CN114748671B - Compound protein slow-release hydrocolloid application and preparation method thereof - Google Patents

Compound protein slow-release hydrocolloid application and preparation method thereof Download PDF

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Publication number
CN114748671B
CN114748671B CN202210287306.4A CN202210287306A CN114748671B CN 114748671 B CN114748671 B CN 114748671B CN 202210287306 A CN202210287306 A CN 202210287306A CN 114748671 B CN114748671 B CN 114748671B
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silk fibroin
hydrocolloid
release
aqueous solution
mussel mucin
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CN114748671A (en
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周晓宁
赵铭
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Deshengkang Suzhou Biotechnology Co ltd
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Deshengkang Suzhou Biotechnology Co ltd
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Priority to CN202211370216.8A priority Critical patent/CN115737888B/en
Priority to CN202211369994.5A priority patent/CN115887730B/en
Priority to CN202210287306.4A priority patent/CN114748671B/en
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    • AHUMAN NECESSITIES
    • A61MEDICAL OR VETERINARY SCIENCE; HYGIENE
    • A61LMETHODS OR APPARATUS FOR STERILISING MATERIALS OR OBJECTS IN GENERAL; DISINFECTION, STERILISATION OR DEODORISATION OF AIR; CHEMICAL ASPECTS OF BANDAGES, DRESSINGS, ABSORBENT PADS OR SURGICAL ARTICLES; MATERIALS FOR BANDAGES, DRESSINGS, ABSORBENT PADS OR SURGICAL ARTICLES
    • A61L15/00Chemical aspects of, or use of materials for, bandages, dressings or absorbent pads
    • A61L15/16Bandages, dressings or absorbent pads for physiological fluids such as urine or blood, e.g. sanitary towels, tampons
    • A61L15/22Bandages, dressings or absorbent pads for physiological fluids such as urine or blood, e.g. sanitary towels, tampons containing macromolecular materials
    • A61L15/32Proteins, polypeptides; Degradation products or derivatives thereof, e.g. albumin, collagen, fibrin, gelatin
    • AHUMAN NECESSITIES
    • A61MEDICAL OR VETERINARY SCIENCE; HYGIENE
    • A61FFILTERS IMPLANTABLE INTO BLOOD VESSELS; PROSTHESES; DEVICES PROVIDING PATENCY TO, OR PREVENTING COLLAPSING OF, TUBULAR STRUCTURES OF THE BODY, e.g. STENTS; ORTHOPAEDIC, NURSING OR CONTRACEPTIVE DEVICES; FOMENTATION; TREATMENT OR PROTECTION OF EYES OR EARS; BANDAGES, DRESSINGS OR ABSORBENT PADS; FIRST-AID KITS
    • A61F13/00Bandages or dressings; Absorbent pads
    • A61F13/02Adhesive bandages or dressings
    • A61F13/0276Apparatus or processes for manufacturing adhesive dressings or bandages
    • A61F13/0289Apparatus or processes for manufacturing adhesive dressings or bandages manufacturing of adhesive dressings
    • AHUMAN NECESSITIES
    • A61MEDICAL OR VETERINARY SCIENCE; HYGIENE
    • A61LMETHODS OR APPARATUS FOR STERILISING MATERIALS OR OBJECTS IN GENERAL; DISINFECTION, STERILISATION OR DEODORISATION OF AIR; CHEMICAL ASPECTS OF BANDAGES, DRESSINGS, ABSORBENT PADS OR SURGICAL ARTICLES; MATERIALS FOR BANDAGES, DRESSINGS, ABSORBENT PADS OR SURGICAL ARTICLES
    • A61L15/00Chemical aspects of, or use of materials for, bandages, dressings or absorbent pads
    • A61L15/16Bandages, dressings or absorbent pads for physiological fluids such as urine or blood, e.g. sanitary towels, tampons
    • A61L15/22Bandages, dressings or absorbent pads for physiological fluids such as urine or blood, e.g. sanitary towels, tampons containing macromolecular materials
    • A61L15/24Macromolecular compounds obtained by reactions only involving carbon-to-carbon unsaturated bonds; Derivatives thereof
    • AHUMAN NECESSITIES
    • A61MEDICAL OR VETERINARY SCIENCE; HYGIENE
    • A61LMETHODS OR APPARATUS FOR STERILISING MATERIALS OR OBJECTS IN GENERAL; DISINFECTION, STERILISATION OR DEODORISATION OF AIR; CHEMICAL ASPECTS OF BANDAGES, DRESSINGS, ABSORBENT PADS OR SURGICAL ARTICLES; MATERIALS FOR BANDAGES, DRESSINGS, ABSORBENT PADS OR SURGICAL ARTICLES
