Manufactured articles comprising nanocellulose elements

Description

1 / 102 MANUFACTURED ARTICLES COMPRISING NANOCELLULOSE ELEMENTS RELATED REQUEST

[001] This application claims the benefit of U.S. Provisional Application 63 / 458,269, filed April 10, 2023. All content of the above patent application is incorporated by reference into the present invention. FIELD OF THE INVENTION

[002] This patent application relates to formulations comprising nanocellulosic materials for use in synthetic or natural bioplastic products. BACKGROUND OF THE INVENTION

[003] Synthetic plastics are materials made of long polymer chains, with chemical and physical properties determined by the type of monomers involved in the polymerization process, how they are linked to each other in the polymer backbone, and what side chains they possess. Most plastics have carbon-based backbones, with or without the incorporation of heteroatoms. Synthetic (“artificial”) plastics are formed from chemical reactions such as condensation, addition, and crosslinking. Representative categories of plastics include acrylics, polyesters, polyurethanes, halogenated polymers, and bioplastics. The latter category, bioplastics, refers to synthetic plastics formed from bioderived monomers, such as proteins, polysaccharides, and sugar derivatives. The vast majority of synthetic plastics, however, are petroleum-based polymers, formed from petrochemical sources.

[004] Approximately 400 million metric tons of synthetic plastics were produced in 2021. Six main types of polymers, all derived from petrochemicals, account for about 70% of this. Petition 870250095211, dated 10 / 17 / 2025, page 11 / 112 2 / 102 Global plastic production: polyethylene terephthalate (PET), high-density polyethylene (HDPE), low-density polyethylene (LDPE), polyvinyl chloride (PVC), polypropylene (PP), and polystyrene (PS). If current trends continue with increasing demand for plastics and expanding production capacities, it is estimated that annual global plastic production will exceed 1.1 billion tons.

[005] The ubiquity of synthetic plastics presents two major environmental challenges. First, they are largely made from petrochemical raw materials and require significant energy consumption for their production, usually associated with the generation of greenhouse gases. Second, conventional synthetic plastics are resistant to degradation, which represents formidable obstacles to effective disposal and often persists in the environment for centuries. Although recycling can recover certain components from plastic waste, it is expensive, complicated and therefore has been poorly adopted: up to 2015, 6.3 billion tons of plastic waste were produced, of which only 9% were recycled, another 79% were deposited in landfills or discarded into the environment (including oceans) and another 12% were incinerated, with the consequent release of greenhouse gases and potentially toxic fumes.Despite the environmental consequences associated with synthetic plastics, they have become ubiquitous in commerce due, in part, to their durability. Because they do not decompose, they can be used to form articles that must be nearly permanent, strong, and resilient. Other properties, such as flexibility, conformability (plasticity), low production costs, and lightness, have increased their attractiveness.

[006] Concerns about the environmental impact of discarded and decomposing plastic articles have led manufacturers to consider Petition 870250095211, dated 10 / 17 / 2025, page 12 / 112 3 / 102 Bio-based alternatives. Composite materials, wholly or in significant part, of biological products or renewable agricultural materials or forest materials have been designated as “bio-based” by the USDA. Biopolymers derived from bio-based materials can be used to form bioplastic materials that offer alternatives to conventional petroleum-derived plastics.

[007] Biopolymers can be produced by biological systems (microorganisms, plants, animals) or chemically synthesized from biological materials such as proteins, starches, and sugars. The main sources of biopolymers are renewable, such as agricultural raw materials or waste. Many biopolymers are biodegradable, meaning they are able to decompose into carbon dioxide, water, and other organic compounds through the enzymatic actions of microorganisms. Bio-based plastics made from precursors such as polylactic acid (PLA), polyhydroxyalkanoates (PHAs), and cellulose are typically considered biodegradable because they can be decomposed in the environment by microorganisms under certain circumstances (such as high heat and long duration for PLA).Certain biodegradable materials are also considered "compostable," meaning they can be broken down by microorganisms to form nutrient-rich organic material capable of enriching the soil and producing end products similar to those produced during natural composting.

[008] Although these bio-based plastic alternatives, for example, polylactic acid plastics, starch-derived plastics or cellulose-based plastics, are of great interest as substrates for the manufacture of plastic materials, their use in common consumer applications, for example, as durable formed articles, containers and packaging, remains limited, partly due to performance limitations. These materials tend to be Petition 870250095211, dated 10 / 17 / 2025, page 13 / 112 4 / 102 hydrophilic and / or lipophilic, having a high affinity for water and / or fats. Therefore, these materials can become waterlogged or impregnated with grease, making them unsuitable as containers for food and other products loaded with water or oil. As water or oil penetrates durable goods, it begins to solvate the containers or packaging materials, affecting their mechanical properties, so that they become structurally weakened and predisposed to failure. These limitations of bio-based plastics have been resolved in many cases by coating the bioplastic materials with substances with strong hydrophobic and oleophobic properties, usually organic substances derived from petroleum, such as polyethylene, polyethyleneimine, PVC, or fluorocarbons, materials that have a well-recognized impact on the environment.Furthermore, although these coatings improve water and oil resistance in bio-based materials, these substances may still lack rigidity and mechanical strength.

[009] To address these limitations, manufacturers have added inorganic and organic materials as particle or fiber diluents to bio-based formulations to improve their mechanical properties and optimize their processing. Compared to materials using inorganic diluents, alternative bioplastics incorporating natural particles or fibers offer advantages in renewability, high strength, relatively easy processing, and other desirable properties. Nanoscale and microscale cellulosic fibers, such as nanofibrillated celluloses (NFCs), microfibrillated celluloses (MFCs), nanocrystalline celluloses (NCCs), and microcrystalline celluloses (MCCs), are particularly attractive diluents for improving strength. Although these nanoscale and microscale cellulose fibers and crystals (collectively called “nanocellulose elements,” “NC elements”) Petition 870250095211, dated 10 / 17 / 2025, page 14 / 112 While NCEs (5 / 102 or NCEs) may be promising for use in biopolymer products, there are limitations. First, the NCE fibers themselves are hydrophilic and therefore do not contribute to the water resistance of a formed product. Therefore, water-repellent treatments are still necessary for articles containing NCEs. More importantly, NCEs need to be transported to where they will be used in highly dilute suspensions (<1 to 10% by weight) to prevent them from becoming entangled with each other. This entanglement can lead to their consolidation into a dense, viscous mass that resists redispersion; if this compact network of aggregated cellulosic elements is further dehydrated, it solidifies even further, a process called hornification. Upon complete drying of the NCE suspension, a substantially indispersible, brick-like solid mass is formed.Therefore, in order to maintain a suspension of NCEs in a usable state, so that the properties of the NCEs it contains are accessible for use in other materials, it must be kept in a highly diluted form.

[010] Despite a decade of academic and industrial efforts, success in drying and redispersing low-cost and effective NCEs has eluded commercial nanocellulose producers. The dual challenges of (a) drying or concentrating the aqueous media in which the NCEs are suspended and (b) subsequently redispersing them are caused by two factors: (1) the propensity of cellulose polymers in NCEs to form hydrogen bonds with each other, adhering adjacent cellulosic elements into irreversible aggregates composed of a set of particles tightly bound to one another that resist redispersion; and (2) the enormous surface area per unit weight associated with the size and morphology of the NCE, considerably increasing the exposure of the NCE surfaces to each other and exacerbating adhesion due to hydrogen bonding. These two factors... Petition 870250095211, dated 10 / 17 / 2025, page 15 / 112 6 / 102 combine to produce hornification associated with concentrated and dried NCE suspensions. The tendency towards hornification in NCE suspensions requires these substances to be transported in a high volume of water, significantly increasing the costs associated with transportation and their use. Although drying techniques such as freeze-drying, spray drying, supercritical fluid drying and atomization, and the like, have been investigated by researchers, they have, at best, produced small samples of redispersed NC elements, using processes whose high cost, energy requirements, and need for specialized equipment prevent their widespread adoption. This resistance to redispersion has hindered the adoption of NCEs as an additive for other bio-based materials.

[011] Therefore, there is still a need in the art for methods and formulations that provide bioplastics with a satisfactory degree of mechanical strength and water / oil resistance, so that they can offer commercially viable alternatives to petroleum-derived plastics for manufactured articles. Insofar as NCEs are to be integrated into bio-based materials for such articles, there is a need to enable their commercial implementation at low cost, without excessive energy requirements and without the need for specialized equipment. To achieve these latter objectives, an unmet need remains to make nanocellulose-containing formulations redispersible and resistant to hornification, so that these formulations can be economically transported and introduced into bio-based composites efficiently and cost-effectively. SUMMARY OF THE INVENTION

[012] The present invention discloses, in embodiments, simple NCE-based materials comprising a simple NCE-based matrix, wherein the simple NCE-based matrix comprises a population of NCEs. Petition 870250095211, dated 10 / 17 / 2025, p. 16 / 112 7 / 102 redispersed, and wherein the simple NCE-based matrix provides an architectural framework for the simple NCE-based material. In some embodiments, the simple NCE-based material comprises a plurality of submatrices. In some embodiments, a pulp or pulp-based substance is integrated into the simple NCE-based matrix; the simple NCE-based matrix may be predominantly pulp. In some embodiments, the simple NCE-based matrix additionally comprises a reinforcing agent or a barrier formulation. In some embodiments, the matrix comprises a reinforcing agent, which may comprise an additional amount of NCEs. In some embodiments, the matrix comprises a barrier formulation that produces oleophobicity, which may comprise methylcellulose. In other embodiments, the matrix comprises a barrier formulation that produces hydrophobicity, which may comprise a resin acid or a combination of resin acids.Also disclosed in the present invention are articles of manufacture comprising the simple NCE-based material described above. In some embodiments, the article of manufacture further comprises a barrier formulation. In some embodiments, the article is shaped into a formed article, which may be shaped as a container.

[013] Also disclosed in the present invention are methods of manufacturing a simple NCE-based material, comprising (a) providing a redispersed suspension comprising redispersed NC elements, wherein the redispersed suspension is produced by the substeps of (i) providing an initial NCE suspension comprising NC elements suspended in a liquid or other fluid medium; (ii) adding a drying / dispersing additive to the initial NCE suspension to form a redispersible NCE suspension; (iii) drying the redispersible NCE suspension to produce a dry material comprising the redispersible NCEs; and (iv) suspending the Petition 870250095211, dated 10 / 17 / 2025, p. 17 / 112 8 / 102 dry material in a resuspension fluid to produce the redispersed suspension; (b) drying or concentrating the redispersed suspension to produce a simple NCE-based matrix, where the simple NCE-based matrix provides an architectural structure for the simple NCE-based material; and (c) adding an additive substance before or after the drying or concentration step, thus producing the simple NCE-based material. In some embodiments, the simple NCE-based matrix comprises a plurality of submatrices. In some embodiments, the additive substance is a bulking agent, which may comprise pulp or a pulp-based material. In some embodiments, the additive substance is a barrier formulation that produces oleophobicity and may comprise methylcellulose. In some embodiments, the additive substance is a barrier formulation that produces hydrophobicity, which may comprise a resin acid or a combination of resin acids.In some applications, the additive substance is an appearance-modifying agent, such as a pigment.

[014] Also disclosed in the present invention are embodiments of NCE-containing composite materials comprising NCE-containing composite matrices, wherein the NCE-containing composite matrix comprises a population of additive NCEs and an existing matrix, wherein the additive NCEs are integrated into the existing matrix, and wherein the existing matrix provides an architectural framework for the NCE-containing composite material. In some embodiments, the existing matrix is ​​bio-based. In some embodiments, the NCE-containing composite material further comprises one or more additive substances, wherein each additive substance is selected from the group consisting of reinforcing agents, barrier formulations, and bulking agents. Also disclosed in the present invention are articles of manufacture comprising the NCE-containing composite material described above. The article of Petition 870250095211, dated 10 / 17 / 2025, page 18 / 112 9 / 102 manufacturing can be selected from the group consisting of transaction cards, containers for liquids, packaging materials for consumer goods, films and thin sheets, and hollow cylinders for flexible tubing. Furthermore, methods for manufacturing a composite material containing NCEs are disclosed in the present invention, comprising: providing a population of additive NCEs and integrating the population into an existing matrix, thereby forming an NCE-containing composite matrix; and adding an additive substance to the NCE-containing composite matrix, thereby producing the NCE-containing composite material.

[015] In still other embodiments, simple NCE-based materials comprising a simple NCE-based matrix are disclosed in the present invention, wherein the simple NCE-based matrix comprises a population of redispersible NCEs treated with a drying / dispersion additive comprising a lower critical solution temperature (LCST) polymer; wherein the simple NCE-based matrix provides an architectural framework for the simple NCE-based material; and wherein the simple NCE-based material comprises a barrier formulation or a barrier substance. In some embodiments, the barrier formulation comprises a substance selected from the group consisting of cellulosic polymers, lipids, proteins, diluents, fatty acids, a resin acid, and combinations of resin acids.In certain aspects, the NCE-based material comprises a barrier substance, and the barrier substance is selected from the group consisting of cellulosic polymers, lipids, proteins, diluents, fatty acids, a resin acid, and combinations of resin acids. In some embodiments, the barrier formulation comprises a resin acid or a combination of resin acids. In certain embodiments, the barrier formulation comprises an oleophobic substance selected from the group. Petition 870250095211, dated 10 / 17 / 2025, p. 19 / 112 10 / 102 consisting of MC, HPMC, CMC, NaCMC, CA, CAB, chitosan, rosin, lignin, pea protein, and zein; in other embodiments, the barrier formulation comprises a hydrophobic substance selected from the group consisting of MC, CA, CAB, chitosan, rosin, hydrophobized starch, lignin, pea protein, and zein. In certain additional embodiments, the barrier substance is an oleophobic substance selected from the group consisting of MC, HPMC, CMC, NaCMC, CA, CAB, chitosan, rosin, lignin, and a vegetable protein; in other embodiments, the barrier substance is a hydrophobic substance selected from the group consisting of MC, CA, CAB, chitosan, rosin, hydrophobized starch, lignin, and a vegetable protein.In some embodiments, the NCE-based material additionally comprises one or more additive substances; in certain aspects, one or more additive substances are selected from a bulking agent, a reinforcing agent, or an appearance-modifying agent, or a combination thereof. In certain aspects, one or more additive substances are the bulking agent, which may comprise pulp or a pulp-based substance; in some embodiments, the simple NCE-based matrix is ​​predominantly pulp. In some embodiments, the bulking agent comprises diluent particles, which may comprise plant-derived organic materials. One or more additive substances may be a reinforcing agent, which may comprise an additional amount of NCEs.Furthermore, plastic substrates comprising these simple NCE-based materials are disclosed in the present invention, as well as articles of manufacture comprising such plastic substrates shaped into a formed article, such as a container or a food product receptacle.

[016] Also disclosed in the present invention are embodiments and methods of manufacturing a plastic article comprising a material Petition 870250095211, dated 10 / 17 / 2025, page 20 / 112 11 / 102 Simple NCE-based material in a flexible state, comprising (a) producing a simple NCE-based material comprising redispersible NC elements, wherein the simple NCE-based material is produced by the substeps of: (i) providing an initial suspension comprising NC elements suspended in a fluid medium; (ii) combining a drying / dispersing additive with the initial suspension to form a flexible suspension of redispersible NCEs; for example, the drying / dispersing additive comprises an LCST polymer; and (iii) adding an additive substance to the flexible suspension of redispersible NCEs, maintaining its flexibility, thereby forming the simple NCE-based material in a flexible state; and (b) forming or shaping the simple NCE-based material in the flexible state into a desired configuration, thereby manufacturing the plastic article.The addictive substance can be selected from the group consisting of boosting agents, barrier formulations, barrier substances, and bulking agents. In some embodiments, the training or shaping step involves extrusion.

[017] Further disclosed in the present invention are NCE-containing composite materials comprising NCE-containing composite matrices, wherein the NCE-containing composite matrix comprises a population of redispersible NCEs treated with a drying / dispersing additive comprising a lower critical solution temperature (LCST) polymer and an existing matrix; wherein the redispersible NCEs are integrated into the existing matrix and wherein the existing matrix provides an architectural framework for the NCE-containing composite material; and wherein the NCE-containing composite materials comprise a barrier formulation or a barrier substance. In some embodiments, the existing matrix comprises a bio-based polymer, which may comprise a cellulose derivative, which may be a poly Petition 870250095211, dated 10 / 17 / 2025, page 21 / 112 12 / 102 hydroxyalkanoate. In some embodiments, the existing matrix comprises a petroleum-derived polymer, which may be derived from a recycled plastic material. In some embodiments, the barrier formulation comprises a substance selected from the group consisting of cellulosic polymers, lipids, proteins, diluents, fatty acids, a resin acid, and combinations of resin acids. In certain aspects, the NCE-containing material comprises a barrier substance, and the barrier substance is selected from the group consisting of cellulosic polymers, lipids, proteins, diluents, fatty acids, a resin acid, and combinations of resin acids.In certain embodiments, the barrier formulation comprises an oleophobic substance selected from the group consisting of MC, HPMC, CMC, NaCMC, CA, CAB, chitosan, rosin, lignin, and a vegetable protein; in other embodiments, the barrier formulation comprises a hydrophobic substance selected from the group consisting of MC, CA, CAB, chitosan, rosin, hydrophobized starch, lignin, and a vegetable protein. In certain additional embodiments, the barrier substance is an oleophobic substance selected from the group consisting of MC, HPMC, CMC, NaCMC, CA, CAB, chitosan, rosin, lignin, and a vegetable protein; in other embodiments, the barrier substance is a hydrophobic substance selected from the group consisting of MC, CA, CAB, chitosan, rosin, hydrophobized starch, lignin, and a vegetable protein. In certain embodiments, the barrier formulation comprises a resin acid or a combination of resin acids.In some embodiments, the NCE-containing material additionally comprises one or more additive substances selected from a bulking agent, a reinforcing agent, or an appearance-modifying agent. In certain embodiments, one or more additive substances produce a selected property in the NCE-containing composite material. Petition 870250095211, dated 10 / 17 / 2025, page 22 / 112 13 / 102 from the group consisting of structural strength, resilience, elasticity, water resistance, and oil and grease resistance. Furthermore, plastic substrates comprising these NCE-containing composite materials are disclosed in the present invention, as well as manufactured articles comprising such plastic substrates shaped into formed articles, such as transaction cards, liquid containers, food containers, food utensils, packaging materials for consumer goods, films and thin sheets, and hollow cylinders for flexible tubing.

[018] Also disclosed in the present invention are methods for manufacturing a plastic article comprising a composite material containing NCE in a flexible state, comprising: (a) producing a composite material containing NCE comprising redispersible NC elements, wherein the NCE-containing composite material is produced by the substeps of (i) providing an initial suspension comprising NC elements suspended in a fluid medium; (ii) combining a drying / dispersing additive with the initial suspension to form a flexible suspension of redispersible NCEs; for example, the drying / dispersing additive comprises an LCST polymer; (iii) integrating the flexible suspension into an existing matrix, thereby forming a composite matrix containing NCE in the flexible state;(iv) add an additive substance and retain the flexibility of at least one of the initial suspension, the flexible suspension, the existing matrix, and the NCE-containing composite matrix, thereby forming the NCE-containing composite material in the flexible state; and (b) form or mold the NCE-containing composite material in the flexible state into a desired configuration, thereby manufacturing the formed article. The additive substance may be selected from the group consisting of reinforcing agents, barrier formulations, barrier substances, and bulking agents. In some embodiments, the forming step; Petition 870250095211, dated 10 / 17 / 2025, page 23 / 112 14 / 102 or formatting includes extrusion. BRIEF DESCRIPTION OF THE FIGURES

[019] FIG. 1 is a block diagram showing a process for producing matrices comprising redispersed nanocellulose elements.

