Antibacterial compound containing shellac nanoparticles and preparation method thereof

The antibacterial coating and gel prepared by combining shellac nanoparticles with polymer carriers solves the problem of the lack of antibacterial properties of traditional medical devices and skin mucosal materials, and achieves excellent antibacterial effects and biocompatibility. It is suitable for a variety of medical devices and skin mucosal surfaces.

CN120437394APending Publication Date: 2025-08-08SOUTHWEST JIAOTONG UNIV
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Patent Information

Application Number
CN202510605679.5
Authority / Receiving Office
CN · China
Patent Type
Applications(China)
Current Assignee / Owner
Filing Date
2025-05-12
Publication Date
2025-08-08

AI Technical Summary

Technical Problem

Traditional medical device materials lack antibacterial properties, resulting in an increased risk of bacterial infection, and bacterial infection makes it difficult for wounds to heal after damage to the skin and mucous membranes.

Method used

The antibacterial coating or gel is prepared by combining shellac nanoparticles with polymer carriers such as PLGA, HA, etc. The weight ratio of shellac nanoparticles in the coating or gel is 1:0.1 to 1:2.0, and is applied to medical devices and the surface of skin mucosa.

Benefits of technology

The prepared antibacterial coatings and gels have excellent antibacterial properties and biocompatibility. They are widely used in the surfaces of medical devices and the skin mucosa, reducing bacterial infections and promoting wound healing.

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Abstract

The invention discloses an antibacterial compound containing shellac nanoparticles and a preparation method of the antibacterial compound, and belongs to the technical field of medical materials. The antibacterial product is a polylactic acid-glycolic acid copolymer (PLGA) loaded shellac nanoparticle antibacterial coating or hyaluronic acid (HA) loaded shellac nanoparticle antibacterial gel. The coating and the gel prepared by the invention have excellent antibacterial performance and good biocompatibility, and the preparation method is relatively simple. The antibacterial coating can be applied to the surfaces of medical instruments such as intravascular stents, artificial heart valves, artificial blood pumps, artificial blood vessels, catheters and vein filters to improve the antibacterial performance of the medical instruments, and can also be applied to the surfaces of skin and mucosa to improve the antibacterial performance.
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Description

Technical Field

[0001] The invention belongs to the technical field of medical materials, and particularly relates to an antibacterial compound containing shellac nanoparticles and a preparation method thereof. Background Art

[0002] Traditional medical device materials such as 316L stainless steel, medical cobalt alloy, Ti-Ni alloy, ultra-high molecular weight polyethylene, polyester, etc. have good mechanical properties and biocompatibility and are often used to prepare medical devices such as vascular stents, artificial blood pumps, artificial joints, artificial bones, artificial heart valves, artificial blood vessels, catheters, etc. However, these biomaterials and devices do not have antibacterial properties and may cause bacterial infections, increase their application risks, and even cause death. Therefore, it is of great significance to modify the surface of traditional medical materials and devices to make them have antibacterial properties. In addition, after the skin and mucous membranes are damaged, bacterial infection on their surface is an important reason for the difficulty in wound healing. Therefore, it is of great significance to develop hydrogels with antibacterial properties and moisturizing effects, which cause less tissue damage during dressing changes and promote wound healing of the skin and mucous membranes. Summary of the Invention

[0003] To address the aforementioned shortcomings of the prior art, the present invention provides an antimicrobial compound containing shellac nanoparticles and a method for preparing the same. The shellac-based antimicrobial product exhibits excellent antimicrobial properties and biocompatibility, is relatively simple to prepare, and has a wide range of applications. It can be applied to the surfaces of medical devices such as vascular stents, prosthetic heart valves, artificial blood pumps, artificial blood vessels, artificial joints, artificial bones, catheters, and venous filters. The antimicrobial gel can also be applied to skin and mucous membranes to enhance its antimicrobial properties.

[0004] To achieve the above-mentioned purpose, the technical solution adopted by the present invention to solve the technical problem is:

[0005] The purpose of the present invention is to provide the use of shellac in preparing antibacterial products.

[0006] Furthermore, the antibacterial product is an antibacterial coating or an antibacterial gel.