    • A61L15/00Chemical aspects of, or use of materials for, bandages, dressings or absorbent pads
    • A61L15/16Bandages, dressings or absorbent pads for physiological fluids such as urine or blood, e.g. sanitary towels, tampons
    • A61L15/22Bandages, dressings or absorbent pads for physiological fluids such as urine or blood, e.g. sanitary towels, tampons containing macromolecular materials
    • A61L15/26Macromolecular compounds obtained otherwise than by reactions only involving carbon-to-carbon unsaturated bonds; Derivatives thereof
    • AHUMAN NECESSITIES
    • A61MEDICAL OR VETERINARY SCIENCE; HYGIENE
    • A61LMETHODS OR APPARATUS FOR STERILISING MATERIALS OR OBJECTS IN GENERAL; DISINFECTION, STERILISATION OR DEODORISATION OF AIR; CHEMICAL ASPECTS OF BANDAGES, DRESSINGS, ABSORBENT PADS OR SURGICAL ARTICLES; MATERIALS FOR BANDAGES, DRESSINGS, ABSORBENT PADS OR SURGICAL ARTICLES
    • A61L15/00Chemical aspects of, or use of materials for, bandages, dressings or absorbent pads
    • A61L15/16Bandages, dressings or absorbent pads for physiological fluids such as urine or blood, e.g. sanitary towels, tampons
    • A61L15/22Bandages, dressings or absorbent pads for physiological fluids such as urine or blood, e.g. sanitary towels, tampons containing macromolecular materials
    • A61L15/28Polysaccharides or their derivatives
    • AHUMAN NECESSITIES
    • A61MEDICAL OR VETERINARY SCIENCE; HYGIENE
    • A61LMETHODS OR APPARATUS FOR STERILISING MATERIALS OR OBJECTS IN GENERAL; DISINFECTION, STERILISATION OR DEODORISATION OF AIR; CHEMICAL ASPECTS OF BANDAGES, DRESSINGS, ABSORBENT PADS OR SURGICAL ARTICLES; MATERIALS FOR BANDAGES, DRESSINGS, ABSORBENT PADS OR SURGICAL ARTICLES
    • A61L15/00Chemical aspects of, or use of materials for, bandages, dressings or absorbent pads
    • A61L15/16Bandages, dressings or absorbent pads for physiological fluids such as urine or blood, e.g. sanitary towels, tampons
    • A61L15/40Bandages, dressings or absorbent pads for physiological fluids such as urine or blood, e.g. sanitary towels, tampons containing ingredients of undetermined constitution or reaction products thereof, e.g. plant or animal extracts
    • AHUMAN NECESSITIES
    • A61MEDICAL OR VETERINARY SCIENCE; HYGIENE
    • A61LMETHODS OR APPARATUS FOR STERILISING MATERIALS OR OBJECTS IN GENERAL; DISINFECTION, STERILISATION OR DEODORISATION OF AIR; CHEMICAL ASPECTS OF BANDAGES, DRESSINGS, ABSORBENT PADS OR SURGICAL ARTICLES; MATERIALS FOR BANDAGES, DRESSINGS, ABSORBENT PADS OR SURGICAL ARTICLES
    • A61L15/00Chemical aspects of, or use of materials for, bandages, dressings or absorbent pads
    • A61L15/16Bandages, dressings or absorbent pads for physiological fluids such as urine or blood, e.g. sanitary towels, tampons
    • A61L15/42Use of materials characterised by their function or physical properties
    • AHUMAN NECESSITIES
    • A61MEDICAL OR VETERINARY SCIENCE; HYGIENE
    • A61LMETHODS OR APPARATUS FOR STERILISING MATERIALS OR OBJECTS IN GENERAL; DISINFECTION, STERILISATION OR DEODORISATION OF AIR; CHEMICAL ASPECTS OF BANDAGES, DRESSINGS, ABSORBENT PADS OR SURGICAL ARTICLES; MATERIALS FOR BANDAGES, DRESSINGS, ABSORBENT PADS OR SURGICAL ARTICLES
    • A61L15/00Chemical aspects of, or use of materials for, bandages, dressings or absorbent pads
    • A61L15/16Bandages, dressings or absorbent pads for physiological fluids such as urine or blood, e.g. sanitary towels, tampons
    • A61L15/42Use of materials characterised by their function or physical properties
    • A61L15/44Medicaments
    • AHUMAN NECESSITIES
    • A61MEDICAL OR VETERINARY SCIENCE; HYGIENE
    • A61LMETHODS OR APPARATUS FOR STERILISING MATERIALS OR OBJECTS IN GENERAL; DISINFECTION, STERILISATION OR DEODORISATION OF AIR; CHEMICAL ASPECTS OF BANDAGES, DRESSINGS, ABSORBENT PADS OR SURGICAL ARTICLES; MATERIALS FOR BANDAGES, DRESSINGS, ABSORBENT PADS OR SURGICAL ARTICLES