[020] FIG. 2 is a block diagram showing a process for producing matrices comprising redispersed nanocellulose elements.

[021] FIG. 3 is a block diagram showing a process for producing matrices comprising redispersed nanocellulose elements. DETAILED DESCRIPTION OF THE INVENTION 1. Components of redispersible nanocellulose element formulations a. Generally redispersible nanocellulose elements

[022] It has been unexpectedly discovered that nanocellulose elements (NCEs) can be treated so that they can be redispersed in formulations to produce useful articles of manufacture, using formulations and methods as set forth in the present invention and as set forth in U.S. Patent Application Publication No. 20220412010A1 (U.S. Patent Application No. 17 / 834,521 filed June 7, 2022; the '521' Application), the contents of which are incorporated by reference in the present invention in their entirety. Using these inventive methods, formulations containing NCEs can be prepared, which can be concentrated or dried and then redispersed without hornification. Such formulations comprising redispersed NCEs can then be employed for the manufacture of useful articles.The formulations themselves can be dried and formed to produce manufactured articles, or they can be integrated into existing matrices to form composites with improved properties compared to the existing matrix itself, or that have additional properties not present in the existing matrix. Petition 870250095211, dated 10 / 17 / 2025, page 24 / 112 15 / 102

[023] Suitable substrates for treatment with the systems and methods disclosed in the present invention (i.e., NFCs and MFCs, and NCCs and MCCs, collectively NCEs) can be derived from all types of cellulosic feedstocks, in particular from plant-derived cellulosic feedstocks. Plant-derived cellulosic feedstocks comprise lignocellulosic materials: lignocellulosic materials are composed of cellulose polymers linked together with varying amounts of lignin. Lignocellulosic materials of all types are suitable for producing NCEs or other lignocellulosic materials, such as cellulose. The plants used as lignocellulosic materials can be woody (such as trees, with firm stems and multi-year growth cycles) or non-woody, with weak stems and annual or limited multi-year growth cycles.Lignocellulosic materials can include specialty crops, such as sorghum and elephant grass, grown for use as biofuels, capable of multiple harvests. Useful materials for cellulose production can be derived, without limitation, from industries such as agriculture (for example, corn straw and corn cobs, sugarcane bagasse, straw, empty palm fruit bunches, pineapple leaves, apple stalks, coconut fiber, mulberry bark, rice husks, bean husks, soybean hulls (or soybean shells), cotton linters, blue agave residues, North African glass, banana pseudostem residues, peanut shells, pistachio shells, grape pomace, shea nut shells, passion fruit peels, fique fiber residues, sago seed husks, algae residues, rush plant stems, and the like), or forestry (sawmill and paper mill waste).

[024] In the various forms, NCEs are conventionally produced from lignocellulosic precursor materials or other cellulosic raw materials of plant origin, through a series of procedures. Petition 870250095211, dated 10 / 17 / 2025, p. 25 / 112 16 / 102 Mechanical and / or chemical processes are carried out in an aqueous medium, in which the aqueous suspension loosens the interfibrillar hydrogen bonds of cellulose to facilitate delamination, resulting in the formation of NCEs. NFCs and MFCs are extracted from plant matter using different techniques, so their morphologies and properties differ. NFCs and MFCs can be differentiated based on their size and shape: cellulose nanofibers have a much smaller diameter than cellulose microfibers and can be straight or rod-shaped, while cellulose microfibers have a larger diameter, are more flexible, and have a more varied and irregular appearance. Although the literature cites a variety of dimensions for NFCs and MFCs, NFC fibers are nanoscale (e.g., have a diameter between 4 and 20 nm), while MFCs can be much larger, although they typically still have nanoscale diameters, e.g., 20 to 100 nm or more.After NCEs are formed from the precursor cellulosic material, they are dispersed in an aqueous medium at low concentrations (<10% by weight) because their high water absorption capacity and tendency to hydrogen bond cause them to form a highly viscous suspension even at low solids concentrations due to hydrogen bonding-induced entanglement of the high aspect ratio NC elements, as described above.

[025] Additives have been discovered, as described in Application '521, which can be used to prepare NCEs so that they are redispersible after being formulated in solutions. These additives are referred to in the present invention as “drying / dispersion additives”. Without delving into theory, these additives function to inhibit or disrupt the hydrogen bonding of NCEs to each other at specific, generally elevated, reaction temperatures, thus preventing consolidation and hornification, while retaining their high intrinsic hydrophilicity which allows easy redispersion in aqueous media. Petition 870250095211, dated 10 / 17 / 2025, page 26 / 112 17 / 102 As used in the present invention, the term redispersion and its grammatical derivatives and related terms refer to a process whereby dry or concentrated NCEs, prepared to be redispersible as described in the present invention, are suspended in a fluid medium (aqueous or non-aqueous), called the resuspension fluid, such that there is a substantially complete dissolution of the dry or concentrated NCE suspension to release its NCE components as resuspended in the resuspension fluid. In some embodiments, aqueous resuspension fluids may be used; in other embodiments, non-aqueous resuspension fluids may be used, such as fluids with hydrophobic or amphiphilic properties.

[026] As used in the present invention, the term redispersible refers to NCEs that have been treated with a drying / dispersing additive as disclosed in the present invention, a treatment that renders the NCEs capable of redispersion. Formulations containing such redispersible NCEs may exist in a liquid, dry, or partially dry state. In a fully dry or partially dry state, the NCEs in the formulation are capable of redispersion by means of suspension in a resuspension fluid. The redispersible NCEs (i.e., NCEs treated with drying / dispersing additives, as disclosed in the present invention) may be contained in liquid formulations before being dried; the presence of the drying / dispersing additives renders such NCEs redispersible, so that they may undergo subsequent redispersion if dried or concentrated.Redispersible NCEs also exist in liquids formed by adding a resuspended fluid to a dry or concentrated formulation containing redispersible NCEs; their resuspended presence in such a liquid demonstrates that they are, in fact, capable of redispersion and are therefore redispersible. To avoid any doubt, this latter group of redispersible NCEs, which... Petition 870250095211, dated 10 / 17 / 2025, page 27 / 112 18 / 102 are formulated to be redispersible and have been resuspended in a resuspension fluid that makes them effectively redispersed; they can also be more specifically termed “redispersed NCEs”; all redispersed cellulosic nanofibers (CNFs) are, by definition, redispersible, but not all redispersible NFCs are redispersed.

[027] In some embodiments, the redispersion results in a suspension of the NCEs such that they are formed as individual NCEs or amorphous coalescences of individual NCEs (both being referred to in the present invention as “resuspended particles”), wherein such resuspended particles have an aspect ratio greater than 10. In some embodiments, the resuspended particles have an aspect ratio between about 10 and about 300, or between about 10 and about 200. In some embodiments, the resuspended particles have an aspect ratio between about 50 and about 150. In some embodiments, the resuspended particles have an aspect ratio between about 25 and about 75. In other embodiments, the resuspended particles have an aspect ratio between about 75 and about 125.

[028] These formulations and methods include several different categories of drying / dispersing additives: (1) certain temperature-responsive polymers that can introduce spacing between NC elements during drying, thus preventing their agglomeration; (2) certain small volatile molecules that can create space between NC elements during drying; and (3) certain small or large non-volatile molecules (“blocking agents”) that prevent hydrogen bonding between or between NC elements during drying. Drying / dispersing additives comprise, without limitation, temperature-responsive polymers, small molecule additives in volatile systems, and blocking agents. All these materials act by disrupting hydrogen bonds at elevated temperatures or at Petition 870250095211, dated 10 / 17 / 2025, page 28 / 112 19 / 102 other circumstances, while creating gaps between the NC elements with additional drying, which will allow subsequent redispersion.

[029] Although certain additives (for example, certain LCST polymers, as described below) are suitable for use as single agents to facilitate drying and redispersion, other additives lend themselves to use as adjuvants in combination with a main drying / dispersion additive, either when administered to the initial NC suspension simultaneously with the main additive, or when administered as a pretreatment to the initial NC suspension or any precursor thereof before adding the main additive, or when administered as a posttreatment to the initial NC suspension after the addition of the main drying / dispersion additive. b. Drying / dispersion additives

[030] It is understood that the drying / dispersing additives disclosed in the present invention can be introduced into the initial suspension containing NCEs individually or in combination to improve the drying process of the NCEs and facilitate their redispersion. The drying / dispersing additives can also be used in combination with other agents that enhance their effectiveness, even if these other agents are not effective as drying / dispersing additives when used alone; such agents, used in combination with the drying / dispersing additives to enhance their effectiveness, are called adjuvants. It is further understood that one or more drying / dispersing additives and / or adjuvants can act together synergistically.Furthermore, combinations of drying / dispersing additives can be introduced sequentially during the preparation of the initial NC suspension and / or before, after, or during the processes employed to produce the initial NC suspension from a cellulosic source feedstock. Petition 870250095211, dated 10 / 17 / 2025, page 29 / 112 20 / 102 or without the addition of adjuvants. For example, non-polymeric additives can be added during the processes used to produce the initial NC suspension from the raw material, but preferably they should be added after the chemical pretreatment of the initial NCEs derived from the cellulosic or lignocellulosic precursor material. i. Temperature-responsive polymers

[031] In some embodiments, certain temperature-responsive polymers can be employed to create space between NC elements during drying, thereby preventing the NC elements from aggregating during the drying process. By preventing dense aggregation and consolidation of the NCEs, the temperature-sensitive polymer allows them to be redispersed upon contact with the resuspension fluid. Temperature-responsive polymers particularly suitable for this purpose are those exhibiting a phenomenon known as LCST (lower critical solution temperature) phase behavior. It is understood that certain LCST polymers are hydrophilic below their LCST transition temperature and become reversibly hydrophobic above their LCST transition temperatures. In other words, below the LCST point, the polymer shows high affinity for water, consistent with its intrinsic molecular hydrophilicity.However, above the LCST point, the polymer repels water and avoids hydrogen bonding. This is evidenced by the observed thermogelation of polymer solutions above this transition temperature. As the polymeric or oligomeric LCST additive self-assembles on the surface of the NC elements (in the form of a monolayer or a few molecular layers), the drying of the NC elements and the resulting morphology of the NC-containing material in the dry state are affected, so that the final redispersion of these NC elements is facilitated.

[032] For use in this scenario, the LCST polymer can be added to Petition 870250095211, dated 10 / 17 / 2025, page 30 / 112 21 / 102 Initial NC suspension at a temperature below the LCST polymer transition temperature. The initial NC suspension is then heated to effect its drying. As water evaporates from the initial NC suspension during drying, its temperature increases and approaches the boiling point of water, eventually exceeding the LCST polymer transition temperature, at which point the LCST polymer loses its hydrophilic character and becomes hydrophobic. When it becomes hydrophobic, the behavior of the LCST polymer changes: at this point, it interferes with the hydrogen bonds that would be forming between the NC elements. The hydrophobic nature of the LCST polymer now drives the aggregation or disaggregation of the NC elements, instead of these processes being driven by the interaction of the hydrophilic cellulosic units of the NC elements.

[033] In some embodiments, selected LCST polymers can significantly or completely hinder dense aggregation and consolidation of NC elements after drying. In some embodiments, the ability of selected LCST polymers to interrupt dense aggregation and consolidation of NC elements is independent of equipment selection and drying mode. For example, the suspension containing the LCST polymer and NC elements can be left quiescent during drying. A wide range of drying temperatures and pressures can be applied to the initial NC suspension in the presence of selected LCST polymers to achieve aggregate-free drying. Dried NC materials incorporating selected LCST polymers, as described in the present invention, can be easily redispersed in water with stirring or gentle agitation, with minimal or no coagulation, or residual dense aggregations or consolidations identified in the redispersed suspension.These characteristics allow for a wide latitude in the parameters for redispersion and for. Petition 870250095211, dated 10 / 17 / 2025, page 31 / 112 22 / 102 processing of redispersed material.

[034] In some embodiments, the list below offers examples of LCST polymers and their analogous short-chain oligomers that can be used as drying / dispersing additives to prevent dense aggregation and consolidation and thus facilitate subsequent redispersion of NC elements. • Methylcellulose • Carboxymethylcellulose • Sodium carboxymethylcellulose • Hydroxyethylcellulose • Hydroxypropylcellulose • Hydroxypropylmethylcellulose • Ethylhydroxyethylcellulose • Polyvinylcaprolactam • Poly(methyl vinyl ether) • Poly(N-isopropylacrylamide) • Poly(N,N-diethylacrylamide) • Poly(ethylene oxide) and poly(propylene oxide) block copolymer • Elastin poly(pentapeptide)

[035] Note that the thermogelling temperature of some of the additives listed above depends on the type and degree of substitution and can be adjusted by the structural design. Advantageously, an LCST polymer selected for use as a drying / dispersing additive can have a transition temperature higher than ambient temperature (e.g., > 25 °C), so that the polymer remains in solution until the drying step begins. Petition 870250095211, dated 10 / 17 / 2025, page 32 / 112 23 / 102 ii. Volatile small molecule additive systems

[036] In some embodiments, volatile systems comprising small molecule additives can be employed alone or in combination with other additives to act as drying / dispersing additives, creating space between the NC elements during drying and thus preventing the NC elements from aggregating during the drying process. Small molecule additives selected for use with volatile systems are miscible with water and have a higher boiling point than that of coexisting water. A useful small molecular additive in a volatile system is further characterized by its much lower tendency to hydrogen bond compared to water.As the volatile system loaded with additive containing the NCEs and the selected small molecule additive undergoes drying, water molecules preferentially evaporate, leaving the small molecule additive behind due to its higher boiling point, thus increasing the concentration of the additive in the remaining solution that remains between the adjacent NC elements. In some embodiments, the molecular segments of the volatile small molecule additives comprise both polar and nonpolar functionalities. Without adhering to theory, it is predicted that the polar segments are attracted to the cellulosic hydroxyl groups, while the nonpolar segments simultaneously interfere with the hydroxyl-hydroxyl interactions, thus reducing the adhesion between the NC elements. Then, as the temperature in the system increases, the additive evaporates, leaving behind the NC elements surrounded by air and therefore separated from each other.The resulting dry material, containing NC elements that are separated from each other by air, can be easily redispersed without forming signs of aggregation or consolidation, such as observable clumps / clots or variations in concentration. The suspension. Petition 870250095211, dated 10 / 17 / 2025, page 33 / 112 24 / 102 redispersed comprises resuspended NC particles that are uniformly distributed within the suspension, where the NC elements retain their nanoscale characteristics and can achieve redispersion with only very gentle stirring / agitation.

[037] In some embodiments, the lists below offer examples of small molecule additives that can be used as drying / dispersing additives in the volatile systems mentioned to prevent dense aggregation and consolidation and thus facilitate the subsequent redispersion of NC elements. The exemplary additives can be divided into two categories: non-ionic and cationic compounds.

[038] Non-ionic candidates may include, without limitation: • Tri(propylene glycol) butyl ether (TPnB) • Di(propylene glycol) propyl ether (DPnP) • Propylene glycol butyl ether (PnB) • Propylene glycol propyl ether (PnP) • Ethylene glycol monobutyl ether • Propylene glycol monomethyl ether acetate • Propylene glycol diacetate • Ethylene glycol diacetate • Benzyl alcohol • 1-Heptanol • 1-Hexanol.

[039] Cationic candidates may include, without limitation: • Ethylenediamine • Diethylenetriamine • Tetraethylene pentaamine • 1,3-Pentanediamine Petition 870250095211, dated 10 / 17 / 2025, page 34 / 112 25 / 102 • Piperazine • 1,2-Cyclohexane diamine • Aniline • Pyridine • Piperazine.

[040] In some embodiments, small molecule additives can completely evaporate from the initial NC suspension, leaving only the NC elements in suspension or in dry form, without additive residue. However, in other embodiments, traces of small molecule additives may remain. For example, with certain cationic additives, their cationic groups can adhere to cellulose molecules, so that traces of the additive remain attached to the cellulose after complete drying. For most industrial applications, residual residues of these additives do not represent a health or environmental problem. However, in some embodiments, a small biodegradable cationic molecule, such as 1,3-pentanediamine, can be selected to avoid such problems. iii. Blocking agents

[041] In some embodiments, small or large non-volatile molecular additives can be employed, in addition to volatile systems as described above, to hinder hydrogen bonding and / or create space between NC elements during drying, thereby blocking interactions between NC elements and thus preventing NC elements from aggregating during the drying process. In some embodiments, surface-functionalized nanometric particles can be employed in the same way. These small or large non-volatile molecular additives and nanoscale particles employed to perform this blocking function are referred to in the present invention as blocking agents or blockers. Petition 870250095211, dated 10 / 17 / 2025, page 35 / 112 26 / 102 As used in the present invention, the term "blocking agent" or blocker includes any non-volatile chemical additive or nanoscale particulate material that, by itself, prevents hydrogen bonding or creates spaces between NC elements, regardless of whether the substance is interposed between or among NC elements, or whether the substance offers temporary competitive binding sites for NC elements, or otherwise.

[042] As an example, caffeine and other xanthine derivatives are small molecule blockers that can be advantageously used to facilitate the isolation of NC elements from each other during a drying or concentration process and their subsequent redispersion. Without adhering to theory, it is predicted that the aromatic nitrogen atoms in certain purines (such as caffeine and other xanthines or xanthine derivatives) and pyrimidines can become hydrogen bonded to the hydroxyl groups of cellulose, presenting a flat, relatively nonpolar, molecularly lubricating and water-filtering outer surface for the NCEs, thus hindering adhesion between NC elements. Caffeine and other xanthines and xanthine derivatives can normally be used in amounts that do not present health or environmental problems, even when used in dosages sufficient to facilitate NC dispersion.

[043] As another example, certain humectant substances can be employed as blocking molecules. Humectants possess multiple hydrophilic sites, such as hydroxyls, esters, and ammonium groups, which can form hydrogen bonds with the surface of NC elements, thus filtering the interaction of these elements with each other through hydrogen bonds and thus hindering dense aggregation and consolidation. In addition, these hygroscopic substances are biocompatible and are already widely used in the pharmaceutical, cosmetic, and food industries. Exemplary candidates for humectants Petition 870250095211, dated 10 / 17 / 2025, page 36 / 112 27 / 102 short and long versions include, but are not limited to, glycerin, caprylyl glycol, ethylhexylglycerin, tribeenin, hydrolyzed soy protein, various amino acids, propylene glycol, methyl gluceth-20, phenyl trimethicone, hyaluronic acid, sorbitol, and gelatin.

[044] As another example, fatty acids can also be employed as blockers. Fatty acids contain hydrophilic sites and a hydrophobic tail. The hydrophilic site can form hydrogen bonds with the surface of NC elements, thus preventing the interaction of these elements with each other through hydrogen bonding, thereby hindering aggregation. Preferably, fatty acids that do not contain so many hydrophilic sites that excessive hydrogen bonding occurs between the NCE particles and the fatty acids can be selected. However, in embodiments where many hydrogen sites can cause dense aggregation and consolidation, the hydrophobic tail of fatty acid blockers can act to physically prevent dense aggregation and consolidation of NC elements by preventing or interfering with hydrogen bonding.In some embodiments, the blocking agent may be a fatty acid, such as stearic acid, palmitic acid, myristic acid, lauric acid, capric acid, caprylic acid, caproic acid, and the like. To facilitate the dispersion of the fatty acid in aqueous solutions of NC elements, a water-soluble fatty acid may be selected. 2. Redispersible and redispersed suspensions of NC elements

[045] The block diagram in FIG. 1 schematically represents the 100 processes involved in the preparation of redispersible suspensions of NC elements that can be further processed to produce redispersed suspensions of NC elements and materials made from them. As shown in FIG. 1, the 100 processes for producing a Petition 870250095211, dated 10 / 17 / 2025, p. 37 / 112 28 / 102 suspension of redispersed NC elements involves four steps.