[0007] One object of the present invention is to provide an antibacterial coating containing shellac nanoparticles, which comprises shellac nanoparticles and a polymer carrier that loads the shellac nanoparticles.

[0008] Furthermore, the polymer carrier is polylactic acid-glycolic acid copolymer (PLGA), hydroxypropyl methylcellulose, methylcellulose, triethyl citrate, polyethylene glycol, polyvinyl alcohol, ethyl cellulose, polylactic acid, polyglycolic acid, polylactide, polyglycolide, copolymer of polylactide and polyglycolide, polyhydroxymethylacrylate, fibrin, silicone, polysiloxane, polydimethylsiloxane, polyvinyl halide and copolymer, cellulose ether, cellulose triacetate, chitosan, and copolymers and / or mixtures of the above polymers.

[0009] Furthermore, the weight ratio of the polymer carrier to the shellac nanoparticles is 1:0.1 to 1:2.0.

[0010] Furthermore, the weight ratio of the polymer carrier to the shellac nanoparticles is 1:0.1, 1:0.2, 1:0.3, 1:04, 1:0.6, 1:0.8, etc.

[0011] Furthermore, shellac nanoparticles were prepared by an antisolvent precipitation method, and the preparation method is as follows:

[0012] (1) dissolving shellac in a solvent to obtain a shellac solution having a concentration of 120-150 mg / mL;

[0013] (2) Filter the shellac solution using a needle filter with a diameter of 0.22 μm to remove insoluble matter;

[0014] (3) The filtered shellac solution was added dropwise to distilled water at a rate of 122 drops / min;

[0015] (4) stirring in a magnetic stirrer at a speed of 600 rpm;

[0016] (5) Filter the shellac aqueous solution using a vacuum filter to remove a small amount of aggregates;

[0017] (6) Using a rotary evaporator at 60°C for 15-20 min, the alcohol is evaporated, and distilled water is added to the evaporated solution. Shellac nanoparticles with a particle size of approximately 200 nm and a concentration of 0.2 mg / mL-25 mg / mL are obtained.

[0018] Furthermore, the solvent for dissolving shellac is ethanol, methanol, sodium hydroxide, potassium hydroxide, calcium hydroxide, sodium amide, quaternary ammonium hydroxide, ammonia water, ethyl acetate, dimethyl sulfoxide, tetrahydrofuran, chloroform, and dichloromethane.

[0019] The preparation method of the above antibacterial coating is as follows:

[0020] (1) dissolving PLGA in an acetone solution to obtain a PLGA solution with a concentration of 1-50 mg / mL; controlling the mass ratio of PLGA to shellac nanoparticles to be 1:0.1-1:0.8;

[0021] (2) After the PLGA shellac nanoparticles mixed solution is fully mixed, it is dropped onto the PVC surface with a drop volume per unit surface of 60 μL / cm 2 -1000μL / cm 2 , and then dried at 37 ° C for 3 hours to obtain an antibacterial coating containing shellac nanoparticles.

[0022] Another object of the present invention is to provide an antibacterial gel containing shellac nanoparticles, which comprises shellac nanoparticles and a polymer gel matrix loaded with the shellac nanoparticles.

[0023] Furthermore, the polymer gel matrix is hyaluronic acid (HA), carbomer, hydroxypropyl methylcellulose, chitosan, xanthan gum, sodium polyacrylate, polyvinyl pyrrolidone, polyethylene glycol, and copolymers and / or mixtures of the above polymers.

[0024] Furthermore, shellac nanoparticles were prepared by an antisolvent precipitation method.

[0025] The preparation method of the above-mentioned antibacterial gel is as follows:

[0026] (1) Weigh a certain amount of HA, add it to RO water in batches, and vortex until it is completely dissolved to obtain a solution with a HA concentration of 1-13 mg / mL;

[0027] (2) A certain concentration of shellac nanoparticles and HA solution were mixed uniformly in a vortex to obtain a gel, and the amounts of HA solution and shellac nanoparticles were adjusted so that the concentration of shellac nanoparticles in the gel was 5-25 mg / mL.

