In some embodiments, the hydrated powder is characterized by an average particle size between 10 μm and 5 mm, between 100 μm and 5 mm, between 100 μm and 1 mm, between 100 μm and 2 mm, and any range therein.

[0172] In some embodiments, the forming step is performed by hot melt processing. In some embodiments, hot melt processing includes extrusion, injection molding, hot blow molding, molding (e.g., casting molding, compression molding, rotational molding) or any combination thereof.

[0173] In some embodiments, the hot melt process is extrusion. In some embodiments, the hot melt process is compression molding.

[0174] In some embodiments, suitable conditions for hot melt processing include temperatures of at least 70°C, at least 80°C, at least 85°C, at least 88°C, at least 89°C, about 90°C, and any range or value between 87 and 120°C, 90 and 120°C, 90 and 100°C, 90 and 110°C, 89 and 110°C, and 89 and 100°C, including any range or value therein.

[0175] In some embodiments, the w / w percentage of ulva in the hydrated powder is at least 40%, or between 40% and 80%, between 50% and 55%, between 55% and 60%, between 60% and 65%, between 65% and 70%, between 40% and 50%, and between 70% and 80%, including any range therein.

[0176] In some embodiments, the water w / w percentage in the hydrated powder is at least 20%, and is between 20% and 60%, 20% and 30%, 20% and 40%, 25% and 30%, 30% and 35%, 30% and 40%, 40% and 50%, and 30% and 60%, including any range therebetween.

[0177] In some embodiments, the hydrated powder is a mixture that further includes a plasticizer. In some embodiments, the w / w percentage of the plasticizer in the mixture is between 5% and 20%, between 5% and 10%, between 10% and 15%, between 15% and 20%, and between 8% and 12%, including any range therebetween.

[0178] In another aspect, a method for manufacturing any of the articles disclosed herein is provided, comprising placing a hydrated powder (i.e., consisting substantially of non-crosslinked or crosslinked ulva and water, and optionally further comprising a plasticizer, as described above) under conditions suitable for extrusion, thereby shaping the ulva article. In some embodiments, the article is an extruded ulva article.

[0179] In some embodiments, the hydrated powder is fed into the extrusion apparatus at an appropriate ratio between 1 and 7000 kg / hr, 1 and 10 kg / hr, 10 and 100 kg / hr, 100 and 1000 kg / hr, 1000 and 7000 kg / h, or any range thereof.

[0180] In some embodiments, suitable extrusion conditions include temperatures of at least 75°C, at least 80°C, at least 85°C, about 80°C, and temperatures between 77 and 90°C, between 78 and 85°C, between 79 and 85°C, between 79 and 83°C, between 79 and 82°C, and between 79 and 81°C, including any range or value therebetween.

[0181] In some embodiments, a method is provided for manufacturing or shaping the cross-linked ulva polysaccharide article of the present invention, the method comprising providing the particulate composition of the present invention under conditions suitable for hot-melt processing, thereby shaping the cross-linked ulva polysaccharide article. In some embodiments, the conditions suitable for hot-melt processing are as described above.

[0182] In some embodiments, the method of manufacturing cross-linked ulva products further includes a preparatory step of manufacturing the particulate composition of the present invention, comprising contacting ulva (non-cross-linked ulva) with water (or an aqueous solution) at a water:ulva ratio of 1:5 to 1:2, 1:4 to 1:3, 1:3 to 1:2, 3:6.5 to 3:7.5, 3:7.2 to 3:6.8, 3:7.1 to 3:6.9, about 3:7, or any range thereof, to form a hydrated powder; adding a cross-linking agent to the hydrated powder to obtain a mixture; providing the mixture under suitable cross-linking conditions to obtain cross-linked ulva; adding a polar organic solvent to obtain precipitated cross-linked ulva; and separating the precipitated cross-linked ulva to obtain the particulate composition.

[0183] In some embodiments, the addition of the crosslinking agent and contact of the ulva polysaccharide with the aqueous solution (or water) are carried out simultaneously or sequentially.

[0184] In some embodiments, suitable crosslinking conditions include pH values ​​between 8 and 14, 9 and 14, 9 and 12, 10 and 14, 10 and 11, 11 and 12, 12 and 13, 13 and 14, and any values ​​in between.

[0185] In some embodiments, the hydrated powder comprising cross-linked ulnar polysaccharide is characterized by a pH value between about 12 and about 13.