[046] Step 1 suspends a population of NCEs 102 in a suspension fluid 104 to produce the initial NCE suspension 108. The processes for forming initial NCE suspensions suitable for further processing using the formulations and methods disclosed in the present invention are familiar in the art. To form a suspension containing NCEs, cellulose sources can be processed using conventional mechanical techniques and optional chemical treatments to extract the component cellulosic nanomaterials (i.e., the NCEs) and retain them suspended in a liquid or other fluid medium. The NC elements thus extracted form the initial NC suspension, which can be treated to make them redispersible in the next step, using the formulations and methods disclosed.

[047] In Step 2, a drying / dispersing additive 110, as described above, is added to the initial NCE suspension 108, to produce a redispersible NCE suspension 112. As discussed previously, the drying / dispersing additive 110 enables the NCEs in the initial NCE suspension 108 to be redispersible. The redispersible NCE suspension 112 is dried in Step 3, to produce a dry material 114 containing redispersible NCEs. The dry material 114 containing the redispersible NCEs is then milled / ground and used as a dry ingredient, or suspended in a resuspension fluid 118 in Step 4, to produce a suspension 120 of the desired concentration of the redispersible NCEs produced as described above; such redispersible NCEs treated by suspension in a resuspension fluid as set forth in Step 4 may also be referred to as “redispersed NCEs”.In some embodiments, the suspension 120 of redispersed NCEs can then be processed on its own, for example, by drying or concentration, as shown in Step 5a, to form a simple NCE-based matrix 122. Petition 870250095211, dated 10 / 17 / 2025, p. 38 / 112 29 / 102 Dry and redispersed NCEs are formed as a continuous sheet. At the microscopic level, the structure is three-dimensional, highly porous, and typically forms a structurally amorphous network; however, semi-crystalline NCE matrices can be synthesized if nanocrystalline elements are used and / or crosslinking strategies, such as grafting and esterification of carboxylic acids on the surface of NCEs, are employed. As used in the present invention, the term amorphous refers to any solid formation in which the components are not organized in a defined and repetitive network pattern. Amorphous structures generally enhance degradability. Furthermore, additive substances (not shown) can be easily incorporated into the simple amorphous NCE-based matrix to produce advantageous characteristics such as malleability, workability, heat tolerance, strength, or oleophobic or hydrophobic properties.

[048] Pulp-based or pulp-containing additives that do not contain NCEs may also be added in order to reduce the amount of NCEs required to produce the desired properties for the matrix. As used in the present invention, the term cellulose-based refers to materials that have been derived from cellulose through processing, forming or treatment, while retaining the cellulose or cellulose derivatives in their substance.

[049] Cellulose is understood to be the manufacture of materials containing cellulose or lignocellulosic fibers, such as wood, non-wood raw materials, specialty crops, waste paper, recycled paper, agricultural waste and the like. Non-wood raw materials such as bagasse, cereal straw, bamboo, rushes, esparto grass, jute, flax and sisal are known in the art as sources of cellulose fibers; certain non-limiting examples of materials containing lignocellulosic fibers are also provided in the present invention. Wood and other plant materials used to make cellulose Petition 870250095211, dated 10 / 17 / 2025, page 39 / 112 30 / 102 contains three main non-aqueous components: cellulose, lignin, and hemicellulose. The chemical and / or mechanical processes for pulp production aim to break down the overall structure of the plant material source into constituent fibers, thus producing the fibrous material containing cellulose known in the art as pulp. Cellulose can also be formed from previously processed materials, such as used or recycled paper or certain fabrics; these materials may not have some or all of the components found in wood or other cellulose materials, but can be subjected to suitable chemical or mechanical processes to transform them into cellulose.

[050] Pulp and pulp-based materials can be used with the formulations, compositions, and methods disclosed in the present invention to be formed or shaped as components or substrates for manufactured articles in any useful shape, such as sheets, fibers, solid articles, molded articles, etc. These additives can act as low-cost bulking agents to add volume to the matrix so that a larger quantity of simple NCE-based matrix is ​​produced; in such a matrix, the redispersible or redispersed NCEs are added in combination with the bulking agent (e.g., conventional pulp or other pulp-based substance) so that the final matrix has the desired mechanical properties.

[051] Although NCEs are understood as additive substances responsible for matrix organization and architectural characteristics with resulting performance attributes, other additives may be added to the matrix to produce advantageous characteristics, as described above, or other desirable properties. For example, appearance-modifying additives, such as pigments or other color-producing agents, may be added to the matrix, or other additives intended to provide properties. Petition 870250095211, dated 10 / 17 / 2025, page 40 / 112 31 / 102 desirable, for example, odor-related agents, emollients, cosmetics, pharmaceuticals, medical products and agricultural active ingredients, fragrances and aromas, and the like. Other related additives may be included in the matrix to enable a specific additive to fulfill its intended purpose. For example, an NCE matrix may include odor-blocking chemicals or natural aromas adapted for release in enclosed locations that have high levels of odorous materials, for example, in items such as gym bags, suitcases, etc., or adapted for use in personal items that are likely to be odorous (e.g., insoles or shoe protectors).An NCE matrix adapted for these purposes may incorporate plasticizers or other additives to adjust the release of odor-controlling agents or to adapt their release to certain environmental conditions (e.g., shoe linings that emit odor-controlling substances when in contact with feet at body temperature). Similarly, an NCE-based matrix may be formulated with deodorant or antiperspirant substances in the interstices of the matrix, with the NCE-based matrix serving to allow for a longer-lasting application of such products to the skin. As further examples, a variety of scents may be employed with the systems disclosed in the present invention. The term scent, as used in the present invention, refers to the variety of odors that may be deliberately incorporated and provided by the matrices as described in the present invention.For example, pleasant aromas can be used for cosmetic or aesthetic purposes, or to mask unpleasant odors. Aromas can be used for medical, veterinary, or agricultural purposes, to act as insect repellents, pesticides, pheromones, growth hormones, or similar substances. Aromas can be obtained from volatile aromatic compounds, such as essential oils, hydrosols, etc. Petition 870250095211, dated 10 / 17 / 2025, page 41 / 112 32 / 102 perfume microcapsules, etc. Exemplary sources may incorporate biological oils and chemical sources suspended in solution for easy application or mixing. Other aroma sources may be water-based, such as hydrosols. Other examples of aroma-based technologies based on the formulations disclosed in the present invention include, without limitation, insecticides for the agricultural sector, perfumes and odor neutralizers for domestic use, and hormones for pets to encourage calm behavior at home. By controlling the release rate through careful manipulation of the underlying technology, applications can be customized to various consumer needs, for example, for agricultural products that release pesticides rapidly during planting season and more slowly when plants are fully grown.The technologies disclosed in the present invention can be easily adapted for agricultural purposes, for example, with the use of pheromones as agricultural active ingredients. Pheromones are understood to be secreted or excreted chemical substances that trigger a social response in members of the same species. Although they may not possess “odors,” as the term is commonly understood, pheromone receptors are normally located in the olfactory epithelium or vomeronasal organ, indicating that they are processed by pathways similar to conventional ones. Pheromones are therefore considered odor-related active agents for the purposes of the present disclosure; they are known to be useful in the agricultural industry as pesticides or artificial growth hormones. The foregoing examples are intended to be illustrative and not limiting.Other examples of additive substances that are useful with the matrices disclosed in the present invention can be easily visualized by those skilled in the art.

[052] Addictive substances may be incorporated or added to Petition 870250095211, dated 10 / 17 / 2025, p. 42 / 112 33 / 102 Simple matrix based on NCE 122 before, during or after processing of Step 5a: the additive substance(s) may be added to the suspension 120 of redispersed NCEs before processing Step 5a and / or may be added as the suspension 120 is dried or concentrated and / or may be added to the simple matrix based on NCE 122. A material comprising the simple matrix based on NCE 122, wherein the simple matrix based on NCE 122 provides the architectural structure for the material and which further comprises any additive substances may be termed an “NCE-based simple material”.When the term “matrix” is employed in the present invention, as in “simple NCE-based matrix,” it is understood that the matrix-forming process described above need not produce a single continuous simple NCE-based matrix, but may instead produce a plurality of simple NCE-based matrices that are more loosely connected to each other or are discontinuous. If a plurality of simple NCE-based matrices is produced by the processes as disclosed in the present invention, the interrelationship of the matrices thus formed provides organization and architecture that can be transferred to the final simple NCE-based material. More specifically, the NCEs, when redispersed, can form tangles or connections with each other that constitute one or more matrices. Physically mixing the liquid formulation comprising the redispersed NCEs can fragment one or more matrices into smaller matrices that associate more freely with each other.This association of smaller matrices can provide the desired structural stability for the plain NCE-based material. This arrangement is compatible with the addition of pulp or pulp-based substances that can act as bulking agents, diluents, and the like. The architecture of the plain NCE-based matrix allows the pulp or pulp-based material to be integrated into the overall matrix without substantially impairing its strength. Petition 870250095211, dated 10 / 17 / 2025, p. 43 / 112 34 / 102 stability and / or durability.

[053] In other embodiments, the suspension 120 can be added to another existing matrix 124, as shown in Step 5b, to form a composite matrix containing NCE 128. The NCEs redispersed in the suspension 120 can be termed “additive NCEs” when they are used in Step 5b to be added to the existing matrix 124. In some embodiments, the existing matrix 124 provides the architectural structure for the NCE-containing composite matrix, while the NCEs are integrated into the NCE-containing composite matrix 128. An existing matrix 124 can provide an amorphous host matrix, or it can produce a more discernibly ordered pattern of atoms or molecules in a regular, lattice-like matrix, as can be seen in a crystal. In the NCE-containing composite matrix 128, the NCEs are intercalated into the existing matrix 124 to form the NCE-containing composite matrix 128.The more additive NCEs the composite matrix containing NCE 128 contains, the more properties the NCE 128-containing composite material will exhibit attributable to the NCEs. For example, a formulation comprising additive NCEs and a pulp-based bulking agent can provide significant strength to an NCE 128-containing composite matrix, while the presence of the pulp-based bulking agent adds volume to the NCE 128-containing composite matrix, potentially making it cheaper to produce. Other properties of the NCE 128-containing composite matrix may be provided by the existing matrix 124 alone or in interaction with any structural organization or other properties provided by the additive NCEs.

[054] In some embodiments, other additive substances may be included in the composite matrix containing NCE to add or improve desirable characteristics such as malleability, workability, heat tolerance, strength, or oleophobic or hydrophobic properties. Such substances Petition 870250095211, dated 10 / 17 / 2025, page 44 / 112 35 / 102 Additives may become available or added to the composite matrix containing NCE 128 before, during, or after the population of redispersed NCEs from the suspension 120 is added to the existing matrix 124. In some embodiments, the existing matrix 124 already includes some or all of the desired additive substances, and their presence is transferred to the composite matrix 128 containing NCE. In other embodiments, the additive substances are included when the redispersed NCEs and the existing matrix 124 are combined in Step 5b to form the composite matrix containing NCE 128. In other embodiments, the additive substances may be introduced into the composite matrix containing NCE 128 after its formation. The composite matrix containing NCE 128 with its included additive substances provides a material that can be further processed, shaped, or otherwise transformed into manufactured articles.A material comprising a composite matrix containing NCE 128, wherein the NCE-containing composite matrix provides the architectural structure for the material and further comprises any additive substances, may be termed an NCE-containing composite material.

[055] Both the simple NCE-based matrix 122 and the composite matrix containing NCE 128 can be used to provide an architectural framework for materials comprising redispersed NCEs, as shown in this Figure, wherein such materials can be formed or shaped to produce manufactured articles. In other embodiments not represented in this Figure, a simple NCE-based matrix or a composite matrix containing NCE can be used to provide an architectural framework for materials comprising redispersible NCEs. 3. Redispersible and redispersed nanocellulose elements on plastic substrates for the production of manufactured articles.

[056] As described above, redispersible NC elements or Petition 870250095211, dated 10 / 17 / 2025, page 45 / 112 36 / 102 redispersed materials produced according to the systems and methods disclosed in the present invention can be included in matrices that are used to form NCE-containing materials, either as components of simple NCE-based materials formed solely or predominantly of redispersible or redispersed NCEs without including another existing matrix, or as components of NCE-containing composite materials comprising an NCE-containing composite matrix having redispersible or redispersed NCEs interspersed in an existing matrix. Both simple NCE-based materials and NCE-containing composite materials can be employed as plastic substrates or as components of plastic substrates that can be transformed into other manufactured articles.As used in the present invention, the term "plastic" refers to a material that incorporates a three-dimensional structure (or "matrix") and retains flexibility, thus producing an NCE-based or NCE-containing material in a flexible state. This plastic material can be formed or shaped from its flexible state to a desired configuration and can further be fixed in the desired configuration so that the configuration is maintained for a designated period. The process of shaping or forming the material from its flexible state to the desired configuration can be carried out by many techniques known in the field, such as extrusion, calendering, injection molding, thermoforming, blow molding, and the like. The process of fixing the material in the desired configuration can also be carried out by many techniques known in the field, such as heating, application of prolonged pressure, and / or incorporation of additives that allow hardening, fixing, or curing.The designated period for maintaining the material in the desired configuration will be determined based on the intended use of the manufactured article and the intended use of the manufactured article itself (e.g., temporary use versus relatively permanent use) and on... Petition 870250095211, dated 10 / 17 / 2025, page 46 / 112 37 / 102 intended processes for the disposal of the material and the manufactured article at the end of its useful life. a. Simple materials based on NCE

[057] NCE-based simple materials can be used as plastic substrates for forming articles with a variety of shapes, with the mechanical properties of these formed articles being due, at least in part, to the structural arrangement provided by the matrix of dry, redispersible or redispersed NCEs that is an integral part of the NCE-based simple material. NCE-based simple materials can therefore be used to form articles that have advantageous mechanical properties such as strength and stability, but which are also designed to be dissolvable or degradable at a time appropriate for consumer use. Such articles are anticipated to have a relatively temporary lifespan and can be disposed of through biodegradation or composting.

[058] For example, this combination of mechanical properties and dissolubility / degradability allows containers to be constructed from materials that have sufficient durability to retain their contents during consumer use, but which are, in addition, susceptible to decomposition at the end of their intended useful life. As used in the present invention, the term “container” should be interpreted broadly, referring to any receptacle, reservoir or partial or complete enclosure that can be employed in connection with an item or product to contain, dispense, distribute, segregate, suspend, structure, package, store or portion said item or product, or to provide similar functionalities derived from the partial or complete enclosure of said item or product within. Exemplary containers include receptacles, reservoirs or Petition 870250095211, dated 10 / 17 / 2025, page 47 / 112 38 / 102 Containers of all shapes and geometries, whether rigid or flexible, and intended for temporary or durable use. Non-limiting examples include cylindrical containers such as bottles, jars, cups, straws, barrels, cans, drums, tubs and the like; straight containers such as boxes, crates, cardboard boxes, cases and the like; flat receptacles such as plates, trays, dishes, lids, supports and the like; and dispensing systems such as tablet capsules or soluble foams that distribute a pharmaceutical, agricultural or other active agent to a target area for application, protection or treatment. Advantageously, containers may provide protection against shock, impact and mechanical damage, and against elements of the external environment such as weather and pests and microbes; in addition, containers may provide protection against the ingress of oil, grease and water and against leakage of fluids exuded by the contained product.For these reasons, containers are particularly useful for protecting food products.

[059] This combination of mechanical and decomposability properties also allows containers to be constructed from simple NCE-based materials for deliberately ephemeral purposes, such as a container for a fertilizer or agricultural product that must decompose in a very short period of time to release the product into the environment. This combination of properties also allows containers to be constructed for rapid or immediate dissolution upon contact with water, for example, to provide active agents for laundry or other household care purposes. Simple NCE-based materials, whose architecture is based solely on the three-dimensional arrangement of NCEs, are entirely bio-based, as they are formed from NC elements. Thus, they offer important alternatives to petroleum-derived formulations used to produce conventional manufactured articles. Petition 870250095211, dated 10 / 17 / 2025, page 48 / 112 39 / 102 used for similar purposes and provide a vehicle for engineering a combination of mechanical properties and solubility that are consistent with the specific purpose of the article.

[060] A significant limitation to the use of plain NCE-based materials is their vulnerability to oil, grease, and water: plain NCE-based materials are substantially made of NCEs in combination with other, generally cheaper, diluent materials such as pulp and pulp-derived substances, which tend to offer little intrinsic resistance to the entry of water or oil / grease into and passage through the material. This vulnerability is exacerbated by the cost of the NCEs themselves: NCEs can be mixed with cheaper bulking agents or diluents to reduce the overall cost of an NCE-based material. Pulp or pulp-based substances are frequently employed for this purpose. However, this material, termed “pulp-dominant,” is especially susceptible to the effects of water and grease.In a predominantly pulp-based material, without any other treatment, exposure to water or oil / grease can lead to loss of structural strength or even loss of integrity of an article formed from these materials.

[061] As used in the present invention, the term “pulp-dominant” refers to a matrix or material in which pulp or a pulp-based material is present in sufficient quantities to have a substantial effect on the mechanical properties of the material. A predominantly pulp matrix may require additional NCE or other reinforcement to make it as strong, stable, or durable as a simple non-predominantly pulp NCE-based material, depending on the end use of the material; furthermore, such material may be treated with barrier formulations to make it resistant to the effects of water, oil, and grease, depending on the end use of the NCE-based material. Petition 870250095211, dated 10 / 17 / 2025, page 49 / 112 40 / 102 For example, a simple NCE-based material, predominantly pulp, can be used to form sheets for personal care items such as tissues or toilet paper without much or any additional reinforcement, whereas a similar material intended for use as paper towels may require more reinforcement, as its end use demands greater strength and resilience. A predominantly pulp material may also benefit from treatments to improve its oil and grease resistance and / or its water resistance, depending on the intended end use of such material.

[062] Simple NCE-based matrices can therefore be treated with formulations that impart oil and grease resistance (oleophobicity) and / or water resistance (hydrophobicity) to the matrix itself or to the materials that make up such matrices. Water resistance in a material is often measured by the water vapor transmission rate, which measures a material's water vapor permeability in units of gm / m2 / day, or g / 100 in2 / day; the term “water resistance” (WR) therefore includes both liquid water resistance and water vapor resistance. The properties of oil and grease resistance (OGR) and water resistance (WR, and collectively with OGR, “OGWR”) can therefore be integrated into the materials themselves or into articles formed from them.These OGWR properties can also be referred to as “barrier properties,” and a substance or formulation that produces barrier properties can be called a “barrier-producing formulation” or “barrier formulation.” A “barrier substance” refers to a substance that produces a barrier property. Both oil / grease resistance (or oleophobicity) and water resistance (or hydrophobicity) can individually be called barrier properties.

[063] Barrier properties can be adjusted in a material Petition 870250095211, dated 10 / 17 / 2025, page 50 / 112 41 / 102 simple containing NCE to allow differential permeability of the material to various fluids (whether oil, grease or water). As an example, in some embodiments, a barrier production formulation may impart OGR and WVR properties to the article it treats, with the relative strength of each property being adjustable by adjusting the ingredients selected for the formulation itself and / or by adjusting the relative amounts of its ingredients, for example, to emphasize hydrophobicity or oleophobicity.

[064] In some embodiments, NCEs alone or NCEs modified with barrier-producing substances such as lignin, wax, fatty acids and the like are able to impart a certain degree of oleophobicity or hydrophobicity to the plain NCE-based material, and their concentration can be adjusted to optimize this barrier property. Without being limited by theory, it is believed that the close packing of NCEs can enhance the barrier properties they provide. Furthermore, despite their intrinsic hydrophilicity, NCEs (alone or modified with barrier-producing substances) can, under certain circumstances, be sufficiently packed into plain NCE-based materials to impart water- or vapor-resistant barrier properties to these materials.

