阅读说明：本技术 植物基功能材料 (Plant-based functional materials ) 是由 马克·罗德里格斯加西亚 图马斯·诺尔斯 阿维亚德·莱文 镰田彩花 于 2020-03-06 设计创作，主要内容包括：本发明涉及植物基材料、其制造方法和包含植物基材料的生物材料。(The present invention relates to a plant-based material, a method for manufacturing the same, and a biomaterial comprising the plant-based material.)

1.A plant-based structured material, wherein the structured material is: a film, a thin film, a micropatterned film (or film), a micro-or nanostructured film, a microgel, a microcapsule, a microbead, a bioscaffold, a biological support, a sponge, a microsponge, a hard capsule, or a functional coating.

2. The plant-based structured material of claim 1, wherein said structured material is a microcapsule.

3. The plant-based structured material of claim 1, wherein said structured material is a microbead.

4. The plant-based structured material of claim 1, wherein said structured material is a biological scaffold or a biological support.

5. The plant-based structured material of claim 1, wherein said structured material is a sponge or a microsponge.

6. The plant-based structured material of claim 1, wherein said structured material is a hard capsule.

7. The plant-based structured material of claim 1, wherein said structured material is a film or membrane.

8. The plant-based structured material of claim 1, wherein said structured material is a micropatterned film, or a micro-or nanostructured film.

9. The plant-based structured material of claim 1, wherein said structured material is a microgel.

10. The plant-based structured material of claim 1, wherein said structured material is a functional coating.

11. The plant-based structured material of any preceding claim, wherein said structured material comprises beta-sheet crystals of a plant protein.

12. The plant-based structured material of claim 11, wherein said structured material comprises at least 40% β -sheet crystals, at least 50% β -sheet crystals, at least 60% β -sheet crystals, at least 70% β -sheet crystals, at least 80% β -sheet crystals, or at least 90% β -sheet crystals.

13. The plant-based structured material according to any one of the preceding claims, wherein said structured material comprises a plant-based protein having a secondary structure with at least 40% intermolecular β -sheet, at least 50% intermolecular β -sheet, at least 60% intermolecular β -sheet, at least 70% intermolecular β -sheet, at least 80% intermolecular β -sheet or at least 90% intermolecular β -sheet.

14. The plant based structured material according to any preceding claim, wherein the storage modulus (G') of the structured material at 10rad/s is greater than 500Pa, greater than 1000Pa, greater than 2500Pa, greater than 3000Pa, greater than 4000 Pa.

15. The plant-based structured material of any preceding claim, wherein said structured material has a young's modulus of more than 20 MPa; preferably more than 50MPa, more than 80MPa, more than 100MPa, more than 200MPa, more than 300MPa, more than 400MPa, more than 500MPa or more than 600 MPa.

16. The plant-based structured material according to any one of the preceding claims, wherein said structured material comprises protein aggregates having an average size of less than 200nm, preferably less than 150nm, less than 125nm, less than 100nm, less than 90nm, less than 80nm, less than 70nm, less than 60nm, less than 50nm, less than 40nm or less than 30 nm.

17. The plant-based structured material of any preceding claim, wherein the plant-based structured material is capable of being thermally reversibly gelled.

18. The plant based structured material according to claim 17, wherein upon heating at elevated temperature and/or by applying mechanical agitation, the plant based structured material will form a protein solution having a storage modulus below 250Pa, preferably below 100Pa, below 50Pa or below 10 Pa.

19. The plant-based structured material of any preceding claim, which is formed via a thermally reversible cold-set gelling process.

20. A plant-based thermoreversible hydrogel.

21. The plant-based thermoreversible hydrogel of claim 20, wherein said hydrogel is molded into, formed into, or otherwise formed into a structured shape by a microfluidic device; the structured hydrogel is then optionally dried.

22. A composite material comprising a plant based material according to any preceding claim, and one or more other biopolymers, such as proteins and/or polysaccharides.

23. A food product, cosmetic product, pharmaceutical product, medical device or biomaterial comprising the plant-based structured material according to claims 1 to 19, the plant-based thermoreversible hydrogel according to claim 20 or 21 or the composite material according to claim 22.

24. A method of producing a plant based material, the method comprising:

a) forming a solution comprising one or more plant-based proteins in a solvent system, wherein the solvent system comprises a miscible cosolvent; wherein the first co-solvent increases the solubility of the one or more plant-based proteins and the second co-solvent decreases the solubility of the one or more plant-based proteins; and

b) inducing a sol-gel transition of the protein in the solution to form a plant-based protein hydrogel.

25. The method of claim 24, the method comprising:

c) forming the plant-based protein hydrogel into a structured material.

26. The method of claim 25, wherein the plant-based protein hydrogel is formed into a structured material before, during, or after the sol-gel transition.

27. The method according to any one of claims 24 to 26, wherein the plant-based protein hydrogel is molded into a structured material or wherein the plant-based protein hydrogel is formed into a structured material using a microfluidic device.