    • A61L2300/00Biologically active materials used in bandages, wound dressings, absorbent pads or medical devices
    • A61L2300/20Biologically active materials used in bandages, wound dressings, absorbent pads or medical devices containing or releasing organic materials
    • A61L2300/252Polypeptides, proteins, e.g. glycoproteins, lipoproteins, cytokines
    • AHUMAN NECESSITIES
    • A61MEDICAL OR VETERINARY SCIENCE; HYGIENE
    • A61LMETHODS OR APPARATUS FOR STERILISING MATERIALS OR OBJECTS IN GENERAL; DISINFECTION, STERILISATION OR DEODORISATION OF AIR; CHEMICAL ASPECTS OF BANDAGES, DRESSINGS, ABSORBENT PADS OR SURGICAL ARTICLES; MATERIALS FOR BANDAGES, DRESSINGS, ABSORBENT PADS OR SURGICAL ARTICLES
    • A61L2300/00Biologically active materials used in bandages, wound dressings, absorbent pads or medical devices
    • A61L2300/60Biologically active materials used in bandages, wound dressings, absorbent pads or medical devices characterised by a special physical form
    • A61L2300/602Type of release, e.g. controlled, sustained, slow
    • AHUMAN NECESSITIES
    • A61MEDICAL OR VETERINARY SCIENCE; HYGIENE
    • A61LMETHODS OR APPARATUS FOR STERILISING MATERIALS OR OBJECTS IN GENERAL; DISINFECTION, STERILISATION OR DEODORISATION OF AIR; CHEMICAL ASPECTS OF BANDAGES, DRESSINGS, ABSORBENT PADS OR SURGICAL ARTICLES; MATERIALS FOR BANDAGES, DRESSINGS, ABSORBENT PADS OR SURGICAL ARTICLES
    • A61L2300/00Biologically active materials used in bandages, wound dressings, absorbent pads or medical devices
    • A61L2300/60Biologically active materials used in bandages, wound dressings, absorbent pads or medical devices characterised by a special physical form
    • A61L2300/62Encapsulated active agents, e.g. emulsified droplets
    • A61L2300/622Microcapsules

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Abstract

The invention discloses a compound protein slow-release hydrocolloid application plaster which is characterized in that raw material components of the hydrocolloid application plaster comprise a water-absorbing high polymer material, a hot-melt pressure-sensitive adhesive and a compound protein-coated microsphere, wherein the mass of the microsphere in the hydrocolloid application plaster is 5-20%; the composite protein comprises silk fibroin and mussel mucin, and the mass ratio of the silk fibroin to the mussel mucin is 1:1-5:1. According to the composite protein slow-release hydrocolloid application patch, the unique interface coverage characteristic of silk fibroin and the adhesive property of mussel mucin are combined, the volatile functional components in the hydrocolloid application patch are packaged in the composite protein formed by the silk fibroin and the mussel mucin, the release rate of the volatile components can be effectively reduced, and the controlled release at different stages can be realized.

Description

Compound protein slow-release hydrocolloid application and preparation method thereof
Technical Field
The invention belongs to the technical field of medical application, and particularly relates to a composite protein slow-release hydrocolloid application and a preparation method thereof.
Background
Hydrocolloid adhesive plaster is a new type of plaster material based on the theory of moist healing, and is prepared by blending water-absorbing high molecular material and hot-melt pressure-sensitive adhesive, and the material combines the adhesive property of the hot-melt pressure-sensitive adhesive and the water absorption of the water-absorbing high molecular material. The hot melt pressure sensitive adhesive provides viscosity, so that the patch can be pasted on a wound surface, and the water absorption macromolecules dispersed in the patch swell after absorbing water, thereby providing a moist closed environment for the wound and promoting the healing of the wound.