[065] In some embodiments, a wide range of additive ingredients can be combined to provide desired barrier properties. For example, a barrier production formulation suitable for use with simple NCE-based matrices may include a cellulose ether, such as methylcellulose, and / or a resin acid. Alternative cellulosic ingredients for the barrier production formulation may include, without limitation, CMC (carboxymethylcellulose), CMCNa (sodium carboxymethylcellulose salt), CA (cellulose acetate), CDA (cellulose diacetate), cellulose triacetate (CTA), CAB (cellulose acetate butyrate), CAPh (cellulose acetate phthalate), CAP Petition 870250095211, dated 10 / 17 / 2025, page 51 / 112 42 / 102 (cellulose acetate propionate), EC (ethylcellulose), HEC (hydroxyethylcellulose), EHEC (ethyl hydroxyethylcellulose), HPC (hydroxypropylcellulose), HPMC (hydroxypropylmethylcellulose), HPMCP (hydroxypropylmethylcellulose phthalate), HPMCAS (hydroxypropylmethylcellulose acetate). Methylcellulose is particularly advantageous in barrier formulations for simple NCE-based matrices due to its oil and grease resistance, high viscosity, and unique lower critical solution temperature (LCST), which causes it to gel when heated. Resin acids and combinations thereof (such as rosin, gum rosin, pitch, and the like) can be used alone or in conjunction with methylcellulose to provide water resistance. Cellulose acetates are also particularly advantageous ingredients in barrier formulations, especially for food and beverage containers, as they can produce both oleophobic and hydrophobic properties.

[066] In more detail, resin acids are bioderived gums that are sticky and insoluble in water in their native state, characterized as unsaturated diterpenecarboxylic acids with a phenanthrene ring structure, having the empirical formula C19H29COOH. Resin acids include abietic acid, palustric acid, levopimaric acid, neoabietic acid, dehydrogenated ibutodic acid, pimaric acid, isopimaric acid, and sandaracopimaric acid. They can be separated into two categories according to their chemical structural formulas: abietic-type resin acids and pimaric-type resin acids. The monomeric molecule of abietic-type resin acid has two conjugated double bonds and one isopropyl bond. Dehydrogenated abietic acid, abietic acid, palustric acid, and levopimaric acid are examples of abietic-type resins.The monomeric molecule of pimaric resins has a methyl and a vinyl group at the C13 position and possesses two independent double bonds. This type of structure is predominantly found in... Petition 870250095211, dated 10 / 17 / 2025, p. 52 / 112 43 / 102 pine-bearing resins and pine resin, such as pimaric acid, isopimaric acid, sandaracopimaric acid and pimaric resin acids.

[067] The carboxyl groups of resin acids can react with a polyol (e.g., glycerol, erythritol, etc.) to form esters (thus linking three or four resin acid molecules to create an oligomer of a basic resin acid building block, such as abietic acid). Resin acids tend to be glassy and rigid at room temperature. Depending on the plasticization, they can be softened by increasing the temperature and the amount of plasticizer used. Resin acids are compatible and miscible with a variety of oils / waxes to adjust thermal or physical properties (such as, but not limited to, glass transition temperature, ductility, and hydrophobicity). For example, beeswax and carnauba wax are soluble in certain resin acids, thus affecting the melting and glass transition temperatures, while decreasing their solubility in solvents.Other examples of oils and waxes suitable for mixing with resin acids include, but are not limited to: • Mineral oils and waxes (paraffins) • Beeswax • Carnauba wax • Linseed wax • Candelilla wax • Lard • Coconut oil • Linseed oil • Eucalyptus essential oil • Cocoa butter • Sweet almond oil Petition 870250095211, dated 10 / 17 / 2025, page 53 / 112 44 / 102 • Olive oil • Palm oil • Castor oil • Sunflower oil • Canola oil.

[068] The proportion of these ingredients in the barrier production formulation can be adjusted to optimize their OGR and WVR properties and thus design the desired amount of OGWR in the NCE-based plain material that is formed by adding the specific barrier production formulation to the NCE-containing plain matrix.

[069] The block diagram in FIG. 2 schematically illustrates how the barrier production formulation can be added during the formation of the simple NCE-based matrix and its subsequent processing. Process 200 in FIG. 2 begins with the supply of a dry material 202 containing redispersible NCEs, where such dry material has been prepared substantially as described in connection with Figure 2.1. The dry material 202 containing the redispersible NCEs is then milled / ground and used as a dry ingredient, or suspended in a resuspension fluid 204 to resuspend the NCEs in the dry material 202 and form a suspension 208 of the desired concentration of redispersed NCEs, substantially as described in connection with FIG. 1. The suspension 208 of redispersed NCEs is then subjected to drying 210 to produce the NCE-based simple matrix 212 which can then be used to form the NCE-based simple material, substantially as described in connection with FIG. 1.A barrier production formulation 214 can be added at points A, B, C, and / or D. More specifically, the barrier production formulation 214 can be added as part of step 206, in which the dry material 202 containing redispersible NCEs is treated with the fluid. Petition 870250095211, dated 10 / 17 / 2025, page 54 / 112 45 / 102 resuspension 204 to produce suspension 208 of redispersed NCEs. For example, barrier production formulation 214 can be added to redispersion fluid 204, as indicated by its introduction at point A. Barrier production formulation 214 can also be added to suspension 208 of redispersed NCEs, as indicated by its introduction at point B. Barrier production formulation 214 can also be added during the drying step 210, in which suspension 208 of redispersed NCEs is processed, to ultimately form the NCE-based plain material 212, as indicated by its introduction at point C. Finally, barrier production formulation can be added to the NCE-based plain material 212, as indicated by its introduction at point D.Although a single barrier production formulation 214 is represented in this Figure, it is understood that a plurality of barrier production formulations or barrier production formulation ingredients may be added at different points of introduction. A first barrier production formulation may be added at one point of introduction, and a second barrier production formulation may be added at a second point of introduction. Combinations of barrier production formulations and their ingredients may be introduced at any point during the process, using methods familiar in the art, such as (without limitation) mixing the formulations, spraying them onto or within the designated substrate, or painting them onto its surface.These barrier production formulations may include redispersed NCEs to enhance performance and act as pore-closers in their interaction with the surface of the existing NCE-containing material on which the coating is deposited. Barrier production formulations that do not contain redispersed NCEs may also be applied to provide enhanced performance. Petition 870250095211, dated 10 / 17 / 2025, page 55 / 112 46 / 102

[070] Examples of formulations for spraying onto or within substrates include the following:

[071] An exemplary formulation for producing an oil, grease and water resistant barrier, to be used as a coating (by weight, based on a total formulation weight of 100 g) includes: • Cellulose acetate butyrate (CAB): 10 g • Rosin: 10 g • Acetone: 79 g • Plasticizer (e.g., but not limited to, triacetin, triethyl citrate, acetyl triethyl citrate, tributyl citrate): 1 g. [ 072] An exemplary formulation for producing an oil, grease, and water-resistant barrier to be used as a coating (by weight, based on a total formulation weight of 100 g) includes: • Methylcellulose (MC): 3 g • Redispersed NCEs (NFC or MFC or combinations thereof): 1 g • Water: 54 g • Rosin: 4 g • Ethanol or Acetone: 38 g. [ 073] Where MC is solubilized in water and then combined with redispersed NCEs. Simultaneously, the resin is solubilized in ethanol or acetone. The two solutions can then be combined to produce an OGWR barrier. [ 074] An exemplary formulation for a hydrophobic coating includes the following ingredients combined to form a solution in acetone (by weight, based on the total weight of the 100 g formulation): • Cellulose acetate (CA): 3.5 g • Ethanol: 7 g Petition 870250095211, dated 10 / 17 / 2025, p. 56 / 112 47 / 102 • Acetone: 82.5 g • Rosin gum (GR): 7 g.

[075] An exemplary formulation for an oleophobic coating includes the following ingredients combined to form an aqueous solution in water (by weight, based on a total formulation weight of 100 g): • Methylcellulose (or any cellulose ether): 75 g • Redispersed NCEs (NFC or MFC or combinations thereof): 25 g.

[076] In more detail, an exemplary simple NCE-based material with OGWR properties can be produced as follows, with the barrier-producing formulation being added to a suspension of redispersible or redispersed NCEs. A suspension of redispersible (in this case, redispersed) NCEs is provided, prepared as discussed above, to which methylcellulose (MC) is added with or without a sugar alcohol plasticizer (glycerol, xylitol, maltitol, sorbitol, erythritol, mannitol, and the like). The addition of these ingredients aims to produce oleophobicity. The suspension of such redispersible or redispersed NCEs may contain NFCs, MFCs, or both. The suspension of such redispersible or redispersed NCEs may also include bulking agents, such as pulp or pulp-based ingredients, to provide more volume to the final simple NCE-based matrix and resulting materials.Separately, a rosin solution is prepared by mixing rosin in an alcohol or ketone solvent (e.g., ethanol or acetone) to obtain a 10-100% by weight (rosin weight / solvent weight) rosin solution in the solvent. After preparing this solution, with the resin properly dissolved, it can be emulsified in water using polyethylene glycol (PEG) at 125% by weight of the resin, preferably using an in-line homogenizer, or it can be mixed directly into the suspension containing redispersible or redispersed NCEs. A small amount. Petition 870250095211, dated 10 / 17 / 2025, page 57 / 112 48 / 102 of the solvent used to prepare the mixture can be added to the NCE suspension before the resin mixture is added to promote homogenization. The mixing process can occur vigorously, for example, by slowly pouring the resin-based formulation into the NCE-containing resuspension at medium to high shear, or by spraying as a fine mist in solution at relatively low shear, to nucleate a fine rosin suspension in the liquid phase throughout the MC-NCE-containing suspension. It is advantageous to add the rosin solution as a highly pressurized stream or to create a water-based emulsion so that the resin particle size is small. After combining these ingredients, the resulting mixture can be dried, producing the simple NCE-based matrix that can be processed to produce simple NCE-based materials.

[077] The addition of resin improves the hydrophobicity of the matrix. The effectiveness of rosin for hydrophobization can be increased by heat treating the rosin before dissolving it in the solvent, for example, by heating the rosin to about 200 °C for about 10 to 30 minutes to remove impurities such as turpentine. Heat treatment will also increase the softening point of the rosin from 45 °C to 59 °C, making it more resistant when subjected to heat during later stages of processing. In one embodiment, rosin may be loaded in an amount of about 35% by weight relative to the weight of the dry pulp, although amounts of rosin relative to the weight of the dry pulp ranging from about 1% by weight to about 50% by weight, about 1% by weight to about 10% by weight, about 8% by weight to about 25% by weight, about 20% by weight to about 40% by weight, or about 35% by weight to about 55% by weight may be employed.In one embodiment, the ratio of redispersible or redispersed NCEs to MC is approximately 1:3. Other NCE to MC ratios ranging from 5:1 to 1:3 may exist. Petition 870250095211, dated 10 / 17 / 2025, pp. 58 / 112 49 / 102 employees.

[078] A simple NCE-based matrix with OGWR properties can be produced by combining the ingredients as described above. This matrix can then be transformed into a simple NCE-based material that can be used to produce manufactured articles. To improve the retention of other additives in the simple NCE-based material, retention aids can be added to the simple NCE-based matrix. Retention aids, usually polymers or cationic surfactants, are familiar in the papermaking industry; for example, substances such as chitosan or PDADMAC can be used as retention aids.

[079] In exemplary embodiments, the OGR and WVR materials, as disclosed in the present invention, can be used as barrier production formulations with simple NCE-based materials, either as coatings to be applied to the surface of the material or as mixing additives. More specifically, the OGR and / or WVR formulations can be used as coatings or can be mixed with the simple NCE-based material, as described above, which can then be shaped (e.g., thermoformed) into a product.

[080] As an example, containers or parts of containers formed from simple NCE-based materials can be prepared with OGR and / or WVR properties, allowing the containers to safely confine and distribute wetted liquids, gels, or solids to the consumer for other purposes. These simple NCE-based materials may be predominantly pulp, with appropriate adjustments of NCE quantities and barrier production formulations based on the amount of pulp or pulp-based materials they contain. In some embodiments, the barrier production formulation may also be applied to the surface of the Petition 870250095211, dated 10 / 17 / 2025, pp. 59 / 112 50 / 102 plain NCE-based material before its forming or molding into the formed article, or the barrier production formulation may be applied to the formed article after forming or molding has occurred. For example, the barrier production formulation may be applied superficially to a precursor material or fabrication article using conventional application procedures such as painting or foil painting, curtain coating and the like, or spraying if the formulation has a viscosity compatible with the selected spraying apparatus. In other embodiments, the barrier production formulation may be integrated into the plain NCE-based formulation (as described above) at any concentration; then, before molding / thermoforming occurs, the mixture may be heated to slightly above the lower critical temperature of the LCST polymer component solution of the barrier production formulation.This procedure allows the LCST polymer dispersed in the mixture to precipitate (or agglutinate) onto the fibers or surface of the simple matrix structure containing NCE.

[081] In some embodiments, a bulking agent, such as pulp or a pulp-based material, may be added to the NCE-based plain matrix to form a predominantly pulp-based NCE plain material, as mentioned above. In such a material, the NCEs may interact with the pulp or with the pulp-based bulking agent, so that they coat or fill the pores between the pulp fibers or the fibers of the pulp-based material. In this capacity, the plain matrix or matrices formed within the NCE-based plain material may act as pore-closers to fill gaps in the pulp material. This pore-closure allows this type of NCE-based plain material to be used with cellulose or cellulose-based substances to form high-value specialty paper products with properties that reflect the behavior of the matrices. Petition 870250095211, dated 10 / 17 / 2025, pp. 60 / 112 51 / 102 NCE. For example, a paper product with NCE matrices incorporated into its pores can offer or improve oil and grease resistance (especially in conjunction with other barrier materials), since the incorporated NCE matrices close the pores within the paper substance that would otherwise allow grease to pass through the product. As another example, a paper product with NCEs incorporated into its pores can be designed to form a removable label backing or a selective adhesive. In some embodiments, barrier production formulations, as described above, can be added to the plain NCE-based material to enhance the effects of the NCE matrices as pore-closers, for example, imparting oleophobic or hydrophobic properties to the material, which can then be transferred to cellulose-predominant paper-type products made from it.

[082] In some embodiments, diluent particles can be added to NCE-based matrices and simple materials for bulk effect and / or to act as pore-closers. These diluent particles can be used in addition to or instead of barrier-producing formulations; in either case, the diluent particles can interact with cellulose fibers and simple NCE matrices to impart barrier properties such as oleophobicity and / or hydrophobicity; furthermore, the diluent particles can affect mechanical properties such as strength, toughness, flexibility, and elasticity.

[083] These diluent particles may include, without limitation, large or small particles of any shape, or mixtures of different sizes and shapes, made of natural or artificial materials, made by any processing method (for example, without limitation, physical grinding, precipitation, emulsification), including organic or inorganic components; by way of Petition 870250095211, dated 10 / 17 / 2025, pp. 61 / 112 52 / 102 illustration, useful particles for this purpose may include, without limitation, sand particles, ceramic particles, biomass materials or particles, mineral particles, resinous materials, glass materials, polymeric materials, rubber materials, compound particulate materials, chemically active materials such as fatty acids, surfactants and sugar alcohols, organic materials such as wood or nut shells that have been chipped, ground, pulverized or crushed to a suitable size (e.g., walnut, pecan, coconut, almond, ivory nut, Brazil nut and the like), seed or fruit pit shells that have been chipped, ground, pulverized or crushed to a suitable size (e.g., plum, olive, peach, cherry, apricot, etc.), coffee powder, pine cone powder, sisal, rice husk ash, rice husk, coconut husk, cotton stalk and the like, chipped, ground, pulverized or crushed parts of other plants,such as corn cobs, specific inorganic particles such as solid glass, glass microspheres, fly ash, silica, alumina, pyrogenic carbon, carbon black, graphite, mica, boron, zirconia, talc, kaolin, titanium dioxide, calcium carbonate (e.g., precipitated calcium carbonate (PCC) or ground calcium carbonate (GCC)), wood flour, lignin, mica, dolomite, wollastonite, halloysite, calcium silicate, flame retardants (such as, but not limited to, halogenated (chlorinated or brominated), phosphorus-based inorganic / mineral flame retardants, nitrogen-based, e.g., hexabromocyclododecane (HBCD), triphenyl phosphate (TPP), tricresyl phosphate (TCP), isopropyl phenol, 3:1 phosphate (PIP 3:1) and the like, as well as combinations or composites of these or similar different materials. In some embodiments, organic materials derived from plants, such as (without limitation) wood or nut shells that have been chipped, ground,pulverized or crushed to a suitable size (for example, walnut, pecan, coconut, almond, ivory nut, Brazil nut and, Petition 870250095211, dated 10 / 17 / 2025, pp. 62 / 112 53 / 102 similar materials); seed husks or fruit pits that have been chipped, ground, pulverized or crushed to a suitable size (e.g., plum, olive, peach, cherry, apricot, etc.); coffee powder, pine cone powder, sisal, rice husk ash, rice husk, coconut husk, cotton stalk and similar materials; and chipped, ground, pulverized or crushed materials from other plants, such as corn cobs, are especially advantageous for use as diluent particles.

[084] Advantageously, in certain embodiments, diluent particles may be selected, either being hydrophobic in nature, or being made hydrophobic (e.g., functionalized PCC), for example, by linking or coating them with a hydrophobic material such as stearic or oleic acid. In some embodiments, the diluent particles may comprise waxes, either as a substance for the particle itself or as a coating for other particles, and these waxes may be in the form of a wax or emulsion (oil-in-water wax emulsion). For example, a wax substance such as beeswax, soy wax, carnauba wax, and the like, may be used as a base particle or as a coating for other diluent particles. As used in the present invention, the term “wax” refers to any lipophilic hydrocarbon and a malleable solid near room temperature, typically with a melting point above 40 °C.As examples, waxes can include long-chain aliphatic hydrocarbons, typically with 20 to 40 carbon atoms per molecule, or fatty acid / alcohol esters, typically containing 12 to 32 carbon atoms per molecule, such as myricyl cerotate, found in beeswax and carnauba wax. Diluent particles can be mixed into the barrier-producing formulation to provide pore-clogging functionalities. b. Composite materials containing NCE Petition 870250095211, dated 10 / 17 / 2025, pp. 63-112 54 / 102

[085] Composite materials containing NCEs, formed from composite matrices in which redispersible or redispersed NCEs are integrated into existing matrices, can be used as plastic substrates to form a multitude of products. After being mixed into the existing matrix, the additive NCEs can be implanted as particles or as more elongated fibrous structures and can align with each other in a straight or randomly oriented manner to form networks or other internal architecture in combination with the existing matrix that is incorporated into the NCE-containing composite material. In some embodiments, the three-dimensional matrix structure of the existing matrix substance is coated and / or impregnated with additive NCEs to form the NCE-containing composite matrix, wherein the presence of the additive NCEs confers a specialized property that exceeds those found in the existing matrix, or that is not found in the existing matrix.For example, composite material containing NCEs can exhibit specialized mechanical properties such as strength, hardness, toughness, brittleness, stiffness, cohesion, durability, impact resistance, optical transparency, and the like, where the presence of NCEs in the NCE-containing composite material produces or enhances this specialized mechanical property.