[0186] In some embodiments, suitable crosslinking conditions further include temperatures between 30 and 70°C, between 30 and 60°C, between 40 and 60°C, between 40 and 50°C, between 50 and 60°C, between 40 and 70°C, between 40 and 45°C, between 45 and 50°C, between 50 and 55°C, between 50 and 60°C, and between 60 and 70°C, including any range therebetween.

[0187] In some embodiments, suitable conditions for crosslinking further include a crosslinking agent amount ranging from about 3% to about 20%, about 4% to about 20%, about 5% to about 20%, about 5% to about 15% w / v, or any range therein, relative to the volume of the hydrated powder.

[0188] In some implementations, suitable crosslinking conditions include reaction time periods ranging from 1 minute to 1 hour, at least 0.5 hours, at least 0.1 hours, at least 1 hour, at least 1.5 hours, at least 2 hours, at least 2.5 hours, at least 3 hours, at least 4 hours, and at least 5 hours, including any range of reaction time periods therebetween.

[0189] In some embodiments, the polar organic solvent is or includes alcohols (e.g., low alcohols such as ethanol or methanol).

[0190] In some embodiments, the present invention provides a combination formulation. In one embodiment, "combination formulation" is specifically defined as a "kit" because the combination partners described above can be packaged or stored independently, or different fixed combinations of different numbers of combination partners can be used, i.e., packaged or stored simultaneously, concurrently, individually or sequentially.

[0191] In some embodiments, the kit includes: (i) a first compartment comprising ulva polysaccharide; (ii) a second compartment comprising a plasticizer; and optionally (iii) a third compartment comprising a crosslinking agent. In some embodiments, any one of the first, second, and third compartments comprises a surfactant, or an additive, or a solvent, or a stabilizer, or any combination thereof.

[0192] In some embodiments, the kit includes instructions for mixing any compartments of the kit to obtain the hydrated powder of the present invention. In some embodiments, the kit includes dilution instructions, as well as instructions for optionally mixing the first compartment, optionally the second compartment, and optionally the third compartment together. In some embodiments, the first compartment, optionally the second compartment, and optionally the third compartment of the kit are mixed together for up to 5 hours before using the hydrated powder obtained by the present invention.

[0193] In some embodiments, mixing includes metering the compartments in an amount sufficient to obtain a predetermined w / w ratio of ursulphurin in the hydrated powder.

[0194] In some implementations, the first compartment, optional second compartment, and optional third compartment of the kit are diluted before mixing.

[0195] General The term “about” as used herein refers to ±10%. Furthermore, all numerical values, such as those referring to the amount or range of elements constituting a formulation, are approximate and may differ from the stated value by up to 10% (+) or (-). It should be understood that the word “about” precedes all numerical names, even if not always explicitly stated.

[0196] The terms “comprises, comprising,” “includes, including,” “having,” and their conjugations mean “including but not limited to.”

[0197] In the specification and claims of this application, each verb “comprise,” “include,” and “have,” and its conjugations, used to indicate one or more objects of the verb, is not necessarily a complete list of components, elements, or parts of a verb’s many or many subjects.

[0198] The term "consisting of" means "including and limited to".

[0199] The term "consisting essentially of" means that the composition, method, or structure may include additional ingredients, steps, and / or portions, provided that these additional ingredients, steps, or portions do not materially alter the essential and novel characteristics of the claimed composition, method, or structure. The term "consisting essentially of" is used to define a formulation that includes the stated element but excludes other elements that may be significant to the formulation.

[0200] As used herein, the term "exemplary" means "as an example, illustration, or description." Any implementation described as "exemplary" is not necessarily to be construed as superior to or advantageous to other implementations and / or as excluding features of other implementations.

[0201] As used herein, the term "optionally" means "provided in some embodiments and not in others." Unless these features conflict, any particular embodiment of the invention may include multiple "optional" features. The terms "optionally" and "further" are used interchangeably herein. The terms "film / films" and "layer / layers" are used interchangeably herein. As used herein, the term "coat" refers to a composite layer disposed on a substrate, excluding the substrate, while the term "substrate" refers to the portion of the composite structure supporting the disposed layers / coatings. In some embodiments, the terms "layer," "film," or other terms used interchangeably herein refer to a substantially uniform thickness of a substantially uniform substance.

[0202] As used herein, the term “substantially” means at least 85%, at least 90%, at least 92%, at least 95%, at least 96%, at least 97%, at least 98%, at least 99%, or between 60 and 99.9%, between 70 and 80%, between 70 and 90%, between 80 and 90%, between 90 and 95%, between 95 and 99.9%, or any range or value in between.