In the prior art, in order to provide more functionality and comfort to the hydrocolloid application, various components such as essence, essential oil and the like are often required to be added into the hydrocolloid application, and the components generally comprise dozens or even hundreds of volatile substances such as aldehyde, ketone, alcohol, ester and the like and can be continuously released from the hydrocolloid application. However, the formation of hydrocolloid requires a heating and melting process, and the ingredients such as essence, essential oil, etc. are directly mixed with hydrocolloid, which causes the loss of volatile ingredients during the formation process. In addition, these components are still volatilized before application, further affecting the effect in actual use. Therefore, how to control the release of volatile components becomes a problem to be solved in hydrocolloid application products.
The silk fibroin is a natural protein extracted from silk, and structurally has a hydrophilic region and a hydrophobic region, so the silk fibroin has an amphiphilic characteristic and certain surface activity, namely the silk fibroin is self-assembled at a fluid interface to form a stable viscoelastic surface or interface layer, and shows strong covering capacity. Mussel is a marine organism of crustacean widely distributed on coastal and offshore areas, its byssus gland can secrete byssus, and the byssus disc formed by byssus can fix mussel on the surface of various solid base materials, and the mussel mucin is the main component of mussel byssus, and has strong adhesive property.
Disclosure of Invention
In view of the above, in order to overcome the defects of the prior art, the present invention aims to provide a composite protein sustained release hydrocolloid patch, which combines the unique interface coverage characteristics of silk fibroin and the adhesive properties of mussel mucin to control the release of volatile components.
In order to achieve the purpose, the invention adopts the following technical scheme:
a compound protein slow-release hydrocolloid application patch comprises raw material components including a water-absorbing high polymer material, a hot-melt pressure-sensitive adhesive and a compound protein coated microsphere, wherein the mass of the microsphere in the hydrocolloid application patch accounts for 5% -20%; the composite protein comprises silk fibroin and mussel mucin, and the mass ratio of the silk fibroin to the mussel mucin is 1:1-5:1. The silk fibroin is deposited on the surface of the functional material through amphipathy to form a shell body, and the mussel mucin is deposited on the surface of the silk fibroin through electrostatic adsorption to play a role in reinforcement. If the content of mussel mucin is too low, it will not work, and if it is too high, it may cause the microspheres to stick to each other.
According to some preferred embodiments of the invention, the microspheres contain a functional material, and the mass ratio of the functional material to the silk fibroin is 5:1-15. The microsphere size and the loading capacity determine that the too low proportion of the functional material indicates that the microsphere is too small, the low loading capacity indicates that the microsphere is too large, and the microsphere is easy to damage.
According to some preferred embodiments of the invention, the functional material is a perfume and/or essential oil.
According to some preferred embodiments of the invention, the water-absorbent polymer material and the hot-melt pressure-sensitive adhesive are 5% to 40% and 40% to 90% by mass of the hydrocolloid application, respectively. This proportion sets up intensity and the water absorption capacity that can compromise hydrocolloid dressing, crosses lowly if hydroscopicity macromolecular material's proportion, and then the dressing absorbs the ability reduction of sepage, can't keep the wound moist, if hydroscopicity macromolecular material's proportion is too high, then hot melt pressure sensitive adhesive cohesion descends, applies ointment or plaster easy fragmentation.
According to some preferred embodiments of the present invention, the water-absorbing polymer material is a mixture of one or more of modified starch, gum arabic, gelatin, pectin, sodium polyacrylate, polyacrylamide, sodium carboxymethyl cellulose, hydroxyethyl cellulose, polyvinyl alcohol, and polyvinylpyrrolidone; the hot-melt pressure-sensitive adhesive is a mixture consisting of one or more of natural rubber, polyurethane rubber, silicon rubber, polyisobutylene rubber, styrene segmented copolymer thermoplastic elastomer, polyacrylate and polyvinyl ether.