[086] As another example, the NCE-containing composite material may exhibit a specialized barrier property, such as an OGWR property, which may be present in the existing matrix but is enhanced in the NCE-containing composite material, or which is absent in the existing matrix but is provided in the NCE-containing composite material. In some embodiments, NCEs alone or NCEs modified with barrier-producing substances such as lignin, wax, fatty acids and the like, are able to impart a certain degree of oleophobicity or hydrophobicity to the NCE-containing composite material, and their concentration can be adjusted to optimize this barrier property. Petition 870250095211, dated 10 / 17 / 2025, pp. 64 / 112 55 / 102 Without being limited by theory, it is believed that the close packing of NCEs can enhance the barrier properties they provide. Furthermore, despite their intrinsic hydrophilicity, NCEs (alone or modified with barrier-producing substances) can, under certain circumstances, be sufficiently packed into NCE-containing composite materials to impart water- or vapor-resistant barrier properties to those materials.

[087] The combination of redispersible or redispersed NCEs with an existing matrix can allow the presence of the NCEs to act as pore-closers in their interaction with the existing matrix. Under these circumstances, the redispersible or redispersed NCEs can interact with the existing matrix to coat it or fill the pores or gaps within the network provided by the existing matrix. In some embodiments, these pore-closing effects can be enhanced when used in combination with other oil and grease repellent additives. In this capacity, the NCEs and any matrices they form can act as pore-closers to fill the gaps in the existing matrix, thus acting as plugs to prevent the passage of certain molecules, such as oil and grease, through the NCE-containing composite matrix. This mechanism is similar to the behavior of NCEs as pore-closers for simple NCE-based materials.Furthermore, diluent particles can be added to composite matrices containing NCE, similarly to how diluent particles can be added to simple NCE-based matrices. The role of diluent particles has been described above in detail with reference to simple NCE-based materials; mutatis mutandis, this description can be applied to the use of diluent particles for NCE-containing composite materials. In short, diluent particles can be added to complex matrices containing NCE for the purpose of... Petition 870250095211, dated 10 / 17 / 2025, pp. 65 / 112 56 / 102 volume and / or to act as pore-closers for simple cellulose-based matrices, alone or in conjunction with other barrier materials. In several embodiments, diluent particles can be used in addition to, or instead of, barrier-producing formulations; in either case, the diluent particles can interact with existing matrices and / or NCE-containing composite matrices to impart barrier properties such as oleophobicity and / or hydrophobicity.

[088] More generally, the process of formulating NCE-containing composite materials from NCE-containing composite matrices can be designed to produce the desired material properties. The production of OGWR properties by incorporating barrier-producing formulations into such materials is an example of how NCE-containing composite matrices can be designed to produce such material properties. Existing matrices can be formulated to make them especially suitable for combination with redispersible or redispersed NCEs in order to form NCE-containing composite matrices and produce NCE-containing composite materials.For example, the degree of flexibility in a product formed from NCE-containing composite materials can be finely adjusted by varying the composition of the existing matrix, the amount of NCE additives used in the existing matrix to form the NCE-containing composite matrix, and / or the amount of various additives intended to optimize the properties of the final NCE-containing composite material. By selecting appropriate additives and polymers for the existing matrix into which the NCEs are integrated to form a composite material, such additives can produce properties such as structural strength, resilience, elasticity, water resistance, oil and grease resistance, and the like, for manufactured articles formed from them, in combination with biodegradability. Petition 870250095211, dated 10 / 17 / 2025, pp. 66 / 112 57 / 102

[089] The block diagram in FIG. 3 schematically illustrates how the barrier production formulation can be added during the formation of the NCE-containing composite matrix and its subsequent processing. Process 300 in FIG. 3 begins with the supply of a dry material 302 containing redispersible NCEs, where such dry material 302 has been prepared substantially as described in connection with FIG. 1. The dry material 302 is then treated with a resuspension fluid 304 in a resuspension step 306 to form a suspension 308 of redispersed NCEs, substantially as described in connection with FIG. 1. The suspension 308 of redispersed NCEs is then combined with an existing matrix 310 to produce the NCE-containing composite matrix 312, substantially as shown in Step 5a in FIG. 1. The composite matrix containing NCE 312 can be combined with additives and / or further processed to form a composite material containing NCE 314.The barrier production formulation 318 can be added at points A and B substantially as described in connection with FIG. 1. Alternatively, or additionally, the barrier production formulation 318 can be added at one or more of the points W, X, Y, and Z.In more detail; barrier production formulation 318 can be added as suspension 308 of redispersed NCEs 308 is mixed with existing matrix 310, as indicated by point W; barrier production formulation 318 can be added to existing matrix 310 before it is mixed with suspension 308 of redispersed NCEs, as indicated by point X; barrier production formulation 310 can be added to the composite matrix containing NCE 312 as it is processed to become the composite material containing NCE 314, as indicated by point Y; and / or barrier production formulation 310 can be added to the composite material containing NCE 314, as indicated by point Z. For the latter. Petition 870250095211, dated 10 / 17 / 2025, pp. 67 / 112 58 / 102 type of application, advantageously the barrier production formulation can be sprayable to allow easy application, either on the surface of the composite material containing NCE 314 or on the surface of formed articles manufactured from it (not shown). Although a single barrier production formulation 318 is represented in this Figure, it is understood that a plurality of barrier production formulations or barrier production formulation ingredients can be added at the different introduction points W, X, Y or Z. A first barrier production formulation can be added at one introduction point, and a second barrier production formulation can be added at a second introduction point. Combinations of barrier production formulations and / or ingredients can be introduced at any point in the process.

[090] In some embodiments, barrier production formulations can be prepared containing biopolymers as additives to impart OGWR properties or other useful properties to NCE-containing composite materials, similarly to how such additives can be used with barrier production formulations combined with plain NCE-based materials. These additives can be added to the barrier production formulation, which can then be combined with the NCE-containing composite matrix as described above. Biopolymers may include biopolymers such as polyhydroxyalkanoates and polylactic acid derivatives. Advantageously, certain exopolysaccharides, such as pullulan, kefiran, cellulose, levan, gellan, and the like, can be used to form films, which can be advantageous for those barrier production formulations that are used as coatings for NCE-containing composite materials and useful articles made from them.Such biopolymers may also include, but are not limited to, exopolysaccharides such as bacterial cellulose, kefiran, pullulan, levan, gellan, and other polysaccharides. Petition 870250095211, dated 10 / 17 / 2025, pp. 68 / 112 59 / 102 natural compounds such as alginate, lignin, carrageenan, gum arabic, starch, and vegetable glucomannans, such as locust bean gum, mannan, guar gum, and the like, and cellulose derivatives. As used in the present invention, the products created by modifying native cellulose polysaccharides are referred to as "cellulose derivatives," "cellulosic polymers," or "cellulose." Such modifications may include chemical modifications, such as cellulose degradation and derivatization of -OH groups. Acid / base, oxidative, biological, and mechanical processing are all examples of degradation reactions. Modifications that introduce new functional groups into the cellulose backbone include reactions such as carboxymethylation, oxidation, and addition reactions. Other reactions such as esterification, acylation, grafting, and etherification may also produce cellulose derivatives. Other examples of reactions that produce cellulose derivatives are well known in the field.

[091] A variety of specialized properties of composite materials using NCEs have already been contemplated in the industry, but their use has been hampered by the redispersion problems mentioned above. The redispersion technologies disclosed in the present invention facilitate the transport of NCE compositions that can be concentrated or dried and then resuspended to be combined with existing matrices, producing NCE-containing composite materials. In some embodiments, these redispersion technologies can produce a uniform mixture of high aspect ratio NCEs within the primary matrix-forming material, allowing the intensification of desirable specialized properties in the final composite, including mechanical properties such as those mentioned above. In other embodiments, the NCE formulations produced using the redispersion technologies disclosed in the present invention can be prepared in such a way as to introduce or intensify properties Petition 870250095211, dated 10 / 17 / 2025, pp. 69 / 112 60 / 102 specialized, such as barrier properties that allow the NCE-containing composite material to have desirable degrees of oil and grease resistance and / or water vapor resistance.

[092] The redispersible and redispersed NCEs produced as described in the present invention can act as diluents in composite matrices containing NCEs. It is understood that diluents improve the mechanical and barrier properties of organic substances, such as plastics, and / or make these materials, or products made from them, more economical to produce or transport, for example, by requiring less expensive ingredients or making them lighter. The redispersible and redispersed NCEs produced as described in the present invention can also be combined with other bulking agents, such as pulp or pulp-based substances, to increase the final volume of the NCE-containing composite matrix while maintaining strength through the presence of the additive NCEs. Although NCEs have already been used as diluents in plastics, their use has been limited by their resistance to redispersibility.

[093] The methods for redispersing NCEs disclosed in the present invention may allow for the more widespread use of NCEs for purposes such as reinforcing composite materials and plastic substrates, and may further allow for a drastic expansion of new uses. As used in the present invention, the term “reinforcement” refers to an improvement of a mechanical characteristic found in the existing matrix relating to strength, hardness, toughness, brittleness, stiffness, cohesion, flexibility, durability or impact resistance, or a provision of such a mechanical characteristic if it is not already present in the existing matrix. A composite matrix containing NCEs with improved mechanical properties compared to the existing matrix may be termed “reinforced”, with the reinforcement of the composite matrix Petition 870250095211, dated 10 / 17 / 2025, pp. 70 / 112 61 / 102 containing NCEs, which is attributable to the presence of NCEs. NCEs can be used as diluents in a variety of environments, as the previous examples demonstrate.

[094] In certain embodiments, the NCE-containing composite matrix is ​​formed from an existing petroleum-derived matrix into which redispersible or redispersed NCEs are incorporated. In other embodiments, the NCE-containing composite matrix is ​​formed from an existing bio-based matrix into which redispersible or redispersed NCEs are incorporated. i. Existing matrices derived from petroleum

[095] In some embodiments, petroleum-derived polymers are used to form existing matrices that are combined with additive NCEs (redispersible or redispersed) to form composite matrices containing NCEs with advantageous properties. A variety of petroleum-derived polymers can be used as existing matrices to form composite matrices with NCEs, for example, polyvinyl alcohol, high-density polyethylene, low-density polyethylene, polyvinyl chloride, acrylonitrile butadiene styrene, polypropylene, polylactic acid, polybutylene succinate, polyethylene succinate, polypropylene succinate and the like. The addition of NCEs to these matrices can provide specialized properties, such as a mechanical property, for example, increased strength and / or flexibility, or a barrier property, such as an oleophobic or hydrophobic property, or a water vapor resistant property.Furthermore, redispersible or redispersed NCEs can be added to matrices as ingredients in a formulation that also includes a bulking agent, such as pulp or a pulp-based substance. These formulations can provide additional volume to the resulting composite matrix containing NCEs, while the NCE component retains or enhances its properties. Petition 870250095211, dated 10 / 17 / 2025, pp. 71 / 112 62 / 102 mechanical improvements compared to the existing matrix. The use of such formulations, comprising redispersible or redispersed NCEs and bulking agents, can reduce the need for other expensive ingredients and thus lower the overall cost of the resulting composite matrix containing NCEs and the materials produced from it.

[096] However, the use of redispersible or redispersed NCEs as additive NCEs in combination with existing hydrophobic matrices presents challenges because the NCEs themselves are hydrophilic. Although incorporating additive NCEs into existing hydrophobic matrices can cause problems due to the weak interfacial resistance between the hydrophobic polymeric matrix and the hydrophilic NC elements, redispersible or redispersed NCEs can be further modified to become more hydrophobic, so that a stronger interface is created. For use in a hydrophobic environment, the NCEs can have their surface modified to match the properties of the existing hydrophobic matrix into which they will be incorporated, so that they are compatible with the existing matrix and can be regularly dispersed within it.In some embodiments, the surface modification of additive NCEs prepared according to the methods disclosed in the present invention can be carried out, for example, by using a hydrophobic monolayer on the NCEs. The methods for this modification may include silane coupling, alkaline treatment, acetylation, carbonylation, TEMPO oxidation, polymer grafting, bacterial modification, surfactant addition, and the like. In some embodiments, the NCEs that have been hydrophobized for use in hydrophobic matrices can be prepared so that they are not only redispersible after drying, but are also, by virtue of their hydrophobic coating, compatible with various existing hydrophobic polymeric matrices, such as thermoplastic and thermoset matrices (e.g., Petition 870250095211, dated 10 / 17 / 2025, pp. 72 / 112 63 / 102 example, polypropylene, polyethylene, polystyrene, polyesters, poly(acrylates / methacrylates), rubbers, silicones, urethanes, epoxies and the like), to produce strong and lightweight composite materials containing NCEs for further processing to provide manufactured articles. Other modifications may include those that enhance the interfacial adhesion between the hydrophobic matrix and the hydrophilic NCEs, such as the incorporation of another additive (e.g., a fatty acid or a surfactant) that has a polar head and a non-polar tail; it would be understood that this additive could interact with both the hydrophobic matrix and the hydrophilic NCEs to improve their adhesion to each other.

[097] As described previously, other additives to obtain desirable properties can be added to NCE-containing composite matrices to produce NCE-containing composite materials useful as plastic substrates. Such additives can be added at any stage of the production of the NCE-containing composite material, for example, by being added to the existing matrix, or to the NCE-containing composite matrix, or to the NCE-containing composite material. For example, plasticizers such as phthalate esters can be employed to make the material more flexible and versatile. This NCE-containing composite material containing a plasticizer can then be shaped by conventional techniques such as extrusion, calendering, injection molding, thermoforming, blow molding and the like, to produce formed articles.The redispersible NCEs incorporated into the composite matrix containing NCEs act as reinforcements, diluents, particles, or fibers that improve the mechanical properties of the material that has been softened by the plasticizers.

[098] In some embodiments, redispersed NCEs can be added to improve the mechanical performance of recycled petroleum-derived plastics, i.e., plastic materials comprising polymers Petition 870250095211, dated 10 / 17 / 2025, pp. 73 / 112 64 / 102 petroleum derivatives, where petroleum-derived plastic is derived from recycled plastic material. Plastic waste can be repurposed to create a variety of formed articles, but significant deterioration in material properties can occur during the recycling process, largely attributed to high heat and mechanical stress. Furthermore, contamination of the recycling stream often occurs due to a lack of consumer awareness of proper recycling habits and sorting errors at the recycling facility. Deterioration (reduction in molecular weight, chain breaks, defects, etc.) and the presence of impurities contribute to reduced strength of recycled plastic compared to its virgin equivalent. Incorporating redispersed NCEs into recycled plastic feedstock can strengthen the weakened matrix. NCEs can be combined with powder, flakes, or other forms of recycled plastic.Recycled plastic feedstock can be a specific polymer or copolymer blend, or it can also be a blend of several recycled plastics. Redispersed NCEs can be combined with the recycled feedstock before or during thermal processing. For example, redispersed NCEs can be fed into an extruder for mixing and dispersion with recycled molten polymer feedstock being processed through the screws. The items produced can be suitable for single-use applications such as food utensils (like cutlery, plates, and straws) or consumer goods packaging, or for long-term applications such as furniture, including tables, chairs, cabinets, and the like. ii. Existing bio-based matrices

[099] In some embodiments, bio-based polymers are used to form the existing matrices that are combined with NCEs. Petition 870250095211, dated 10 / 17 / 2025, pp. 74 / 112 65 / 102 additives to form composite matrices containing NCEs with advantageous properties. Under these circumstances, all structural components of the NCE-containing composite matrix are bio-based, as is the NCE-containing composite material formed from the NCE-containing composite matrix. This NCE-containing composite material can be used as a plastic substrate to be transformed into manufactured articles. The production of this plastic substrate from bio-based components (i.e., redispersible or redispersed NCEs (additives) and an existing bio-based matrix) offers sustainability benefits, both in eliminating dependence on petrochemical raw materials and in facilitating the degradation and disposal of products formed from these plastic materials.

[100] In embodiments that use bio-based polymers to form the existing matrix, the constitutive bio-based polymer that forms the existing matrix may be a homopolymer, copolymer, polymer blend, or any combination thereof. Additive ingredients may be combined with the constitutive bio-based polymer to optimize the properties of the existing matrix. For example, cellulose acetate (CA) and cellulose butyrate (CAB) may be mixed in an acetone solution or blended in a molten state under high shear, such as extrusion, to form an existing matrix; alternatively, one of the two cellulosic polymers may be used independently.Additional or alternative cellulosic polymers that can be used for the existing matrix include cellulose acetate propionate, methylcellulose, hydroxypropylmethylcellulose, sodium carboxymethylcellulose, carboxymethylcellulose, cellulose acetate phthalate, hydroxyethylcellulose, chitosan, and the like. Polyhydroxyalkanoates (PHAs), including poly-3-hydroxybutyrate (PHB), polyhydroxyvalerate (PHV), polyhydroxyhexanoate (PHH), and the like, may also be used. Petition 870250095211, dated 10 / 17 / 2025, pp. 75 / 112 66 / 102 used to form a matrix. Polybutylene succinate (PBS), polybutylene-coadipate succinate (PBSA), and the like produced from biomass can also be used to form a matrix. In some embodiments, one or more plasticizers may be added to the existing matrix to soften and increase its flexibility. Bio-based plasticizers may be added to the existing matrix, including fatty acids, polyols, epoxidized triglyceride vegetable oils, alkyl esters of adipic and citric acids, and the like; examples of such plasticizers include, without limitation, triglycerin, tributyl citrate, triethyl citrate, acetyl triethyl citrate, polyethylene glycol, epoxidized soybean oil, oleic acid, and the like.Bio-based resinous materials, such as gum resin, can be added to hydrophobize, harden, and / or bind the existing matrix and limit the degree of flexibility; such materials have other advantages, for example, acting as a glue-like substance to fix matrix parts to each other or to form bridges between them. These materials may have the added advantage of assisting in the hydrophobization of the matrix and any subsequent materials derived from it, if water resistance is desired for end-use applications. Other additives may be included to optimize the material properties for end-use applications.For example, diluents and bulking agents can be added: pulp can be included as a diluent or bulking agent in the existing matrix to reduce costs and improve texture; wood flour, sawdust, ash, mineral powders, lignin, and other low-cost diluent particles can be used to reduce costs and / or close pores within a matrix; precipitated calcium carbonate and stearic acid can be added to the existing matrix to improve hardness and hydrophobicity, and precipitated calcium carbonate alone can be added to act as a nucleating agent or to provide gloss. Alternatively, or in combination with other additives, a. Petition 870250095211, dated 10 / 17 / 2025, pp. 76 / 112 67 / 102 oil-grease resistant and / or water-resistant (OGWR) formulations can be incorporated into existing matrices to achieve hydrophobicity and oleophobicity as desired. Additives that enhance biodegradability can be used to aid in the rapid decomposition of matrices after disposal; for example, silica particles can be integrated into a CAB-plasticized matrix.

[101] As examples, photocatalysts, pro-oxidants, and enzymes can be used to accelerate the degradation of NCE-containing materials such as plastics when they enter the landfill. Using the example of enzymes, and without limiting ourselves to theories, it is understood that the following mechanisms explain the activities of some of these additives that enhance biodegradability. To degrade the different cellulose derivatives, first the functional groups need to be broken, and then the β-1,4 linkages in the cellulose backbone can be broken further. Unmodified cellulose can be degraded by the enzymes cellulase and β-glucosidase. Lipase or acetylsterase are examples of enzymes that can be used to hydrolyze the acetyl group in cellulose acetate. By incorporating enzymes into the plastic matrix, their activity can accelerate its degradation, for example, while it is in a waste facility or landfill.Methods for incorporating enzymes into the matrix can include physical adsorption, covalent bonding, crosslinking, and encapsulation. Additionally, enzymes can be immobilized onto particles and then incorporated into the existing matrix for better retention and distribution. Furthermore, enzyme loading and enzyme selection can be adjusted to accelerate or decelerate the degradation rate under different circumstances. For example, enzymes active within specific temperature ranges and pH environments can be selected to initiate degradation when the plastic material containing NCE is intended for home composting or soil, or... Petition 870250095211, dated 10 / 17 / 2025, pp. 77 / 112 68 / 102 Alternatively, when the plastic material is intended for a slower degradation process, by being deposited in a sanitary landfill.