[0028] Another object of the present invention is to provide the use of the above-mentioned shellac, antibacterial coating or antibacterial gel in the preparation of antibacterial medical materials or medical devices.

[0029] Furthermore, antibacterial coatings can be deposited on the surfaces of medical devices such as vascular stents, artificial heart valves, artificial blood pumps, artificial blood vessels, artificial joints, artificial bones, catheters, and venous filters to produce corresponding antibacterial medical materials or medical devices; or antibacterial gels can be applied to the skin or mucous membrane surfaces to improve antibacterial properties.

[0030] Beneficial effects of the present invention:

[0031] The present invention first prepares shellac nanoparticles through an antisolvent precipitation method. Then, using PLGA and HA as carriers, a shellac nanoparticle coating and a shellac nanoparticle gel are prepared. Both the coating and gel exhibit excellent antibacterial properties. The preparation method is relatively simple and has a wide range of applications, including biomedical materials, medical device coatings, and skin and mucous membrane surfaces. BRIEF DESCRIPTION OF THE DRAWINGS

[0032] Figure 1 is the Fourier infrared spectrum of the prepared PLGA-loaded shellac nanoparticle coating;

[0033] Figure 2 This is a test diagram of the antibacterial performance of shellac nanoparticles;

[0034] Figure 3 The figure shows the antibacterial performance test of the prepared PLGA-loaded shellac nanoparticle coating;

[0035] Figure 4 Figure 2 is a cell compatibility test diagram of the prepared PLGA-loaded shellac nanoparticle coating;

[0036] Figure 5 This is a graph showing the semi-in vivo blood circulation results of the prepared PLGA-loaded shellac nanoparticle coating;

[0037] Figure 6 This is a diagram showing the antibacterial performance test of the prepared HA-loaded shellac nanoparticle gel. DETAILED DESCRIPTION

[0038] The specific embodiments of the present invention are described below to facilitate understanding of the present invention by those skilled in the art. However, it should be clear that the present invention is not limited to the scope of the specific embodiments. For those skilled in the art, as long as various changes are within the spirit and scope of the present invention as defined and determined by the appended claims, these changes are obvious, and all inventions and creations utilizing the concepts of the present invention are protected.

[0039] Example 1

[0040] An antibacterial coating containing shellac nanoparticles is prepared as follows:

[0041] (1) Dissolve 2.5 g of shellac in 20 mL of anhydrous ethanol and sonicate until dissolved to obtain a shellac ethanol solution. Pass the shellac ethanol solution through a 0.22 μm syringe filter to remove insoluble matter.

[0042] (2) Using a 0.45 mm diameter syringe, drip the filtered shellac ethanol solution into 100 mL of distilled water at a rate of 122 drops / min. Stir the solution using a magnetic stirrer at 600 rpm until the shellac solution is completely dripped. Filter the raw shellac nanoparticles by vacuum filtration using slow filter paper to remove a small amount of aggregates.

[0043] (3) Evaporate the alcohol using a rotary evaporator at 60°C for 15 min. Add distilled water to the evaporated solution to make the volume 100 mL.

[0044] (4) The final colloid concentration of shellac nanoparticles was 25 mg / mL;

[0045] (5) dissolving PLGA in acetone to obtain a PLGA solution with a concentration of 20 mg / mL;

[0046] (6) adding the shellac nanoparticle solution to the PLGA solution, with the weight ratio of PLGA to shellac nanoparticles being 1:0.1 / 1:0.8;

[0047] (7) The PLGA and shellac nanoparticle solutions were thoroughly mixed, 50 μL of the mixed solution was added dropwise onto the PVC substrate, and dried at 37°C to obtain a coating.

[0048] Example 2

[0049] An antibacterial coating containing shellac nanoparticles is prepared as follows:

[0050] (1) Dissolve 2.5 g of shellac in 20 mL of anhydrous ethanol and sonicate until dissolved to obtain a shellac ethanol solution. Pass the shellac ethanol solution through a 0.22 μm syringe filter to remove insoluble matter.