[0203] Unless the context clearly specifies otherwise, the singular forms “a,” “an,” and “the” used herein include plural references. For example, the terms “a compound” or “at least one compound” can include multiple compounds, including mixtures thereof.

[0204] Throughout this application, various embodiments of the invention may be presented in a range format. It should be understood that the range format is merely for convenience and brevity and should not be construed as an inflexible limitation of the scope of the invention. Therefore, the description of a range should be considered as specifically disclosing all possible subranges and the individual values ​​within that range. For example, a description of a range such as 1 to 6 should be considered as specifically disclosing subranges such as 1 to 3, 1 to 4, 1 to 5, 2 to 4, 2 to 6, 3 to 6, etc., and the individual numbers within that range, such as 1, 2, 3, 4, 5, and 6. This applies regardless of the breadth of the range.

[0205] Wherever a range of numbers is specified in this document, it means that any referenced number (fraction or integer) within the specified range is included. The phrases “range between the first and second indicator numbers” and “range from the first to the second indicator number” are used interchangeably in this document and are intended to include the first and second indicator numbers and all fractions and integers in between.

[0206] As used herein, the term "method" refers to the manner, means, techniques, and procedures for accomplishing a given task, including but not limited to those manner, means, techniques, and procedures known or readily developed by practitioners in the fields of chemistry, pharmacology, biology, biochemistry, and medicine.

[0207] Other terms used herein are meant to be defined by their well-known meaning in the art.

[0208] It should be understood that, for clarity, certain features of the invention described in the context of a single embodiment may also be provided in combination in a single embodiment. Conversely, for brevity, various features of the invention described in the context of a single embodiment may also be provided individually, or in any suitable sub-combination, or appropriately provided in any other described embodiment of the invention. Certain features described in the context of various embodiments should not be considered essential features of those embodiments unless the embodiment is inoperable without these elements.

[0209] The various embodiments and aspects of the invention described above and claimed in the appended claims are experimentally supported in the following examples.

[0210] Example Example 1 Purification of Ulva protopanax An exemplary processing method for Ulva prolifera biomass to obtain partially purified Ulva prolifera. Fresh Ulva prolifera is air-dried and ground to form a powder with a typical particle size distribution of less than 1 mm in diameter. Distilled water is added to the powder at a weight / volume ratio of 10:1 between water and Ulva prolifera powder, and the mixture is mixed at a heating temperature (80-90°C) for 2-4 hours. The mixture is then filtered through a 25-250 µm membrane and centrifuged to remove cell lysates. Precipitation of the Ulva prolifera-based substance is then induced by adding ethanol to the supernatant, and the resulting greenish-white precipitate is discarded. The resulting clear liquid is centrifuged, filtered through a 40 µm mesh, or incubated at 4°C for 4 days to induce phase separation. Three phases are obtained: 1. a greenish-white solid (floating on the liquid), 2. a clear yellow liquid, and 3. a greenish-gray phase with a gel-like consistency. The second phase is discarded, and the first and third phases are collected, dried, and ground into powder. Optionally, the powder is further washed with ethanol and centrifuged before grinding to extract the green pigment (e.g., chlorophyll).

[0211] The obtained extract (concentration 1 g / 100 ml) exhibited strong UV / Vis absorbance in the regions between 390 and 500 nm and between 650 and 700 nm. The UV / Vis spectrum of the extract showed two peaks: a first peak at approximately 420 nm and a second peak at approximately 660 nm, corresponding to chlorophyll absorption.

[0212] The extracted ulva polysaccharide was analyzed by FTIR, showing characteristic carbonyl, hydroxyl, COC, COS, and sulfate IR peaks (e.g., at 3375–3380, 1624–1630, 1417–1420, 1125–1226, 1055–1085, 820–856 cm⁻¹). -1 (Location).

[0213] The sulfated polymers in the extracted ulnar polysaccharide were analyzed by GPC, and the following average molecular weight / MW distribution values ​​of the sulfated polymers were obtained: Example 2 Non-crosslinked ulmosan products Rigid film (sheet) formation: Add 30% (w / v) distilled water to dry ulva polysaccharide powder and gently stir at 50°C until the water is completely absorbed by the ulva polysaccharide powder (approximately 1 hour). The hydrated powder is then transferred to a heat treatment process. The powder is dispersed in a compression molding die and placed in a press preheated to 90°C, then heated for 3-5 minutes until completely melted, and then compressed at 2 bar to form a film. The molded film is cooled and removed from the die.