[102] Ultraviolet (UV) resistance can also be imparted to the existing matrix or to the NCE-containing composite matrix with additives that absorb or stabilize UV ​​radiation. For example, carbon black or other UV-absorbing dyes can be added as pigments. In some embodiments, lignin, a bio-based material containing different UV functional groups, including phenolic units, ketones, chromophores, and conjugated double bonds that can confer UV resistance, can be incorporated as a UV-absorbing additive in the polymer matrix to enhance long-term stability. In some embodiments, lignin can be combined with the NCE-containing matrix for manufactured articles (e.g., sunglasses frames) that are commonly exposed to UV rays.

[103] In some embodiments, the existing matrix or the composite matrix containing NCEs may be magnetized with additives such as band ferric oxide. Although the additives are described above as being added to the existing matrix, it is understood that they may be introduced directly into the composite matrix formulation (i.e., after the additive NCEs are combined with the existing matrix), in addition to or instead of introducing them into the existing matrix.

[104] In one embodiment, a composite matrix containing NCEs for use in an NCE-containing composite material can be prepared as follows. In this embodiment, the existing bio-based matrix is ​​prepared to include performance-enhancing additives, and this existing matrix is ​​then combined with the redispersible or redispersed NCEs (additives). In one embodiment, to prepare the existing bio-based matrix, the matrix-forming ingredients are dissolved in an acetone or water solution, Petition 870250095211, dated 10 / 17 / 2025, pp. 78-112 69 / 102 depending on the solubility parameters of the matrix, to form a solution containing about 2% by weight to about 25% by weight, about 5% by weight to about 15% by weight, about 5% by weight to about 50% by weight, or about 20% by weight to about 75% by weight of these ingredients, for example, a 12% by weight solution of these ingredients; in other embodiments, solvent may not be required. Thermal processing and high shear mixing can be used to create a hot melt of the matrix material. Powder, pellets, or other forms of the matrix can be fed into a twin-screw extruder and heated to a softened state that can be combined with redispersible NCEs and other additives. Matrix-forming ingredients may include constitutive polymer ingredients (e.g., cellulose acetate (CA), cellulose acetate butyrate (CAB) or the like, and other cellulose ethers such as methylcellulose, carboxymethylcellulose,Hydroxypropylcellulose, carboxymethylcellulose, sodium carboxymethylcellulose, hydroxymethylcellulose and the like, polyhydroxyalkanoates (PHAs), such as poly-3-hydroxybutyrate (PHB), polyhydroxyvalerate (PHV), polyhydroxyhexanoate (PHH), polybutylene succinate (PBS) and the like, or combinations of such polymer ingredients) may be combined with plasticizers (e.g., triacetin, triethyl citrate, acetyltriethyl citrate, glycerol, xylitol, trehalose, sorbitol, mannitol, polyethylene glycol, polypropylene glycol, epoxidized soybean oil, castor oil, palm oil and the like), together with rosin or derivatives thereof, diluents such as calcium carbonate or silica, bulking agents such as pulp or pulp-based materials and / or fatty acids (preferably saturated), such as stearic acid, lauric acid, Palmitic acid, oleic acid, and related substances. For example,CAB or another biopolymer may be added in a range of about 55% to about 95%; plasticizer may be added in a range of about 0.1% to about 20%; the resin of, Petition 870250095211, dated 10 / 17 / 2025, pp. 79-112 70 / 102 gum can be added in a range of about 10% to about 40%. As another example, CAB or another biopolymer can be added in a range of about 60% to about 90%; the plasticizer can be added in a range of about 0.1% to about 20%; stearic acid can be added in a range of about 5% to about 25%, and calcium carbonate can be added in a range of about 3% to about 17%, with the ratio of stearic acid to calcium carbonate at about 3:2. In another example, HPC or another biopolymer can be added in a range of about 55% to about 95%; the plasticizer can be added in a range of about 5% to about 40%, and gum resin can be added in a range of about 10% to about 40%. As another example, HPC or another biopolymer can be added in a range of about 5 to about 50%; the plasticizer can be added in a range of about 0.5% to about 30%.

[105] For example, ingredients such as rosin, a plasticizer, and cellulose acetate butyrate (or any other biopolymer or combination of biopolymers) are combined with other additives; under certain circumstances, the order of combination may be important. In some embodiments, the less viscous ingredients are combined first (rosin, PCC, stearic acid), with the subsequent addition of CAB, followed by the addition of the plasticizer. The solution is stirred until the mixture is homogeneous and remains free of lumps. This solution thickens to provide the existing matrix into which the additive NCEs are to be incorporated.

[106] In parallel, additive NCEs are prepared. In one embodiment, a selected quantity of dry, redispersible material containing NC, prepared as described above, is resuspended in a resuspension fluid, such as water, by mixing thoroughly with a suspension mixer. Petition 870250095211, dated 10 / 17 / 2025, pages 80 / 112 71 / 102

[107] In this way, a formulation of redispersed additive NCEs is produced. In one embodiment, a formulation of redispersed NCEs may contain an amount of redispersed NCEs suitable to achieve the desired properties in the NCE-containing composite material. An amount of redispersed NCEs ranging from about 1% to about 50% (% by weight) of the entire NCE-containing composite matrix may be used, with a range of about 5% to about 40% being advantageous. The use of less water in this formulation will facilitate the drying of the material into which the NCE additives will be incorporated, aiding in its moldability. This additive NCE formulation is then combined with the existing matrix to produce the NCE-containing composite matrix. In this embodiment, no additional ingredients are added to the NCE-containing composite matrix, since the appropriate ingredients have already been added to the existing matrix.A surfactant such as capryl glucoside can be added; without delving into theory, it is understood that such an additive can bind polar and non-polar components during mixing and processing. The composite matrix containing NCE and any other desired ingredients can then be mixed under high shear by a suspended agitator, a high-shear mixer, a twin-screw extruder, and the like, to produce the NCE-containing composite material. This initial forming process can be adjusted based on the viscosity requirements of the manufacturing process used to produce the article formed from the NCE-containing composite material. 4. Manufactured articles with OGWR properties a. General OGWR properties

[108] In embodiments, barrier production formulations may be prepared to emphasize OGR properties or WVR properties or both; in some embodiments, barrier production formulations may include both types of properties, and the components of Petition 870250095211, dated 10 / 17 / 2025, pp. 81 / 112 72 / 102 formulations can be adjusted to accentuate or balance OGR or WVR properties. For example, there is a variety of cellulosic polymers, with the various polymers having different degrees of hydrophobicity or oleophobicity, so a cellulosic polymer can be selected to produce the desired degree of OGR and / or WVR. Barrier production formulations to produce water resistance can include a variety of cellulose-based polymers, and specifically those that are more hydrophobic. In general, cellulose-based polymers tend to be oleophobic (hydrophilic), so it may be beneficial to include other materials in barrier production formulations if greater water resistance is desired. For example, methylcellulose offers good oil / grease resistance but not as much water resistance. A mixture of methylcellulose (MC) and cellulose acetate (CA) can be provided to adjust OGR and WVR properties.The LCST polymers discussed work well for oil resistance, but the films / coatings created with them are soluble at room temperature, making their water resistance properties less efficient. Cellulose acetate and lipids are some examples of additives that can be used to adjust barrier production formulations to be more hydrophobic, and combining this component with a more oleophobic material can provide resistance to both oil and water. Cellulose acetate, in particular, can provide both hydrophobic and oleophobic properties. Cellulose acetate and other cellulose acetate derivatives (e.g., without limitation, cellulose acetate butyrate) are unique because they also exhibit a degree of oleophobicity in addition to their strong hydrophobicity.Similarly, certain diluents have more hydrophobic or oleophobic properties: for example, a diluent such as wax can be selected to increase hydrophobicity, or, for example, a large surplus of NCEs can be added. Petition 870250095211, dated 10 / 17 / 2025, pp. 82-112 73 / 102 pore-tightening agents to increase oleophobicity. Fatty acids, alone or combined with charged binding agents, such as a mineral (e.g., calcium carbonate combined with stearic acid), can also be used to increase hydrophobicity.

[109] In some embodiments, substances such as NCEs, MC, HPMC, CMC, NaCMC, CA, CAB, chitosan, rosin, lignin, vegetable proteins (such as pea protein, zein and the like) and / or any combination thereof may be employed as oleophobic substances to provide oil resistance; in some embodiments, substances such as MC, CA, CAB, chitosan, rosin, hydrophobized starch, lignin, pea protein, zein and / or any combination thereof may be employed as hydrophobic substances to provide resistance to water and / or water vapor.

[110] In more detail, depending on the balance and quantities of ingredients, barrier production formulations can be classified into three general categories: 1) those that provide balanced OGR and WVR properties; 2) those that provide some or no hydrophobicity, but substantial oleophobicity; and 3) those that provide some or no oleophobicity, but substantial hydrophobicity. Articles incorporating Category 1 barrier production formulations can be used for applications such as food packaging, where both oil repellency and water repellency are advantageous.Articles incorporating Category 2 barrier production formulations can be used for applications where oil resistance is the most important attribute, for example, in containers for oils or greasy materials and for packaging pre-measured quantities of oil-based products such as salad dressings or cosmetic lotions, or for use as more durable reservoirs that can hold motor oil and similar fluids instead of containers of... Petition 870250095211, dated 10 / 17 / 2025, pp. 83-112 74 / 102 metal used for this purpose. Articles incorporating Category 3 barrier production formulations may be used for applications where water repellency (even waterproofing) is the most important attribute, for example, in coffee cups and beverage can holders in six-packs, or in grocery bags and other containers (such as cardboard boxes) or packaging intended to be substantially water-resistant or leak-proof. b. Exemplary oleophobic and hydrophobic manufactured articles

[111] The ubiquity of plastic products offers a wide range of other opportunities to replace NCE-containing materials, as described in the present invention, with conventional petroleum-derived plastics currently employed. In view of the environmental challenges that accompany the production and disposal of conventional petroleum-derived plastics, NCE-containing composite materials, as disclosed in the present invention, offer welcome alternatives. Illustrative examples include, without limitation, transaction cards, plastic bottles, packaging and wrappings, space fillers (shock, thermal and acoustic insulation), films and sheets, straws and food utensils such as cutlery, enhanced OGWR and resistance of paper-based products (such as, without limitation, cardboard, paperboard and any fiber-based products), structural plastics, enamels and foams, and the like.Bio-based materials containing NCEs for the production of useful manufactured articles can be customized and manipulated to produce desired performance and degradability properties. i. Transaction cards

[112] Transaction cards, common in routine business applications, are small, lightweight, and easily portable devices used for Petition 870250095211, dated 10 / 17 / 2025, pp. 84 / 112 75 / 102 perform administrative transactions, such as transferring payments, opening accounts, providing identification, and the like. These transaction cards are ubiquitous in modern commerce. Examples include credit cards, debit cards, prepaid gift cards (collectively payment cards), transportation passes, identity cards, insurance cards, hotel keys, and the like. They are typically formed from petroleum-derived substances that provide a lightweight and durable substrate for molding, printing, and incorporating specialized components such as iron oxide for magnetic stripes, inks, dyes, and chips. They are typically made as PVC laminates, a petroleum-derived plastic that takes hundreds of years to degrade. In 2020, it was estimated that there were six billion payment cards in circulation; each year, 30 million kg of PVC are used for issuing these cards.

[113] Although it is recognized that these transaction cards may include materials other than petroleum-derived plastics, such as metals, glass, silicon, and resins, converting petroleum-derived plastic sources to bio-based sources may have distinct advantages for the disposal of these cards. For example, in cases where the cards or fragmented waste from them is incinerated in a recycling facility, a bio-based material would generate fewer toxic gases than petroleum-derived alternatives. Furthermore, bio-based materials that can be biodegraded can undergo programmed decomposition in waste management facilities, so that their incineration can be avoided.

[114] Using the methods described above, more environmentally friendly alternative substrates for transaction cards can be produced by combining an existing bio-based matrix with redispersed NCEs (additives) to produce a composite matrix containing NCEs. As discussed earlier, the Petition 870250095211, dated 10 / 17 / 2025, pages 85 / 112 76 / 102 composite matrix containing NCE in combination with any desirable additives constitutes the NCE-containing composite material that can be used as a plastic substrate to form transaction cards. For these products, it is advantageous to include water-resistant additives so that the card maintains its integrity throughout its service life.

[115] A basic formulation for NCE-containing composite material useful in the formation of transaction cards may include the following ingredients combined to form a 5% by weight to 50% by weight solution, for example, a 12% by weight solution in acetone, or as solids in a high shear mixer such as a hot melt extruder (by weight, based on a total formulation weight of 100 g): • Cellulose acetate butyrate (CAB): 36 g • Redispersed NCEs (NFC or MFC or combinations thereof): 36 g • Rosin gum (GR): 26 g • Plasticizer (triacetin, triethyl citrate or acetyltriethyl citrate): 2 g.

[116] Although specific quantities of these ingredients are given for the exemplary formulation above, it is understood that ranges of these ingredients can be added to create other formulations with advantageous properties. As an example, the nanocellulose component can be added in a range of about 5% to about 50%; CAB can be added in a range of about 30% to about 70%; the plasticizer can be added in a range of about 0.1% to about 15%; rosin gum can be added in a range of about 5% to about 45%. In this formulation, CAB in combination with rosin gum and plasticizer can produce an existing matrix to be combined with the additive NCEs to produce the NCE-containing composite material. In composite materials Petition 870250095211, dated 10 / 17 / 2025, pp. 86 / 112 77 / 102 containing NCE with a relatively higher amount of CAB, the CAB will have more influence on the properties of the overall composite material containing NCE, compared to the influence of the NCEs; on the other hand, in composite materials containing NCE with a relatively higher amount of redispersed NCEs, the NCEs will have more influence on the properties of the overall composite material containing NCE, compared to the influence of the CAB. In some embodiments, the redispersed NCEs can be combined with a bulking agent, such as pulp or a pulp-based material, to be added to the existing CAB-based matrix.

[117] A basic formulation for NCE-containing composite material useful in the formation of transaction cards may include the following ingredients combined to form a 5% by weight to 50% by weight solution, for example, a 12% by weight solution in acetone or as solids in a high shear mixer such as a hot melt extruder (by weight, based on a total formulation weight of 100 g): • A cellulose derivative, such as cellulose acetate butyrate (CAB): 41 g • Redispersed NCEs (NFC or MFR or combinations thereof): 28 g • Pulp: 9 g • Capryl glycoside: 2 g • Plasticizer (triacetin, triethyl citrate or acetyl triethyl citrate): 4 g • Rosin gum: 16 g.

[118] This basic formulation can be modified to produce an NCE-containing composite material that produces a flexible card with enhanced hardness. Such a formulation may include the following ingredients combined to form a 5% by weight to 50% by weight solution, for example, a Petition 870250095211, dated 10 / 17 / 2025, pp. 87 / 112 78 / 102 12% by weight solution in acetone or as solids in a high-shear mixer, such as a hot melt extruder (by weight, based on a total formulation weight of 100 g): • A cellulose derivative, such as cellulose acetate butyrate (CAB): 36 g • Redispersed NCEs (NFC or MFC or combinations thereof): 36 g • Plasticizer (triacetin, triethyl citrate or acetyltriethyl citrate): 2 g • Stearic acid: 16 g • Precipitated calcium carbonate (PCC): 10 g.

[119] Although specific quantities of these ingredients are given for the exemplary formulation above, it is understood that ranges of these ingredients may be added to create other formulations with advantageous properties. As examples, the nanocellulose component may be added in a range of about 5% to about 50%; CAB may be added in a range of about 30% to about 70%; the plasticizer may be added in a range of about 0.1% to about 15%; stearic acid may be added in a range of about 1% to about 12%; calcium carbonate (PCC) may be added in an amount of about 0.6% to about 8%, with a desirable stearic acid: PCC ratio of about 3:2.In composite materials containing NCEs with a relatively higher amount of CAB, the CAB will have a greater influence on the properties of the overall composite material containing NCEs, compared to the influence of the NCEs; on the other hand, in composite materials containing NCEs with a relatively higher amount of redispersed NCEs, the NCEs will have a greater influence on the properties of the overall composite material containing NCEs, compared to the influence of the CAB. In some embodiments, the redispersed NCEs can be combined with one. Petition 870250095211, dated 10 / 17 / 2025, pp. 88 / 112 79 / 102 bulking agent, such as pulp or a pulp-based material, to be added to the existing CAB-based matrix. In this formulation, CAB in combination with rosin gum and plasticizer can produce an existing matrix to be combined with NCE additives to produce the NCE-containing composite material. Without delving into theory, it is understood that the addition of a fatty acid (e.g., stearic acid) is amphiphilic, thus providing hydrophobic properties to the matrix and facilitating the incorporation of hydrophilic PCC particles into the matrix; the PCC particles can act as a hardening reinforcing agent in the CAB matrix.

[120] Barrier production formulations can be integrated into NCE-containing composite materials used to form transaction cards to produce OGWR properties. In some embodiments, hydrophobic properties are imparted to the NCE-containing composite material by including a hydrophobic agent in the existing matrix or in the NCE-containing composite, so that the final transaction card product is water-resistant and more durable. In other embodiments, a bio-based hydrophobic and / or oleophobic coating can be painted onto the surface of the formed transaction card product or onto the surface of one or more layers of NCE-containing composite materials that are laminated together to form the transaction card.Suitable hydrophobic agents include, without limitation, those organic compounds that have a highly polar region and an apolar region, allowing the compound to bind or complex with hydrophilic NCEs and provide an apolar outer surface. Examples of hydrophobic agents include fatty acids such as stearic acid, lauric acid, palmitic acid, oleic acid, and the like; surfactants such as fatty amines or fatty alcohols; rosin components such as abietic acid, neoabietic acid, palustric acid, pimaric acid, isopimaric acid, and dehydroabienic acid; and... Petition 870250095211, dated 10 / 17 / 2025, pp. 89-112 80 / 102 natural waxes, such as lanolin, beeswax and carnauba wax, and the like. Hydrophobic agents may include silanes, siloxanes or silica micro / nanoparticles, but these are less advantageous for the materials disclosed in the present invention due to their environmental impact.

[121] Hydrophobizing formulations, including formulations that can be added to the NCE-containing composite matrix and formulations that can be coated onto the surface of one or more layers of NCE-containing composite materials, may include ingredients such as cellulose acetate (CA) in a range of about 25% to about 70%; rosin gum (GR) in a range of about 25% to about 70%; and a plasticizer such as triacetin, triethyl citrate, or acetyl triethyl citrate in a range of about 1% to about 20%. To produce a hydrophobizing formulation, the preceding ingredients can be dissolved in an ethanol / alcohol solvent mixture, in a ratio of about 0.1% to about 20% hydrophobizing ingredients (by weight), about 10% to about 50% ethanol (by weight), and about 50% to about 70% acetone (by weight).

[122] An exemplary formulation for such a hydrophobic and oleophobic coating may include the following ingredients combined to form a solution in acetone (by weight, based on the total weight of the 100 g formulation): • Cellulose acetate (CA): 7 g • Ethanol: 14 g • Acetone: 71 g • Rosin gum (GR): 7 g • Plasticizer (triacetin, triethyl citrate or acetyl triethyl citrate): lg·

[123] An exemplary formulation for producing an oil, grease and water resistant barrier to be used as a coating (by weight, based on a Petition 870250095211, dated 10 / 17 / 2025, pp. 90-112 81 / 102 (total formulation weight of 100 g) includes: • Methylcellulose (MC): 3 g • Redispersed NCEs (NFC or MFC or combinations thereof): 1 g • Water: 54 g • Rosin: 4 g • Ethanol or Acetone: 38 g.