[0051] (2) Using a 0.45 mm diameter syringe, drip the filtered shellac ethanol solution into 100 mL of distilled water at a rate of 122 drops / min. Stir the solution using a magnetic stirrer at 600 rpm until the shellac solution is completely dripped. Filter the raw shellac nanoparticles by vacuum filtration using slow filter paper to remove a small amount of aggregates.

[0052] (3) Evaporate the alcohol using a rotary evaporator at 60°C for 15 min. Add distilled water to the evaporated solution to make the volume 100 mL.

[0053] (4) The final colloid concentration of shellac nanoparticles was 25 mg / mL;

[0054] (5) dissolving hydroxypropyl methylcellulose in an aqueous solution to obtain a solution with a concentration of 1 mg / mL;

[0055] (6) adding the shellac nanoparticle solution to the polyhydroxymethacrylate solution, with the weight ratio of polyhydroxymethacrylate to shellac nanoparticles being 1:0.3;

[0056] (7) The hydroxypropyl methylcellulose and shellac nanoparticle solution were thoroughly mixed, and 50 μL of the mixed solution was added dropwise to the PVC substrate. The coating was obtained after vacuum drying at 37°C.

[0057] Example 3

[0058] An antibacterial coating containing shellac nanoparticles is prepared as follows:

[0059] (1) Dissolve 2.5 g of shellac in 20 mL of anhydrous ethanol and sonicate until dissolved to obtain a shellac ethanol solution. Pass the shellac ethanol solution through a 0.22 μm syringe filter to remove insoluble matter.

[0060] (2) Using a 0.45 mm diameter syringe, drip the filtered shellac ethanol solution into 100 mL of distilled water at a rate of 122 drops / min. Stir the solution using a magnetic stirrer at 600 rpm until the shellac solution is completely dripped. Filter the raw shellac nanoparticles by vacuum filtration using slow filter paper to remove a small amount of aggregates.

[0061] (3) Evaporate the alcohol using a rotary evaporator at 60°C for 15 min. Add distilled water to the evaporated solution to make the volume 100 mL.

[0062] (4) The final colloid concentration of shellac nanoparticles was 25 mg / mL;

[0063] (5) dissolving polylactic acid in chloroform to obtain a polylactic acid solution with a concentration of 30 mg / mL;

[0064] (6) adding the shellac nanoparticle solution to the polylactic acid solution, with the weight ratio of polylactic acid to shellac nanoparticles being 1:0.4;

[0065] (7) The polylactic acid and shellac nanoparticle solutions were thoroughly mixed, and 50 μL of the mixed solution was added dropwise to the PVC substrate. The coating was obtained by vacuum drying at 37°C.

[0066] Example 4

[0067] An antibacterial gel containing shellac nanoparticles, the preparation method of which is as follows:

[0068] (1) Dissolve 2.5 g of shellac in 20 mL of anhydrous ethanol and sonicate until dissolved to obtain a shellac ethanol solution. Pass the shellac ethanol solution through a 0.22 μm syringe filter to remove insoluble matter.

[0069] (2) Using a 0.45 mm diameter syringe, the filtered shellac ethanol solution was dripped into 100 mL of distilled water at a rate of 122 drops / min. The solution was stirred at 600 rpm using a magnetic stirrer until the shellac solution was completely dripped. The raw shellac nanoparticles were filtered by vacuum filtration using slow filter paper to remove a small amount of aggregates.

[0070] (3) Evaporate the alcohol using a rotary evaporator at 60°C for 15 min. Add distilled water to the evaporated solution to make the volume 100 mL.

[0071] (4) The final colloid concentration of shellac nanoparticles obtained was 25 mg / mL.

[0072] (5) Weigh a certain amount of hyaluronic acid and add it to RO water in batches. Oscillate it in a vortex until it is completely dissolved, so that the concentration of hyaluronic acid is 10 mg / mL.

[0073] (6) A certain concentration of shellac nanoparticles and hyaluronic acid were mixed uniformly in a vortex to obtain a gel. The amounts of HA solution and shellac nanoparticles were adjusted so that the concentration of shellac nanoparticles in the gel was 12.5 mg / mL.