[0214] The mechanical properties of the resulting film were tested and compared with those of a similar film manufactured by solvent casting (both films having a thickness of ~0.1 mm). The mechanical properties were determined according to ASTM D-882.

[0215] Table 1 below summarizes the results of the test.

[0216] Table 1: As shown in Table 1, compared with solvent-cast films, the films of the present invention exhibit almost twice the strain and more than four times the stress under maximum load.

[0217] Furthermore, the inventors successfully manufactured a film based on ulva by extrusion. In short, ulva powder is premixed with water (30% w) and optionally a plasticizer (10% glycerol), fed into an extruder with a flat die, and processed at 80°C to form a film.

[0218] Example 3 Non-crosslinked ulmosan products with plasticizers Flexible film formation: 30% (w / v) distilled water and 5-20% w / w glycerol (Sigma-Aldrich, Israel) are added to dried ulnar polysaccharide powder and gently stirred at 50°C until the water is completely absorbed by the powder (approximately 1 hour) to obtain a mixture. The mixture is then transferred to a heat treatment process. The mixture is dispersed in a compression molding die and placed in a press preheated to 90°C, then heated for 3-5 minutes until completely melted, and then compressed at 2 bar to form a film. The molded film is cooled and removed from the die.

[0219] Optionally, as described in Example 2, the mixture containing 10% glycerol is extruded to form an extruded film.

[0220] Example 4 Cross-linked Ulva protease products Ulva protosan powder was completely dissolved at 3% (w / v) in a 40 mM NaOH solution at pH 12.5. 5-15% of 1,2,7,8-diepoxyoctane (Sigma-Aldrich) was added to the film. Films were prepared using granulated cross-linked ulva protosan as previously described in the non-cross-linking process, with the solution (w / w) stirred at 50°C for 3 h. The ulva protosan was then precipitated in ethanol and dried to produce granulated material.

[0221] The inventors speculate that the granulated material can be further processed into the thermomelting of exemplary articles of the present invention (e.g., films) by compression molding and / or extrusion.

[0222] All publications, patents, and patent applications mentioned in this specification are incorporated herein by reference in their entirety, to the same extent that each individual publication, patent, or patent application is specifically and individually indicated to be incorporated herein by reference. Furthermore, any reference or identification of any reference in this application should not be construed as an admission that such reference is prior art to the invention. The use of section headings should not be construed as necessarily limiting.

[0223] Although the invention has been described in conjunction with specific embodiments thereof, it will be apparent to those skilled in the art that many alternatives, modifications, and variations will be apparent. Therefore, it is intended to cover all such alternatives, modifications, and variations falling within the spirit and broad scope of the appended claims.

Claims

1. A product of ulvan wherein the product of ulvan is characterized by a water content between about 1 to about 25%; and wherein the product of ulvan is obtained by hot melt processing.

2. The product of ulvan of claim 1, wherein the product of ulvan further comprises a plasticizer.

3. A product of ulvan which is a composite comprising ulvan and a plasticizer; wherein the w / w concentration of the plasticizer within the product of ulvan is between 0.5 to 30%, and wherein the product of ulvan is obtained by hot melt processing.

4. The product of ulvan of claim 2 or 3, wherein the plasticizer comprises a water soluble polymer, a diol, a triol, a monosaccharide, a disaccharide, including any combination thereof.

5. The product of ulvan of claim 4, wherein the plasticizer is glycerol.

6. The product of ulvan of any one of claims 1 to 5, wherein the ulvan within the product of ulvan is non-crosslinked ulvan; and wherein the product of ulvan is substantially free of a crosslinking agent.

7. The product of ulvan of any one of claims 1 to 6, and wherein the product of ulvan is flowable at a temperature between 89 to 120 °C, at a pressure of 1 bar.

8. The Ulvan preparation according to any one of claims 1 to 7, in the form of a film, characterized in that at least one of: a strain at maximum load higher than 25%; and a stress at maximum load exceeding 12 MPa.

9. A product of ulvan, wherein the ulvan is crosslinked ulvan, wherein the w / w concentration of a crosslinking agent within the crosslinked ulvan is between 5 to 25%; and wherein the product of ulvan is obtained by hot melt processing.

10. The product of ulvan of claim 9, wherein the crosslinking agent is a multifunctional covalent crosslinking agent.

11. The product of ulvan of claim 10, wherein the multifunctional covalent crosslinking agent is a diepoxyalkyl.

12. The product of ulvan of any one of claims 1 to 11, wherein the w / w percentage of ulvan in the product of ulvan is between 60 to 98% by dry weight of the product of ulvan.