The invention also provides a preparation method of the compound protein slow-release hydrocolloid patch, which comprises the following steps:
adding a functional material into a silk fibroin aqueous solution, uniformly mixing, then adding a mussel mucin aqueous solution, uniformly mixing, adding ethanol into the system, continuously stirring, and then centrifuging and cleaning to obtain microspheres wrapped by the composite protein; and blending the microspheres coated by the composite protein with a water-absorbing high polymer material and a hot-melt pressure-sensitive adhesive, and performing extrusion and calendaring molding to obtain the composite protein slow-release hydrocolloid patch.
According to some preferred embodiments of the invention, the concentration of the silk fibroin aqueous solution is 2% -15% by mass. If the concentration of the silk fibroin aqueous solution is too low, sufficient silk fibroin cannot be deposited on the surface of the functional material, and if the concentration is too high, the viscosity of the solution is too high, so that the microspheres cannot be prepared.
According to some preferred embodiments of the present invention, the ratio of the functional material to the aqueous solution of silk fibroin (i.e., the mass ratio to the aqueous solution of silk fibroin) is 1. Within this range, the functional material and the silk fibroin aqueous solution can form a stable emulsion. The mass ratio of the functional material to the silk fibroin is 5:1-15, which corresponds to the mass ratio of the functional material to the silk fibroin in the microsphere, and the mass ratio added in the preparation process corresponds to the mass ratio, because the silk fibroin solution is not 100% available in the preparation process, the silk fibroin deposited on the surface of the essential oil microsphere is calculated, and the surplus silk fibroin is still in the solution.
According to some preferred embodiments of the present invention, the concentration of the mussel mucin aqueous solution is 2% to 15% by mass. If the concentration is too low, the silk fibroin can not be compounded with enough silk fibroin, and if the concentration is too high, the solution viscosity is too high and the silk fibroin is not easy to mix.
According to some preferred embodiments of the present invention, the ethanol is added in an amount of 10% to 30% of the total volume of the mixed solution formed by the functional material, the silk fibroin aqueous solution and the mussel mucin aqueous solution. The ethanol is used for converting the silk fibroin into beta-folded conformation, and promoting the silk fibroin to form a shell layer of the microsphere, so that the microsphere is more stable in an aqueous solution. If the addition amount of the ethanol is too small, the silk fibroin can not form a shell layer, and if the addition amount of the ethanol is increased beyond the proportion, the appearance of the shell layer is not obviously changed.
In some embodiments of the present invention, the preparation method of the composite protein sustained release hydrocolloid application specifically comprises the following steps:
1. preparing the silk fibroin aqueous solution with the mass percentage concentration of 2-15%.
2. Adding essential oil into the silk fibroin aqueous solution, and stirring by using a high-speed homogenizer to form white emulsion, wherein the ratio of the essential oil to the silk fibroin aqueous solution is 1.
3. Preparing the mussel mucin water solution with the mass percentage concentration of 2-15%. Adding mussel mucin water solution into the emulsion, and stirring at room temperature for 24h.
4. And adding ethanol into the solution, wherein the addition amount of the ethanol is 10-30% of the total amount of the solution, continuously stirring for 12h, and then centrifuging and cleaning to obtain the essential oil microspheres wrapped by the compound protein. The particle size of the microsphere is 10-100 μm. Wherein, the ethanol is used for converting the silk fibroin into beta-folded conformation, and promoting the silk fibroin to form a shell layer of the microsphere, so that the microsphere is more stable in aqueous solution.
5. And blending the essential oil microspheres with the hot-melt pressure-sensitive adhesive and the hydrocolloid, extruding by a double screw, and performing calendaring molding to obtain the composite protein slow-release hydrocolloid patch.
The principle of the invention is as follows: since the functional materials such as essential oil and other volatile components are insoluble in water and are oil phases, the functional materials are blended with water under the action of strong shearing, the oil phases can form micro liquid drops to be dispersed in a water phase, and silk fibroin has amphipathy and can wrap the surfaces of oil drops. In addition, the surface of the silk fibroin in a neutral aqueous solution is negatively charged, and after the mussel mucin with positive charge is added, the mussel mucin can be automatically deposited on the surface of the silk fibroin, so that the silk fibroin-mussel mucin composite protein coated essential oil microspheres are finally formed. After mussel mucin is deposited on the surface of silk fibroin, dopa groups of the mussel mucin are self-crosslinked to form a net structure, so that a silk fibroin shell layer is reinforced, and the microspheres are more stable.