28. The method according to any one of claims 24 to 27, wherein the method is used to produce a structured material; for example, a film, a thin film, a micropatterned film (or film), a micro-or nanostructured film, a microgel, a microcapsule, a microbead, a bioscaffold, a bioholdfast, a sponge, a microsponge, a hard capsule, or a functional coating.

29. The method of any one of claims 24 to 28, wherein the one or more plant proteins are obtained from soy, pea, rice, potato, wheat, zein, or sorghum; preferably the one or more vegetable proteins are selected from soy protein, pea protein, potato protein and/or rice protein.

30. The process of any one of claims 24 to 29, wherein the first co-solvent is an organic acid; preferably acetic acid and/or an alpha-hydroxy acid; wherein the alpha-hydroxy acid may preferably be selected from glycolic acid, lactic acid, malic acid, citric acid and/or tartaric acid; among the particularly preferred organic acids are acetic acid and/or lactic acid.

31. The method of any one of claims 24 to 30, wherein the second co-solvent or the additional co-solvent or co-solvents is an aqueous buffer; preferably selected from the group consisting of water, ethanol, methanol, acetone, acetonitrile, dimethyl sulfoxide, dimethylformamide, formamide, 2-propanol, 1-butanol, 1-propanol, hexanol, tert-butanol, ethyl acetate or hexafluoroisopropanol, particularly preferably water and/or ethanol; further, water is particularly preferred.

32. The method according to any one of claims 24 to 31, wherein the solvent system comprises a co-solvent ratio of about 20-80% v/v, preferably about 20-60% v/v, about 25-55% v/v, about 30-50% v/v, about 20%, about 30%, about 40%, about 50% or about 60% v/v, most preferably about 30-50% v/v.

33. The method according to any one of claims 24 to 32, further comprising subjecting the protein solution comprising one or more plant based proteins and a solvent system to mechanical shearing, preferably sonication.

34. The method of any one of claims 24 to 33, wherein the protein solution is heated to a first temperature above the sol-gel temperature of the one or more plant-based proteins and then lowered to a second temperature below the sol-gel temperature of the one or more plant-based proteins to form a hydrogel.

35. A plant-based hydrogel formed using the method of any one of claims 24 to 34.

36. A thermally reversible process for obtaining a plant-based material, the thermally reversible process comprising:

a) forming a solution comprising one or more plant-based proteins in a solvent system, wherein the solvent system comprises a miscible co-solvent; wherein the first co-solvent increases the solubility of the one or more plant-based proteins and the second co-solvent decreases the solubility of the one or more plant-based proteins; and

b) inducing a sol-gel transition of the protein in the solution to form a plant-based protein hydrogel.

37. The thermally reversible method of claim 36, wherein the solvent system is then removed such that the plant-based protein hydrogel no longer has thermally reversible properties.

Technical Field

The present invention relates to plant based materials, a method for the manufacture thereof and a biomaterial comprising a plant based material according to the present invention.

Background

Synthetic polymers such as plastics exhibit excellent mechanical and chemical properties and have been widely used during the past 60 years. However, these polymers are non-biodegradable and can accumulate in the environment, causing economic damage and possibly affecting human health through the food chain and air.

The development of materials exhibiting high functionality as well as high biodegradability and biocompatibility is a key goal to meet the social demand for improved material performance in the fields from packaging to pharmaceuticals and the like.

Self-assembly appears as an attractive route towards the manufacture of such materials, but most of the building blocks developed to date have originated from synthesis.

Among the different types of biopolymers that can be used as building blocks for the production of new functional materials, proteins are interesting candidates due to their ability to self-assemble into functional structures.

Currently, the use of these materials in commercial applications is limited to highly soluble proteins of animal origin. Animal proteins commonly used in food products, such as whey proteins, exhibit good biocompatibility, biodegradability, amphiphilicity and functional properties such as water solubility, emulsifying and foaming ability. However, there is an increasing demand for replacing proteins of animal origin with plant-based proteins, not only because of their less environmental impact, but also because of their lower allergenicity and reduced cost.

Self-assembled materials formed from plant-based proteins have been reported, wherein hydrogels can be obtained from soy and pea proteins under a range of experimental conditions. However, the mechanical properties obtained from structured plant-based materials are generally lower compared to those obtained from materials of animal origin; and vegetable proteins are more difficult to process, at least in part due to their inherently low solubility in water.

Thus, plant-based proteins have not been successfully used as biomaterials to date, and the production of structured proteinaceous materials from renewable and cost-effective sources and with environmentally sustainable processes remains a challenge.

Summary of The Invention

According to one aspect of the present invention, there is provided a method for producing a plant-based material, comprising:

a) forming a solution comprising one or more plant-based proteins in a solvent system, wherein the solvent system comprises a miscible cosolvent; wherein the first co-solvent increases the solubility of the one or more plant-based proteins and the second co-solvent decreases the solubility of the one or more plant-based proteins; and

b) inducing the protein in the solution to undergo a sol-gel transition to form a plant-based protein hydrogel.