[124] An exemplary formulation for an oleophobic coating includes the following ingredients combined to form an aqueous solution in water (by weight, based on a total formulation weight of 100 g): • Methylcellulose (or any cellulose ether): 75 g • Redispersed NCEs (NFC or MFC or combinations thereof): 25 g. ii. Plastic bottles

[125] Plastic bottles are conventionally made from various types of petroleum-derived polymers, including, without limitation, polyethylene terephthalate, polyethylene, polypropylene, polycarbonate, and the like. These manufactured articles are widely used commercially, serving as containers for a virtually unlimited variety of liquid and solid substances, such as foods (e.g., condiments, cooking oils, salad dressings, and the like), soaps, shampoos, household products, industrial products, personal care items, cosmetics, and pharmaceuticals. A significant environmental challenge is posed by durability after the end of their useful life: the materials from which these items are made can take hundreds or thousands of years to decompose. Plastic bottles used as containers for drinking water exemplify the burden these items impose on the environment.More than 80% of plastic water bottles produced end up in landfills; it is estimated that more than 2 million tons of discarded water bottles currently reside in landfills, where they can be properly disposed of. Petition 870250095211, dated 10 / 17 / 2025, pp. 91 / 112 82 / 102 remain reasonably intact for centuries.

[126] Using the methods disclosed in the present invention, a flexible bio-based plastic substrate can be produced for the manufacture of plastic bottles by combining an existing matrix formed from bio-derived polymers with a population of redispersed NCEs produced as described above. The redispersed NCEs combined with the existing matrix can therefore form a bio-based composite matrix containing NCEs that can be used to replace non-degradable plastics currently processed into plastic bottles and similar containers. The use of redispersed NCEs in the composite matrix has the added advantage of creating a physical barrier to prevent oxygen molecules from penetrating the material.This plastic substrate can be designed to maintain its integrity over a predetermined lifespan, while also being adapted for decomposition (e.g., through biodegradation or composting) at the end of its designated lifespan.

[127] An exemplary formulation for producing a plastic bottle may include the following ingredients combined in an acetone solution or as solids in a high-shear mixer, such as a hot melt extruder (by weight, based on a total formulation weight of 100 g): • Cellulose acetate butyrate (CAB): 60 g • Redispersed NFC: 10 g • Rosin gum (GR): 25 g • Plasticizer (triacetin, triethyl citrate or acetyl triethyl citrate): 5 g.

[128] An exemplary formulation for producing a plastic bottle may include the following ingredients combined in an acetone solution or as solids in a high-shear mixer, such as an extruder. Petition 870250095211, dated 10 / 17 / 2025, pages 92 / 112 83 / 102 hot melt (by weight, based on a total formulation weight of 100 g): • Cellulose acetate butyrate (CAB): 52 g • Redispersed NFC: 17 g • Pulp fiber: 6 g • Rosin gum (GR): 20 g • Plasticizer (triacetin, triethyl citrate or acetyl triethyl citrate): 5g.

[129] Although specific quantities of these ingredients are given for the exemplary formulation above, it is understood that ranges of these ingredients may be added to create other formulations with advantageous properties. As an example, the nanocellulose component may be added in a range of about 1% to about 30%; CAB may be added in a range of about 30% to about 90%; the plasticizer may be added in a range of about 1% to about 35%, preferably in a range of about 15% to about 25%; rosin may be added in a range of about 5% to about 25%.In composite materials containing NCEs with a relatively higher amount of CAB, the CAB will have a greater influence on the properties of the overall composite material containing NCEs, compared to the influence of the NCEs; on the other hand, in composite materials containing NCEs with a relatively higher amount of redispersed NCEs, the NCEs will have a greater influence on the properties of the overall composite material containing NCEs, compared to the influence of the CAB.

[130] In the production of a suitable composite matrix containing NCE, the ingredients listed above may be added within ranges intended to optimize certain desirable properties. For example, a lower concentration of nanocellulose (e.g., between about 1% and about 15%, with less nanocellulose resulting in better optical clarity) may Petition 870250095211, dated 10 / 17 / 2025, pp. 93-112 84 / 102 can be used to achieve a desired degree of mechanical strength and optical clarity. A higher concentration of plasticizer compared to the transaction card formulation, for example, an amount of plasticizer above 5% by weight of the total recipe, will help achieve desirable external characteristics such as gloss or smoothness, as well as introducing more flexibility into the formed object. For products that require a more durable structure (e.g., shampoo bottles or pill containers), a formulation with less plasticizer can be used, and the container walls can be thicker. To manufacture the plastic bottle from the NCE-containing composite material, it can be heated and shaped using conventional techniques such as blow molding.

[131] When used to contain aqueous fluids, a plastic bottle made of NCE-containing composite material requires hydrophobic properties to prevent leaks. When used to contain oil-based liquids, such as cooking oils, oleophobic properties are needed to prevent leaks. Barrier production formulations can be integrated into NCE-containing composite materials used to form plastic bottles to produce the necessary OGWR properties. In some embodiments, hydrophobic properties are imparted to the NCE-containing composite material by including a hydrophobic agent in the existing matrix or in the NCE-containing composite, so that the product is water-resistant and more durable.In other embodiments, a bio-based hydrophobic coating may be painted onto the surface of the formed transaction card product or onto the surface of one or more layers of NCE-containing composite materials that are laminated together to form the transaction card. iii. Packaging for consumer goods Petition 870250095211, dated 10 / 17 / 2025, pp. 94 / 112 85 / 102

[132] Although there are similarities between the requirements for the manufacture of plastic bottles and the requirements for the manufacture of other types of packaging for consumer goods, the properties of these different product categories will differ because they are used for different purposes. For example, plastic bottles may have a considerably longer shelf life compared to other types of containers and must remain impermeable to water and / or oil throughout their shelf life, while packaging for other products may be designed for shorter shelf lives or less demanding performance requirements, and the materials used to form them may be adjusted accordingly. Typically, plastic bottles require significant structural strength to allow them to be transported and stacked while protecting their liquid contents. Petroleum-derived polymers have been extremely well-suited to meeting such performance requirements.However, when these materials are made from petroleum-derived polymers, they impose significant burdens on the environment both during manufacturing and disposal, regardless of their original intended use, because petroleum-derived polymers make these materials durable and resistant to disposal.

[133] NCE-containing composite materials can be designed to meet the performance needs of specific containers (such as balance between flexibility, strength and lightness) and, in addition, to allow for programmable decomposition. For example, to replace PVC in clamshell packaging and rigid cartons with high rigidity, an NCE-containing composite material can be provided with a higher concentration of NCE reinforcement in the bio-based matrix. As another example, a substitute for PET used in more flexible food containers may comprise an NCE-containing composite material with a lower concentration of NFC reinforcement. Petition 870250095211, dated 10 / 17 / 2025, pages 95 / 112 86 / 102 and higher plasticizer content. Methods for forming composite materials containing NCE in containers and packaging materials include those familiar in the industry, such as (without limitation) thermoforming, vacuum forming, injection molding, extrusion and the like.

[134] In some embodiments, composite matrices can be produced from existing biodegradable matrices with combinations of specialized properties, such as advantageous mechanical properties and barrier properties. For example, packaging materials can be formed from existing natural polymeric matrices, as described above, such as starch or derivatized cellulose (cellulose ethers or cellulose acetate), with barrier-producing materials optionally added and with reinforcement provided by redispersed NCEs. In some embodiments, small NCE particles, for example, molded as fibers or bundled balls of longer reinforced NCE fibers, can be incorporated into the overall matrix of the packaging material for greater shock absorption. The NCE yarns for this purpose may have intrinsic hydrophobicity and, optionally, may be treated with materials to improve their oil and grease resistance.Overall, these existing bio-based matrices incorporating redispersed NCE reinforcements (such as NCE fibers and / or NCE-reinforced polymer fibers) can be used for many packaging applications, including peanut packaging, bladders, cardboard boxes, etc.

[135] Packaging in general requires OGWR properties suitable for use. Packaging or a container intended for use with food products must contain any food-related fluids within the enclosure and must protect the contents from exposure to external moisture, grease, and oil. The packaging or container must also remain structurally sound. Petition 870250095211, dated 10 / 17 / 2025, pp. 96 / 112 87 / 102 intact, even if it comes into contact with moisture, grease, or oil. The OGWR attributes of the packaging or container contribute to its structural stability, preventing oil, grease, or water from impairing its strength or resilience. Barrier production formulations can also be used to produce OGWR properties in plain NCE-based materials and in NCE-containing composite materials used as packaging or containers.

[136] For example, a pouch, capsule or other packaging article made of OGR or WVR formed from NCEs, as described in the present invention, can serve as a container for condiments, sauces or other liquid or gelatinous food substances, allowing the consumer to open the packaging and dispense the food substance as desired. This packaging can conveniently contain and dispense aqueous or oil-based food substances such as soy sauce, ketchup, mustard, mayonnaise, salad dressings, dairy products and the like, thereby reducing the plastic waste associated with conventional packaging for such food substances.

[137] An exemplary formulation for producing containers for substances not sensitive to oxygen (e.g., salt / pepper) may include the following ingredients (by weight, based on the total weight of the 100 g formulation): • Methylcellulose (MC): 85.5 g • Xylitol: 4.5 g • NCE: 10 g.

[138] An exemplary formulation for producing containers for oxygen-sensitive materials (e.g., transparent films for meat trays) may include the following ingredients (by weight, based on the total weight of the 100 g formulation): • Polyvinyl alcohol (PVA): 23.75 g Petition 870250095211, dated 10 / 17 / 2025, pp. 97 / 112 88 / 102 • Polyvinyl acetate (PVAc): 23.75 g • Methylcellulose (MC): 42.75 g • Maltitol: 4.75 g • NCE: 5 g.

[139] An exemplary formulation for producing a water-resistant barrier, to be mixed into a paste to be molded and thermoformed (by weight, based on a total formulation weight of 1000 g dry): • 0.4% by weight of aqueous pulp paste: 8325 g (33.33 g dry weight) • Redispersible NCEs: 7.9175 g (NCE) and 23.7525 g (MC) • Rosin: 35 g (in Ethanol: 50 g) • An exemplary formulation for producing an oil, grease and water resistant barrier, to be mixed or used as a coating (by weight, based on a total formulation weight of 100 g) • Cellulose acetate butyrate (CAB): 10 g • Rosin: 10 g • Acetone: 79 g • Plasticizer (e.g., but not limited to triacetin, triethyl citrate, acetyl triethyl citrate, tributyl citrate): 1 g.

[140] An exemplary formulation for such a hydrophobic coating includes the following ingredients combined to form a solution in acetone (by weight, based on the total weight of the 100 g formulation): • Cellulose acetate (CA): 7 g • Ethanol: 14 g • Acetone: 71 g • Rosin gum (GR): 7 g • Plasticizer (triacetin, triethyl citrate or acetyl triethyl citrate): lg. Petition 870250095211, dated 10 / 17 / 2025, pp. 98 / 112 89 / 102

[141] Adding a barrier production formulation for OGWR purposes is especially useful in the preparation of versatile and simple NCE-based materials: their mechanical properties are primarily provided by the simple NCE-based matrix itself, and this matrix, especially if predominantly pulp, is vulnerable to the penetration of oil, grease, and water. Adding a barrier production formulation to such a simple NCE-based material can provide resistance to essential oils, greases, or water, and thus protect the contents from such incursions and further protect the integrity of the material itself or the packaging or containers made from it. iv. Films and thin sheets

[142] For example, thin films and sheets used as wrappers or containers (such as stretch films, plastic bags, garbage bags, etc.) have requirements for flexibility, elasticity, oil and water resistance, and strength. Currently, they are typically made of polyethylene. As a substitute, a bio-based composite matrix containing NCE can be produced by using a cellulosic polymer as a matrix-forming element in the existing matrix and modifying this matrix or the final NCE-containing composite matrix to produce the desired elasticity.Potential cellulose derivatives include, but are not limited to, CMC (carboxymethylcellulose), CMCNa (sodium carboxymethylcellulose salt), CA (cellulose acetate), CDA (cellulose diacetate), cellulose triacetate (CTA), CAB (cellulose acetate butyrate), CAPh (cellulose acetate phthalate), CAP (cellulose acetate propionate), EC (ethylcellulose), HEC (hydroxyethylcellulose), EHEC (ethyl hydroxyethylcellulose), HPC (hydroxypropylcellulose), HPMC (hydroxypropylmethylcellulose), HPMCP (hydroxypropylmethylcellulose phthalate), HPMCAS (hydroxypropylmethylcellulose acetate). To achieve high elasticity, large tangles of polymer chains can be produced in the existing matrix. A. Petition 870250095211, dated 10 / 17 / 2025, pp. 99 / 112 90 / 102 Incorporation of long-chain crosslinkers into the main chain of the natural polymer via esterification can form a highly entangled and bonded structure to provide the desired elasticity. For example, any mono- or dicarboxylic acid (e.g., but not limited to sebacic acid) can be crosslinked to the cellulosic polymer (e.g., cellulose diacetate) in the presence of an acid catalyst. The existing matrix thus prepared can be combined with the redispersed NFCs to form the NCE-containing composite matrix with suitable strength and elasticity. Other ingredients can be included in the existing matrix or the NCE-containing composite matrix to form the final NCE-containing composite material that can be used to form specific manufactured articles using current industry methods.

[143] Composite films or sheets formed from NCE-containing composite materials can be transparent or translucent, as desired, with superior mechanical properties such as tear resistance, as well as biodegradability. On the other hand, conventional transparent or translucent films and sheets, such as those used in Ziplock bags, garbage bags, supermarket bags and the like, are normally formed from polyolefins, such as polyethylene and polypropylene, which are derived from petroleum and degrade slowly. In some embodiments, films and sheets formed by incorporating NCEs, as described in the present invention, can be used for a multitude of other packaging applications where strength is desirable, to provide a biodegradable alternative to conventional polyolefin-based packaging materials.

[144] A film or sheet with barrier properties, such as OGWR properties, offers important advantages when employed in commercial contexts. For example, the film or sheet can be used as Petition 870250095211, dated 10 / 17 / 2025, pp. 100 / 112 91 / 102 a wrapper or packaging with optimized resistance to oils and greases and / or optimized resistance to water or water vapor, for use as a wrapper or packaging for delicate products. In embodiments, the film or sheet may be further adjusted to improve oil resistance when encountering oils or oil suspensions, to optimize water resistance when encountering aqueous solutions or suspensions, to add strength, or to reduce gas permeability to produce more airtight packaging properties. In some embodiments, the NCE-containing composite materials with OGWR properties, as disclosed in the present invention, may be modified by adding additional polymers or particles to the matrix material (e.g., PVA, PVOH, hydroxyethyl butyrate, exfoliated clay, and the like) to improve their airtight properties.

[145] For example, films or sheets with OGWR properties that are formed from NCE-containing composite materials can be used as components or entire containers for liquids such as milk (e.g., shelf-stable milk cartons), to be sterilizable by techniques such as ultraviolet sterilization and other methods familiar to those skilled in the art. In some embodiments, such films or sheets can be transparent or translucent, with superior mechanical properties such as tear resistance or stiffness, offering a viable alternative to conventional packaging and airtight films made of polyolefins.

[146] As another example, films and sheets with OGWR properties formed from NCE-containing composite materials can be used as wrappers for food products. The existing matrix that contributes to the NCE-containing composite materials used for these purposes may comprise conventional biodegradable polymers, naturally derived, such as cellulose ethers, cellulose esters, starch ethers, Petition 870250095211, dated 10 / 17 / 2025, pages 101 / 112 92 / 102 starch esters, polyvinyl alcohol, hydroxyethyl butyrate, or any combination thereof. In these NCE-containing composite materials, NCEs can contribute to improved mechanical strength, stiffness, and tear resistance of the material, which can be enhanced by the inclusion of dispersing additives in the material. OGWR properties in the film or sheet can be produced by the inclusion of a barrier-producing formulation with oleophobic and / or hydrophobic properties. In some embodiments, additive NCEs can be prepared to provide OGWR properties to the NCE-containing composite material, for example, if these fibers are coated with films that produce these properties. With appropriate plasticizers, cellulose acetate or other hydrophobic and elastic materials can be added to impart elasticity to the coated fibers, or they can be incorporated into the polymer matrix to provide flexibility and elasticity to the products.For products that must be impermeable to gases, polyvinyl alcohol or polyvinyl acetate / polyvinyl alcohol copolymers can be used.

[147] In more detail, a composite film or sheet containing NCE can be prepared from an existing matrix comprising biodegradable materials such as cellulose ethers, cellulose esters, starch ethers, starch esters, polyvinyl alcohol, hydroxyethyl butyrate, polyvinyl acetate, or any combination thereof; additives can then be supplied to produce the specific properties for a particular commercial need. As mentioned earlier, the properties of OWGR are especially advantageous; various additives, as described above, can act as barrier-producing formulations to produce these properties. Other additives can be included in the NCE-containing composite material to produce other properties. For example, a film or Petition 870250095211, dated 10 / 17 / 2025, pp. 102 / 112 93 / 102 sheet that requires gas barrier properties can be made of a composite material containing NCE which includes polyvinyl alcohol, polyvinyl acetate, copolymers thereof or mixtures thereof.

[148] The proportions of ingredients in the NCE-containing composite matrix and in the NCE-containing composite materials can also be adjusted to improve certain properties. In some embodiments, NCEs can be added in concentrations ranging from 1% by weight to 10% by weight to improve mechanical strength. In some embodiments, an existing matrix can be prepared to increase the physical integrity of the resulting NCE-containing composite matrix by using polymers selected for physical integrity and selecting high molecular weight versions thereof (e.g., in molecular weight ranges from tens of thousands of g / mol to millions of g / mol, such as from one hundred thousand g / mol to millions of g / mol). Plasticizers can be incorporated in concentrations ranging from, for example, about 1% by weight to about 50% by weight, or about 1% by weight to about 10% by weight, or about 5% to about 15%, to impart flexibility.Useful plasticizers may include, but are not limited to, 1,2-propanediol, xylitol, erythritol, maltitol, and mannitol, or fatty acids such as caprylic acid, caproic acid, or similar acids. Fatty acids used as plasticizers can be beneficial in barrier applications due to their hydrophobic nature. For large-scale processing, the complete formulation (including redispersed NCEs, existing matrix(es), plasticizers, barrier production formulations, and other desired additives) can be mixed in a large tank and pumped to an extruder with a slit die. The extruded sheets can then be pressed and / or perforated with cylinders. After drying (cylinders or heated ovens), the pressed sheets can be collected onto cylinders or shaped into bags or sachets. Petition 870250095211, dated 10 / 17 / 2025, pages 103 / 112 94 / 102 (v. Hollow cylinders for flexible tubing, such as straws)

[149] One application that combines the characteristics of biodegradability, strength, and barrier properties is the use of NCE materials to form a hollow cylinder that can be used to form a flexible tube, for example, for use as a biodegradable straw. Because straws are designed to be used with a variety of liquids, including alcohol, fats, acids, and the like, at various temperatures, and because straws require sufficient strength to withstand deformation during normal use, there has been a trend toward using more durable plastics that are not biodegradable; biodegradable materials alone do not have the liquid tolerance and strength to withstand the stresses that straws typically face. The use of NCE materials alone or in combination with other biodegradable materials can provide the necessary liquid tolerance and strength while allowing the product to be biodegradable.