The microspheres are blended with hot-melt pressure-sensitive adhesive and water-absorbing high molecular materials such as hydrocolloid to obtain the hydrocolloid patch, and when the patch is not used, the escape rate of essential oil is obviously lower than that of the hydrocolloid patch obtained by directly blending the essential oil with the hot-melt pressure-sensitive adhesive and the hydrocolloid. The hydrocolloid patch obtained by the invention is applied to the surface of skin, after the hydrocolloid and the compound protein absorb water, the compound protein shell swells, the intermolecular distance is increased, the permeability of the compound protein is increased, and the release of essential oil is accelerated, so that the controllable release of volatile components is realized.
Due to the implementation of the technical scheme, compared with the prior art, the invention has the following advantages: according to the composite protein slow-release hydrocolloid patch, the unique interface coverage characteristic of silk fibroin and the adhesive property of mussel mucin are combined, the volatile functional ingredients in the hydrocolloid patch are packaged in the composite protein consisting of the silk fibroin and the mussel mucin, the release rate of the volatile ingredients can be effectively reduced, and the controlled release at different stages can be realized.
Detailed Description
In order to make those skilled in the art better understand the technical solution of the present invention, the technical solution in the embodiments of the present invention will be clearly and completely described below, and it is obvious that the described embodiments are only a part of the embodiments of the present invention, and not all embodiments. All other embodiments, which can be derived by a person skilled in the art from the embodiments given herein without making any creative effort, shall fall within the protection scope of the present invention.
Example 1
The raw material components of the compound protein slow-release hydrocolloid patch in the embodiment comprise a hydrocolloid, a hot-melt pressure-sensitive adhesive and a microsphere coated by a compound protein. Wherein the mass ratio of the microspheres in the hydrocolloid application patch is 10%, the mass ratio of the water-absorbing polymer in the hydrocolloid application patch is 25%, and the mass ratio of the hot-melt pressure-sensitive adhesive in the hydrocolloid application patch is 65%.
The composite protein comprises silk fibroin and mussel mucin, and the mass ratio of the silk fibroin to the mussel mucin is 3:1.
The composite protein coated microspheres in the embodiment are composite protein coated essential oil microspheres, wherein the mass ratio of the essential oil to the silk fibroin is 9:1.
The preparation method of the composite protein slow-release hydrocolloid application patch in the embodiment specifically comprises the following steps:
1. preparing silk fibroin aqueous solution with the mass percentage concentration of 10%.
2. Adding the essential oil into the silk fibroin aqueous solution, and stirring by using a high-speed homogenizer (the stirring speed is 5000 RPM) to form a white emulsion, wherein the ratio of the essential oil to the silk fibroin aqueous solution is 1.
3. Preparing a mussel mucin water solution with the mass percentage concentration of 10%. Adding mussel mucin water solution into the emulsion, and stirring at room temperature for 24h.
4. And adding ethanol into the solution, wherein the addition amount of the ethanol is 10% of the total amount of the solution, continuously stirring for 12h, and then centrifuging and cleaning to obtain the essential oil microspheres wrapped by the compound protein.
5. And (3) blending the essential oil microspheres with the hot-melt pressure-sensitive adhesive and the hydrocolloid, and performing twin-screw extrusion and calendaring molding to obtain the composite protein slow-release hydrocolloid patch.
Example 2
The raw material components of the composite protein slow-release hydrocolloid patch in the embodiment comprise hydrocolloid, hot-melt pressure-sensitive adhesive and microspheres wrapped by composite protein. Wherein the mass ratio of the microspheres in the hydrocolloid application plaster is 5%, the mass ratio of the water-absorbing polymer in the hydrocolloid application plaster is 40%, and the mass ratio of the hot-melt pressure-sensitive adhesive in the hydrocolloid application plaster is 55%.
The composite protein comprises silk fibroin and mussel mucin, and the mass ratio of the silk fibroin to the mussel mucin is 5:1.
The composite protein coated microspheres in the embodiment are composite protein coated essential oil microspheres, wherein the mass ratio of the essential oil to the silk fibroin is 9:1.
The preparation method of the composite protein slow-release hydrocolloid application in the embodiment specifically comprises the following steps:
1. preparing silk fibroin aqueous solution with the mass percentage concentration of 5%.
2. Adding the essential oil into the silk fibroin aqueous solution, and stirring by using a high-speed homogenizer (the stirring speed is 5000 RPM) to form a white emulsion, wherein the ratio of the essential oil to the silk fibroin aqueous solution is 1.