13. The product of ulvan of any one of claims 1 to 12, wherein the product of ulvan is compostable, degradable, biodegradable, or any combination thereof.

14. The product of ulvan of any one of claims 1 to 13, in the form of a film, a sheet, a tape, a web, a nonwoven material, a granule, or a container comprising any combination thereof.

15. The product of ulvan of any one of claims 1 to 14, which is (i) a thermoformed article, wherein the thermoforming is performed at a temperature between 89 to 120 °C; or (ii) an extruded article, wherein the extrusion is performed at a temperature between 79 to 85 °C.

16. A method for manufacturing the Ulva polysaccharide article of any one of claims 1 to 15, comprising contacting Ulva polysaccharide with water under suitable conditions, thereby obtaining a hydrated powder; and shaping the hydrated powder under conditions suitable for hot melt processing; wherein the hydrated powder is flowable under conditions suitable for hot melt processing; and wherein the proportion of water in the hydrated powder is between 20 and 60% w / w.

17. The method of claim 16, wherein the contacting comprises mixing; and wherein the suitable conditions comprise a temperature between 30 and 70 °C and a time period between 1 minute and 10 h.

18. The method of claim 16 or 17, wherein the Ulva polysaccharide is a dry matter of an aqueous extract of a species of the Ulva genus of algae; and wherein the aqueous extract is a whole plant extract.

19. The method of claim 18, wherein the whole plant extract includes chlorophyll, and is characterized by the first UV peak has a maximum at a wavelength between 400 and 440 nm, and the second UV peak has a maximum at a wavelength between 640 and 680 nm.

20. The method of any one of claims 16 to 19, wherein the contacting further comprises adding the plasticizer.

21. The method of claim 20, wherein the concentration of the plasticizer in the hydrated powder is between about 5 and about 20% w / v.

22. The method of any one of claims 16 to 21, wherein the hot melt processing comprises any injection, hot blown film, thermoforming, or any combination thereof; and wherein the conditions suitable for hot melt processing comprise a temperature between about 89 and about 120 °C.

23. The method of claim 22, wherein the conditions suitable for hot melt processing comprise a temperature between about 90 and about 95 °C.

24. The method of any one of claims 16 to 21, wherein the hot melt processing is extrusion; wherein the shaping step comprises feeding the plurality of particles into an extruder; and wherein conditions suitable for hot melt processing comprise a temperature between 78 and 85 °C.

25. A method of manufacturing the Ulva polysaccharide article of any one of claims 9 to 15, the method comprising: contacting non-crosslinked Ulva polysaccharide with water in a water:Ulva polysaccharide ratio between 1:5 and 1:2, and with a crosslinking agent under conditions suitable for crosslinking, thereby obtaining crosslinked Ulva polysaccharide; adding a polar organic solvent in an amount sufficient to precipitate the crosslinked Ulva polysaccharide, thereby obtaining a plurality of particles; and providing the plurality of particles under conditions suitable for hot melt processing; thereby obtaining the article.

26. The method of claim 25, further comprising isolating the plurality of particles.

27. The method of claim 25 or 26, wherein the conditions suitable for crosslinking comprise a concentration of crosslinking agent in a range between about 3 and about 20% w / v, and optionally comprise any one of: a pH of the hydrated powder between 8 and 14; and a temperature between 30 and 70 °C.

28. The method of any one of claims 25 to 27, wherein the crosslinked Ulva polysaccharide is characterized by a degree of crosslinking between 5 and 25%.

29. The method of any one of claims 25-28, wherein the method further comprises a preliminary step of processing the Ulva biomass to obtain the Ulva polysaccharide.

30. The method of claim 29, wherein the processing comprises water extraction of the Ulva biomass to obtain a whole plant extract, and drying the whole plant extract to obtain a dry matter.

31. The method of claim 30, wherein the Ulva biomass comprises an algal species of the genus Ulva; and wherein the water extraction further comprises separating water-soluble or water-dispersible fractions from solid sediments.

32. The method of claim 30 or 31, wherein the dry matter is a partially purified Ulva polysaccharide further comprising chlorophyll.

33. The method of any one of claims 25-32, wherein the hot-melt processing comprises any one of extrusion, injection, hot blown film, molding, or any combination thereof.

34. The method of any one of claims 25-32, wherein the hot-melt processing is extrusion; wherein the providing step comprises feeding the plurality of particles into an extruder; and wherein the conditions suitable for hot-melt processing comprise a temperature between 78-85 °C.

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