[150] A simple NCE-based material, such as described above, can be molded as a sheet and rolled into a hollow cylinder to act as a straw. This material can be predominantly pulp-based, so that it is economically formed with pulp or pulp-based bulking agents as the main component, in combination with the simple NCE-based matrix. Barrier production formulations are advantageous for providing the hydrophobicity or oleophobicity required by the intended end use of the hollow cylinder, such as a straw. As an example, bagasse or other fibrous agricultural waste products can be a source of NCEs that are redispersed according to the methods disclosed in the present invention; such NCEs can then be blended into a formulation comprising CA, rosin, and plasticizer to produce an NCE-containing composite material that can be extruded to form straws. Petition 870250095211, dated 10 / 17 / 2025, pages 104 / 112 95 / 102

[151] In other embodiments, a composite material containing NCEs can be formed with the desired OGWR properties, for example, by using a cellulose-based material, such as methylcellulose, for an existing matrix in combination with additive NCEs. In such a composite, cellulose acetate or other materials can be selected to produce hydrophobicity. For example, certain biodegradable LCST polymers or hydrophobic cellulosic polymers, such as CA or CAB, or other materials such as polyvinyl alcohol or copolymers thereof, such as polyvinyl acetate / polyvinyl alcohol, lipids, waxes, hydrophobic starch, fatty acids, or any other similar hydrophobic polymers can be included in the NCE-containing composite material to increase its hydrophobicity.

[152] In some embodiments, NCE-containing composite materials with OGWR properties can be mixed in an aqueous vehicle to produce a viscous mixture that can then be formed as a sheet or extruded as a hollow cylinder. Reinforcing materials, such as spun hydrogel fibers, can be added to the composite to improve strength and flexibility. For embodiments with OGWR properties, the ratio of OGR or WVR ingredients to NCEs can be from about 1:1 to about 12:1, or between about 3:1 to about 9:1. In another embodiment, a 2-3% NCE suspension can be mixed with an MC or other cellulose-containing suspension. In some embodiments, the NCE formulation may comprise CMFs as well as CNFs, or may comprise more CMFs than CNFs, or may consist essentially of CMFs, with the CMF to CNF ratio being adjusted to optimize the strength of the final formulation.In some embodiments, regular pulp can be used in addition to or instead of derivatized cellulose in the mixture. Eliminating or reducing the amount of glycerol or other plasticizer used in the formulation can improve the stiffness of the product. Petition 870250095211, dated 10 / 17 / 2025, pages 105 / 112 96 / 102 straw. EXAMPLES Example 1: Production of redispersible NCE sheets

[153] Redispersible NCE sheets were produced by combining a drying / dispersing additive with an NCE paste and then drying it at high temperature in an oven. There are several combinations and multiple ratios of additives that can be used to create dry redispersible NCE sheets. For this specific example, the polymer hydroxypropyl methylcellulose (HPMC) was used as a dispersing additive in combination with nanofibrillated cellulose (NFC) at a ratio of 5:1 NFC:HPMC. The ingredients were combined in an aqueous solution consisting of 1.25% by weight of NFC. Table 1: Ingredients for creating redispersible NFC. 3% by weight of NFC Water HPMC 41.67 g (1.25 g dry) 58.08 0.25 g

[154] First, 0.25 g of HPMC was added to 58.08 g of water in a beaker while stirring at medium-high speed for about 15 minutes. After that, the stirring speed was reduced to the lowest setting, continuing to mix until all bubbles on the surface dissipated. After removing the beaker from the stirrer plate, 41.67 g of NFC at 3% by weight (1.25 g of NFC by dry weight) were added. These ingredients were then mixed using a stirrer at 250 rpm for 15 minutes. The fully mixed sample was then poured onto a silicone mat and spread evenly over the mat using a dosing blade set to 1.5 mm thickness. The mat with the sample was placed in an oven and dried at 60 °C until the sample was completely dry (about 2 hours). The dried sheet was slowly removed from the silicone mat. As a result of these procedures, the previously non-dispersible NFCs Petition 870250095211, dated 10 / 17 / 2025, pp. 106 / 112 97 / 102 were modified with drying / dispersing additives so that they could be redispersed when combined with water. A dry sheet containing such redispersible NFCs was produced by these procedures. Example 2: Formulation and manufacture of composite transaction card sheets containing NCE.

[155] The materials used in this example may include: • Cellulose acetate butyrate (Sigma Aldrich) • Rosin gum (Sigma Aldrich) • Calcium carbonate (Sigma Aldrich) • Stearic acid (Sigma Aldrich) • Triacetin (Sigma Aldrich) • Triethyl 2-acetyl citrate (Sigma Aldrich) • Hydroxymethylpropylcellulose: Sigma-Aldrich • Acetone (McMaster Carr) • Capryl glucoside (Berkley Green).

[156] The equipment used in this example may include: • Corning stirring plate • ONiLAB suspended agitator • CRUSHANUG Ultimate Design 5-ton hydraulic heat press machine with 3x5 inch double heated plates • Dia Vac pump • Binder forced convection oven.

[157] This experiment tested initial formulations for producing a credit card with the structure of a composite material containing NCEs, wherein the NCE-containing composite material comprised a matrix containing redispersed NCEs. There were three main steps in this process: matrix formulation, reinforcement addition, and heat press fabrication. Petition 870250095211, dated 10 / 17 / 2025, pages 107 / 112 98 / 102

[158] Matrix formulation: An acetone solution containing 12% by weight of matrix ingredients was formed by adding each of the desired components, one by one, to a beaker of acetone while the beaker was mixing on a magnetic stir bar. The matrix ingredients were added in a designated order, allowing sufficient time for the mixture to homogenize before adding the next component. Subsequently, CAB, CA, or a combination of the two were added and stirred until no lumps remained (~30 minutes to 1 hour). Finally, but optionally, the plasticizer was added to the mixture and stirred for at least 15 minutes to obtain a homogeneous mixture.

[159] The following ingredients were used to create three different matrices. The ingredients are listed in the order in which they were added to the acetone beaker. Specific quantities of each component used are described in Table 2 below. • Matrix 1: Rosin, capryl glucoside (CG), CAB, TEA • Matrix 2: Stearic acid, CC, CAB, TEA • Matrix 3: Rosin, stearic acid, CC, CAB, triacetin Table 2: Recipes for Matrices 1, 2 and 3 Matrix CAB Rosin Stearic Plasticizer CC CG Acetone 1 73 g 20.4 5.6 0 g 0 g 1 g 733 g 2 67 g 0 g 8.3 15 g 10 g 0 g 733 g 3 67 g 17 2 8 g 6 0 g 733 g

[160] The following ingredients were used to create three different matrices. The ingredients are listed in the order in which they were added to the acetone beaker. Specific quantities of each component used are described in Table 3 below.

[161] Addition of the formulation containing redispersed NCEs: Sheets of redispersible NCEs prepared as described in Example 1 were added to a large beaker and vigorously mixed with a stirrer suspended by Petition 870250095211, dated 10 / 17 / 2025, pp. 108 / 112 99 / 102 minutes. In these experiments, we used equal amounts of dry NCE and CAB. Acetone was added to the fully dispersed fibers and thoroughly mixed with a stirring rod. The amount of acetone included was 40% of the weight of the redispersed NFC solution. Once the mixture was homogenized, the reinforcement was ready to be added to the matrix. The table below (Table 3) lists the amount of NCE and acetone needed for addition to Matrices 1, 2, and 3. TABLE 3 Matrix Sheet of Dispersible NCE Acetone 1 73 g 29.2 g 2 67 g 26.8 g 3 67 g 26.8 g

[162] The redispersed NCE acetone mixture was then added to the beaker containing the matrix ingredients and mixed on the overhead stirrer using a turbine stirrer for 10 minutes until homogeneous.

[163] Fabrication of heat presses: The final step of this experiment involved using a heat press to form the newly created composite mixture into a fine structure, such as that which could be employed in transaction cards. Before the material was inserted into the heat press, excess acetone was removed using a sieve and a vacuum filtration pump. The filtration system consisted of a vacuum pump and two Erlenmeyer flasks, all connected by tubing. A sieve was taped to a funnel and connected to the first flask with tubing. The composite material was then placed in the sieve and the vacuum was applied. The liquid was extracted from the composite material through the sieve and then the funnel; the liquid then passed through the tubing to be collected in the first Erlenmeyer flask. When no more liquid was being pulled through the funnel, this step was complete. The composite material containing NCE solidified after the removal of excess liquid.It wasn't completely dry, a desirable state for keeping the material together until it was pressed by the heat press. Petition 870250095211, dated 10 / 17 / 2025, pages 109 / 112 100 / 102

[164] The heat press was switched on and set to 110 °C. Five grams of the NCE-containing composite material were manually pressed into a flat rectangular shape (~3 mm thick) and placed between two pieces of silicone mat. After heating the press, the silicone mats containing the composite material were placed on the lower plate of the press. The upper plate was then lowered to begin heating the material by lightly touching the upper silicone mat. After two minutes, the plate was lowered a little further to apply some pressure. These processes were repeated until sufficient pressure was applied to press the material to the desired thickness, for example, a 1 mm thick sheet that could be cut into shapes that would be useful for transaction cards, such as credit cards. Example 3: Formulation and manufacture of composite transaction card sheets containing NCE.

[165] Matrix formulation: An acetone solution containing 10% by weight of matrix ingredients was formed by adding each of the desired components, one by one, to a beaker of acetone while the beaker was mixed on a magnetic stir bar. The matrix ingredients were added in a designated order, allowing sufficient time for the mixture to homogenize before adding the next component. First, the resin was added to the acetone, followed by CAB or CA, and finally, a plasticizer. Mixing continued until the solution was homogeneous before adding more ingredients.

[166] Sheets of redispersible NCEs prepared as described in Example 1 were added to a large beaker and vigorously mixed with a suspended stirrer for 30 minutes. The amount of NCE used depended on the desired final stiffness of the material. The cards were produced with Petition 870250095211, dated 10 / 17 / 2025, pages 110 / 112 101 / 102 a higher NFC load of around 28% and lower loads of around 17%. The pulp was then added to the redispersed NCE solution and mixed. Next, acetone was added to the solution.

[167] Acetone was added to the fully dispersed and well-mixed fibers with a stirring rod. The amount of acetone included was 40% of the weight of the redispersed NFC solution. After the mixture was homogenized, the reinforcement was ready to be added to the matrix with a 23x load relative to the solid fibers (1:23 pulp+NCE: acetone). The addition of acetone aided in the addition of hydrophilic cellulose fibers in a hydrophobic solution. Ideally, low levels of pulp solids and redispersed NCEs in water were used to aid in homogeneous mixing. After the addition of acetone, the solution was again mixed under high shear with a suspended stirrer. Capryl glycoside was also added to this solution to help bind the polar and non-polar components during mixing in the next step. After the matrix and reinforcement were thoroughly mixed, the two solutions were ready to be combined.The reinforcing solution was added slowly to the matrix solution, which was being vigorously mixed under high shear conditions.

[168] The table below (Table 4) lists exemplary formulations of cards produced with CAB. These formulation ratios can also be applied to samples produced by extrusion. TABLE 4 Hydrophilic solution Hydrophobic solution Pulp NFC Goat Rosin CAB TEA 91.7 275.2 22.9 156 412.8 41.3 76.2 228.7 19.1 172.8 457.4 45.7 57 170.9 14.2 193.7 512.8 51.3

[169] Manufacturing of thermal presses: The final stage of this experiment involved the use of a thermal press to form the newly compound mixture. Petition 870250095211, 10 / 17 / 2025, p. 111 / 112 102 / 102 created in a thin structure, such as that which could be used in transaction cards or other rigid packaging applications. Before heat pressing the material, some of the solvent was evaporated by heating the material uniformly in an oven at 50 to 70 °C for 5 to 30 minutes. The heat press was switched on and set to 120 °C. A rectangular mold was placed in the press on a silicone mat and filled with the composite material. A mesh screen and a second silicone mat were placed on top of the mold. The top plate was then lowered to begin heating the material by lightly touching the top silicone mat. After two minutes, the plate was lowered a little further to apply more pressure.These processes were repeated until sufficient pressure was applied to press the material to the desired thickness and evaporate the solvent, for example, a 1 mm thick sheet that could be cut into shapes that would be useful for transaction cards, such as credit cards.

[170] Although this invention has been particularly shown and described with reference to its preferred embodiments, it will be understood by those skilled in the art that various alterations in form and details may be made to it without departing from the scope of the invention covered by the appended claims. All published or unpublished United States patents and United States patent applications cited in the present invention are incorporated by reference. All published foreign patents and patent applications cited in the present invention are incorporated by reference. All other published references, documents, manuscripts, and scientific literature cited in the present invention are incorporated by reference. The relevant teachings of all patents, published applications, and references cited in the present invention are incorporated by reference in their entirety. Petition 870250095211, dated 10 / 17 / 2025, page 112 / 112

Claims

1 / 6 CLAIMS 1. NCE-based simple material, characterized in that it comprises an NCE-based simple matrix, wherein the NCE-based simple matrix comprises a population of redispersible NCEs treated with a drying / dispersion additive comprising a lower critical solution temperature (LCST) polymer; wherein the NCE-based simple matrix provides an architectural framework for the NCE-based simple material; and wherein the NCE-based simple material further comprises a barrier formulation.

2. Simple NCE-based material according to claim 1, characterized in that the barrier formulation comprises a substance selected from the group consisting of cellulosic polymers, lipids, proteins, diluents, fatty acids, a resin acid and combinations of resin acids.

3. Simple NCE-based material according to claim 2, characterized in that the barrier formulation comprises a resin acid or a combination of resin acids.

4. Simple NCE-based material according to claim 1, characterized in that the barrier formulation comprises an oleophobic substance selected from the group consisting of MC, HPMC, CMC, NaCMC, CA, CAB, chitosan, rosin, lignin and a vegetable protein.

5. Simple NCE-based material according to claim 1, characterized in that the barrier formulation comprises a hydrophobic substance selected from the group consisting of MC, CA, CAB, chitosan, rosin, hydrophobized starch, lignin and a vegetable protein.

6. Simple material based on NCE, according to claim 1, Petition 870250091197, dated 06 / 10 / 2025, p. 289 / 294 2 / 6 characterized in that it further comprises one or more additive substances selected from the group consisting of a bulking agent, a reinforcing agent or an appearance-modifying agent, or a combination thereof.

7. Simple material based on NCE, according to claim 6, characterized in that one or more additive substances are a bulking agent.

8. Simple NCE-based material according to claim 7, characterized in that the bulking agent comprises pulp or a pulp-based substance.

9. Simple NCE-based material according to claim 8, characterized in that the simple NCE-based matrix is ​​predominantly pulp.

10. Simple NCE-based material according to claim 7, characterized in that the bulking agent comprises diluent particles.

11. Simple NCE-based material according to claim 10, characterized in that the diluent particles comprise plant-derived organic materials.

12. Simple material based on NCEs, according to claim 6, characterized in that one or more additive substances are a reinforcing agent, and the reinforcing agent comprises an additional quantity of NCEs.

13. Plastic substrate, characterized in that it comprises the simple NCE-based material defined in claim 1.

14. Article of manufacture, characterized in that it comprises the plastic substrate defined in claim 13 molded into a formed article. Petition 870250091197, dated 06 / 10 / 2025, pp. 290 / 294 3 / 6 15. Article of manufacture, according to claim 14, characterized in that the formed article is a container.

16. Article of manufacture, according to claim 15, characterized in that the container is a container for a food product.

17. A method for manufacturing a plastic article, characterized in that it comprises a simple NCE-based material in a flexible state, comprising: a. producing a simple NCE-based material comprising redispersible NC elements, wherein the simple NCE-based material is produced by the sub-steps of: i. providing an initial suspension comprising NC elements suspended in a fluid medium; ii. combining a drying / dispersing additive with the initial suspension to form a flexible suspension of redispersible NCEs; and iii. adding one or more additive substances to the flexible suspension of redispersible NCEs, maintaining their flexibility, thus forming the simple NCE-based material in a flexible state; b. forming or shaping the simple NCE-based material in the flexible state into a desired configuration, thus manufacturing the plastic article.

18. Method according to claim 17, characterized in that one or more additive substances are selected from the group consisting of boosting agents, barrier formulations and bulking agents, and a combination thereof.

19. Manufacturing method according to claim 17, characterized in that the forming or shaping step comprises extrusion. Petition 870250091197, dated 06 / 10 / 2025, pp. 291 / 294 4 / 6 20. NCE-containing composite material, characterized in that it comprises an NCE-containing composite matrix, wherein the NCE-containing composite matrix comprises a population of redispersible NCEs treated with a drying / dispersion additive comprising a lower critical solution temperature (LCST) polymer, and an existing matrix; wherein the redispersible NCEs are integrated into the existing matrix, and wherein the existing matrix provides an architectural framework for the NCE-containing composite material; and wherein the NCE-containing composite material further comprises a barrier formulation.

21. Composite material containing NCE, according to claim 20, characterized in that the existing matrix comprises a bio-based polymer.

22. Composite material containing NCE, according to claim 21, characterized in that the bio-based polymer comprises a cellulose derivative.

23. Composite material containing NCE, according to claim 22, characterized in that the cellulose derivative is a polyhydroxyalkanoate.

24. Composite material containing NCE, according to claim 20, characterized in that the existing matrix comprises a petroleum-derived polymer.

25. Composite material containing NCE, according to claim 24, characterized in that the petroleum-derived polymer was derived from a plastic material that was recycled.

26. Composite material containing NCE, according to claim 20, characterized in that the barrier formulation comprises a substance selected from the group consisting of cellulosic polymers, lipids, proteins, diluents, fatty acids, a resin acid and combinations of resin acids.

27. Composite material containing NCE, according to claim 26, characterized in that the barrier formulation comprises a resin acid or a combination of resin acids.

28. NCE-based composite material according to claim 20, characterized in that it further comprises one or more additive substances selected from the group consisting of a bulking agent, a reinforcing agent or an appearance-modifying agent, or a combination thereof.

29. Composite material containing NCE, according to claim 20, characterized in that one or more additive substances produce in the NCE-containing composite material a property selected from the group consisting of structural strength, resilience, elasticity, water resistance, and oil and grease resistance.

30. Plastic substrate, characterized in that it comprises the composite material containing NCE defined in claim 20.

31. A manufactured article, characterized in that it comprises the plastic substrate defined in claim 30 molded into a formed article.

32. A manufactured article according to claim 31, characterized in that the formed article is selected from the group consisting of transaction cards, containers for liquids, containers for food products, packaging materials for consumer goods, films and thin sheets, and hollow cylinders for flexible tubing.

33. Method of manufacturing a plastic article, characterized by Petition 870250091197, dated 06 / 10 / 2025, pp. 293 / 294 6 / 6, in the fact that it comprises a composite material containing NCE in a flexible state, comprising: a. producing a composite material containing NCE comprising redispersible NC elements, wherein the NCE-containing composite material is produced by the substeps of: i. providing an initial suspension comprising NC elements suspended in a fluid medium; ii. combining a drying / dispersing additive with the initial suspension to form a flexible suspension of redispersible NCEs; iii. integrating the flexible suspension into an existing matrix, thereby forming a composite matrix containing NCE in the flexible state; iv. adding an additive substance and maintaining the flexibility of at least one of the initial suspension, the flexible suspension, the existing matrix and the NCE-containing composite matrix, thereby forming the NCE-containing composite material in the flexible state; and b.To form or mold the NCE-containing composite material in a flexible state into a desired configuration, thereby manufacturing the formed article.

34. Method according to claim 33, characterized in that the additive substance is selected from the group consisting of reinforcing agents, barrier formulations and bulking agents.

35. Method according to claim 33, characterized in that the forming or shaping step comprises extrusion. Petition 870250091197, dated 06 / 10 / 2025, pp. 294 / 294

Images