3. And preparing a mussel mucin aqueous solution with the mass percentage concentration of 2%. The mussel mucin aqueous solution is added to the above emulsion, and stirred at room temperature for 24h.
4. And adding ethanol into the solution, wherein the addition amount of the ethanol is 10% of the total amount of the solution, continuously stirring for 12h, and then centrifuging and cleaning to obtain the essential oil microspheres wrapped by the compound protein.
5. And blending the essential oil microspheres with the hot-melt pressure-sensitive adhesive and the hydrocolloid, extruding by a double screw, and performing calendaring molding to obtain the composite protein slow-release hydrocolloid patch.
Example 3
The raw material components of the composite protein slow-release hydrocolloid patch in the embodiment comprise hydrocolloid, hot-melt pressure-sensitive adhesive and microspheres wrapped by composite protein. Wherein the mass ratio of the microspheres in the hydrocolloid application patch is 20%, the mass ratio of the water-absorbing polymer in the hydrocolloid application patch is 20%, and the mass ratio of the hot-melt pressure-sensitive adhesive in the hydrocolloid application patch is 60%.
The composite protein comprises silk fibroin and mussel mucin, and the mass ratio of the silk fibroin to the mussel mucin is 1:1.
The composite protein coated microspheres in the embodiment are composite protein coated essential oil microspheres, wherein the mass ratio of the essential oil to the silk fibroin is 6:1.
The preparation method of the composite protein slow-release hydrocolloid application patch in the embodiment specifically comprises the following steps:
1. preparing silk fibroin aqueous solution with the mass percentage concentration of 10%.
2. Adding the essential oil into the silk fibroin aqueous solution, and stirring by using a high-speed homogenizer (the stirring speed is 5000 RPM) to form a white emulsion, wherein the ratio of the essential oil to the silk fibroin aqueous solution is 1.
3. Preparing a mussel mucin water solution with the mass percentage concentration of 5%. Adding mussel mucin water solution into the emulsion, and stirring at room temperature for 24h.
4. And adding ethanol into the solution, wherein the addition amount of the ethanol is 10% of the total amount of the solution, continuously stirring for 12h, and then centrifuging and cleaning to obtain the essential oil microspheres wrapped by the compound protein.
5. And blending the essential oil microspheres with the hot-melt pressure-sensitive adhesive and the hydrocolloid, extruding by a double screw, and performing calendaring molding to obtain the composite protein slow-release hydrocolloid patch.
Comparative example 1
This comparative example differs from example 1 in that: the mass ratio between silk fibroin and mussel mucin in this comparative example was 1:2. The other formulation ingredients and preparation steps were substantially the same as in example 1. In the preparation process of the comparative example, the microspheres are mutually adhered and agglomerated and are not uniformly dispersed.
Comparative example 2
The comparative example differs from example 1 in that: the mass ratio between the essential oil and the silk fibroin in this comparative example was 2:1. The other formulation ingredients and preparation steps were substantially the same as in example 1.
Comparative example 3
This comparative example differs from example 1 in that: the concentration of the silk fibroin aqueous solution in this comparative example was 17%. The other formulation ingredients and preparation steps were substantially the same as in example 1. In the preparation process of the comparative example, due to the fact that the solution viscosity is too high, deposition of silk fibroin and mussel mucin to the surface of essential oil droplets is hindered, and microspheres cannot be formed.
Comparative example 4
The comparative example differs from example 1 in that: the amount of ethanol added in this comparative example was 5%. The other formulation ingredients and preparation steps were substantially the same as in example 1.
Comparative example 5
This comparative example differs from example 1 in that: the microspheres in this comparative example do not contain mussel mucin, nor does the preparation process require the addition of an aqueous mussel mucin solution. The other formulation ingredients and preparation steps were substantially the same as in example 1.
Comparative example 6
In the comparative example, the essential oil microspheres in example 1 are replaced by essential oil with the same quality, and the essential oil microspheres are added into hot-melt pressure sensitive adhesive and hydrocolloid to be blended, extruded and pressed to obtain hydrocolloid application.