In another embodiment, the method comprises the steps of:

c) plant-based protein hydrogels are formed into structured materials.

Forming the plant-based protein hydrogel into a structured material allows for the formation of structured materials, such as gels, films, microgels, microcapsules, and the like. In a preferred embodiment, the protein hydrogel may be formed into a prescribed shape by molding. In another preferred embodiment, the protein hydrogel may be formed into a defined shape using a microfluidic device.

The present inventors have identified a new method for making functional materials from plant-based proteins. By utilizing a co-solvent mixture, control can be exerted over the sol-gel transition, allowing the formation of structurally robust materials from renewable vegetable protein sources. The method allows for the production of a number of structured materials, including hydrogels, films, microcapsules, microgels, microsponges, and the like. Structured materials can be reliably formed without the need for cross-linking agents or any other hazardous materials, making them suitable for human contact. These materials are also derived from renewable sources, thus reducing environmental impact relative to synthetic analogs.

In another aspect, there is provided the use of a co-solvent mixture for modulating the properties of a plant-based protein in solution to control sol-gel conditions and thereby form a plant-based material.

Sol-gel conditions can be controlled by selecting a solvent system comprising miscible co-solvents, wherein a first co-solvent increases the solubility of one or more plant-based proteins and a second co-solvent decreases the solubility of the one or more plant-based proteins.

The ratio of the first co-solvent to the second co-solvent may vary from about 20-80% v/v, about 20-60% v/v, about 25-55% v/v, about 30-50% v/v, about 20%, about 30%, about 40%, about 50% or about 60% v/v, most preferably about 30-50% v/v. Such ratios result in functionally useful materials.

The solvent system may contain one or more first co-solvents and/or one or more second co-solvents.

For the first time, scalable methods can be used to reliably and reproducibly form plant-based materials. By being able to control sol-gel conditions, the properties of the resulting material can be adjusted and/or the manufacturing process adjusted to allow for the production of useful biomaterials.

The method according to the present invention allows the formation of plant-based structured material formed via a thermally reversible cold-set gelation (thermal-reversible gel-setting process) process. The plant-based structured material may be a plant-based protein supramolecular structure; or may be a 3-dimensional network of aggregated and tangled plant-based protein supramolecular structures.

The thermally reversible cold-setting gelling process can be considered as a process: wherein the plant-based protein molecules can be heated above a certain temperature to form a liquid solution that can be processed to a desired configuration and then cooled to enable a sol-gel transition to form a network of self-assembled protein aggregates that are maintained by non-covalent intermolecular interactions. Thus, the gelling process according to the invention does not require covalent chemical crosslinking and is therefore reversible. The present invention includes a thermally reversible cold gelation process.

Thus, in another aspect, there is provided a plant-based structured material formed via a thermally reversible cold-setting gelling process; wherein the structured material can optionally be a film, a thin film, a micropatterned film (or film), a micro-or nanostructured film, a microgel, a microcapsule, a microbead, a bioscaffold, a biological support, a sponge, a microsponge, a hard capsule, or a functional coating.

In another aspect, a plant-based thermoreversible gel is provided.

In another aspect, a plant-based thermoreversible hydrogel is provided.

In another aspect, a composite material is provided comprising a plant based material according to the invention, and one or more other biopolymers, such as proteins, polysaccharides and the like.

In another aspect, there is provided a material prepared according to the method of the present invention.

The plant-based materials of the present invention and the methods for making them allow for precise control of the sol-gel transition, thereby opening the use of plant-based proteins for forming biomaterials that have heretofore been successfully made using only animal-derived proteins. Suitable biological materials include membranes, microbeads, microcapsules, scaffolds, gels, sponges and the like.

In another aspect, there is provided a microbead comprising a plant-based material according to the invention.

In another aspect, there is provided a microcapsule comprising a plant-based material according to the invention.

In another aspect, there is provided a hard capsule comprising the plant-based material according to the present invention.

In another aspect, a sponge or microsponge comprising a plant-based material according to the invention is provided.

In another aspect, there is provided a film, preferably a thin film, comprising the plant based material according to the invention.

In another aspect, there is provided a nano-or micro-patterned film comprising a plant-based material according to the present invention.

In another aspect, there is provided a bioscaffold comprising a plant-based hydrogel according to the invention.

In another aspect, a functional coating comprising a plant-based hydrogel according to the invention is provided.

In another aspect, a food, cosmetic, pharmaceutical or medical device comprising the plant based material according to the invention is provided.

In another aspect, there is provided a thermoreversible method for obtaining a plant based material comprising:

a) forming a solution comprising one or more plant-based proteins in a solvent system comprising a miscible cosolvent; wherein the first co-solvent increases the solubility of the one or more plant-based proteins and the second co-solvent decreases the solubility of the one or more plant-based proteins; and

b) inducing the protein in the solution to undergo a sol-gel transition to form a plant-based protein hydrogel.

After the material is obtained, the thermo-reversible nature of the material can be removed.