Test and results
Respectively dissolving the hydrocolloid patches prepared in the same mass of the embodiment and the comparative example in ethyl acetate, and measuring the initial content of the essential oil by using ultraviolet; and in an unused state, the patch is placed in a room temperature environment of 25 ℃ and physiological saline for 6 months, and the content of the residual essential oil is periodically detected. The content of the essential oil is calculated by the following method: dissolving essential oil in ethyl acetate to prepare standard solutions with different concentrations, measuring absorbance by using a spectrophotometer to obtain a standard curve, dissolving a sample to be measured in ethyl acetate to measure absorbance, and calculating the concentration by using the standard curve. The results are shown in Table 1.
TABLE 1 test results
Figure BDA0003558796490000071
As can be seen from the test results in table 1, the essential oil coated with the complex protein has lower loss of the essential oil in the blending thermoforming process with the hydrocolloid and the hot melt pressure sensitive adhesive, compared with the essential oil not coated with the protein; the release amount of the essential oil coated by the composite protein is obviously lower than that of a hydrocolloid patch obtained by direct blending; and the hydrocolloid is applied to the surface of the skin, so that after seepage and water vapor are absorbed by the hydrocolloid, the release rate of the essential oil is increased, and controllable release can be realized.
Aiming at the problem that volatile components such as essence and essential oil are added directly into the existing hydrocolloid patch and then the volatilization rate of the components is too high, a slow-release and controlled-release structure is designed by utilizing composite protein of silk fibroin and mussel mucin, the volatile components can be packaged in the composite protein, the release rate of the volatile components can be effectively reduced, and the controlled release at different stages can be realized.
The above embodiments are merely illustrative of the technical concept and features of the present invention, and the purpose thereof is to enable those skilled in the art to understand the content of the present invention and implement the invention, and not to limit the scope of the invention, and all equivalent changes or modifications made according to the spirit of the present invention should be covered by the scope of the present invention.

Claims (10)

1. The compound protein slow-release hydrocolloid application is characterized in that raw material components of the hydrocolloid application comprise a water-absorbent high polymer material, a hot-melt pressure-sensitive adhesive and compound protein-coated microspheres, wherein the mass ratio of the compound protein-coated microspheres in the hydrocolloid application is 5% -20%; the composite protein comprises silk fibroin and mussel mucin, and the mass ratio of the silk fibroin to the mussel mucin is 1:1-5:1.
2. The composite protein sustained release hydrocolloid dressing of claim 1, wherein the microspheres contain a functional material, and the mass ratio of the functional material to the silk fibroin is 5:1-15.
3. The composite protein slow release hydrocolloid dressing of claim 2, wherein said functional material is a fragrance and/or an essential oil.
4. The composite protein sustained-release hydrocolloid application patch according to claim 1, wherein the water-absorbent polymer material and the hot-melt pressure-sensitive adhesive are 5-40% and 40-90% by mass of the hydrocolloid application patch, respectively.
5. The composite protein sustained-release hydrocolloid dressing of claim 1, wherein the water-absorbing high-molecular material is a mixture of one or more of modified starch, acacia, gelatin, pectin, sodium polyacrylate, polyacrylamide, sodium carboxymethylcellulose, hydroxyethyl cellulose, polyvinyl alcohol, and polyvinyl pyrrolidone; the hot-melt pressure-sensitive adhesive is a mixture consisting of one or more of natural rubber, polyurethane rubber, silicon rubber, polyisobutylene rubber, styrene segmented copolymer thermoplastic elastomer, polyacrylate and polyvinyl ether.
6. The preparation method of the compound protein slow-release hydrocolloid application is characterized by comprising the following steps of:
adding a functional material into a silk fibroin aqueous solution, uniformly mixing, then adding a mussel mucin aqueous solution, uniformly mixing, adding ethanol into the system, continuously stirring, and then centrifuging and cleaning to obtain microspheres wrapped by the composite protein; and blending the microspheres coated with the composite protein, the water-absorbent polymer material and the hot-melt pressure-sensitive adhesive, and extruding and calendaring to obtain the composite protein slow-release hydrocolloid patch.
7. The preparation method of claim 6, wherein the concentration of the silk fibroin aqueous solution is 2% -15% by mass.
8. The preparation method of claim 6, wherein the mass ratio of the functional material to the silk fibroin aqueous solution is 1.
9. The method according to claim 6, wherein the concentration of the mussel mucin aqueous solution is 2-15% by mass.
10. The preparation method of claim 6, wherein the amount of ethanol added is 10-30% of the total volume of the mixed solution formed by the functional material, the aqueous solution of silk fibroin and the aqueous solution of mussel mucin.
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