[0074] Example 5

[0075] An antibacterial gel containing shellac nanoparticles, the preparation method of which is as follows:

[0076] (1) Dissolve 2.5 g of shellac in 20 mL of anhydrous ethanol and sonicate until dissolved to obtain a shellac ethanol solution. Pass the shellac ethanol solution through a 0.22 μm syringe filter to remove insoluble matter.

[0077] (2) Using a 0.45 mm diameter syringe, the filtered shellac ethanol solution was dripped into 100 mL of distilled water at a rate of 122 drops / min. The solution was stirred at 600 rpm using a magnetic stirrer until the shellac solution was completely dripped. The raw shellac nanoparticles were filtered by vacuum filtration using slow filter paper to remove a small amount of aggregates.

[0078] (3) Evaporate the alcohol using a rotary evaporator at 60°C for 15 min. Add distilled water to the evaporated solution to make the volume 100 mL.

[0079] (4) The final colloid concentration of shellac nanoparticles obtained was 25 mg / mL.

[0080] (5) Weigh a certain amount of chitosan, add it to acetic acid in batches, and vortex it in a vortexer until it is completely dissolved, so that the concentration of chitosan is 10 mg / mL.

[0081] (6) Mixing a certain concentration of shellac nanoparticles and chitosan in a vortex to obtain a gel. The amounts of chitosan solution and shellac nanoparticles are adjusted so that the concentration of shellac nanoparticles in the gel is 5 mg / mL.

[0082] Example 6

[0083] An antibacterial gel containing shellac nanoparticles, the preparation method of which is as follows:

[0084] (1) Dissolve 2.5 g of shellac in 20 mL of anhydrous ethanol and sonicate until dissolved to obtain a shellac ethanol solution. Pass the shellac ethanol solution through a 0.22 μm syringe filter to remove insoluble matter.

[0085] (2) Using a 0.45 mm diameter syringe, the filtered shellac ethanol solution was dripped into 100 mL of distilled water at a rate of 122 drops / min. The solution was stirred at 600 rpm using a magnetic stirrer until the shellac solution was completely dripped. The raw shellac nanoparticles were filtered by vacuum filtration using slow filter paper to remove a small amount of aggregates.

[0086] (3) Evaporate the alcohol using a rotary evaporator at 60°C for 15 min. Add distilled water to the evaporated solution to make the volume 100 mL.

[0087] (4) The final colloid concentration of shellac nanoparticles obtained was 25 mg / mL.

[0088] (5) Weigh a certain amount of polyethylene glycol and add it to RO water in batches. Oscillate it in a vortex until it is completely dissolved, so that the concentration of polyethylene glycol is 10 mg / mL.

[0089] (6) Mixing a certain concentration of shellac nanoparticles with polyethylene glycol in a vortex to obtain a gel. The amounts of polyethylene glycol solution and shellac nanoparticles are adjusted to obtain a shellac nanoparticle concentration of 25 mg / mL in the gel.

[0090] Test example

[0091] 1. Study on the performance of PLGA-loaded shellac nanoparticle coating

[0092] (1) The prepared PLGA-loaded shellac nanoparticle coating was tested by Fourier transform infrared spectroscopy. Figure 1 From the test results, it can be seen that the present invention successfully prepared the PLGA-loaded shellac nanoparticle coating.

[0093] (2) Antibacterial performance testing

[0094] The antibacterial properties of shellac nanoparticles and the prepared PLGA-loaded shellac nanoparticle coating were tested, and the results are shown in Figure 2 and Figure 3 .

[0095] like Figure 2 As shown, the shellac nanoparticles with the lowest concentration of 0.2 mg / mL had excellent antibacterial properties; Figure 3 As shown, the PLGA-loaded shellac nanoparticle coating (shellac nanoparticle concentration greater than 3.4 mg / mL) prepared in the present invention has excellent antibacterial properties.

[0096] (3) Biocompatibility testing

[0097] Figure 4 The cell compatibility of the PLGA-loaded shellac nanoparticle coatings prepared in the present invention was evaluated. The results showed that, except for the coating with a PLGA to shellac nanoparticle mass ratio of 1:0.8, which had certain cytotoxicity, the other PLGA-loaded shellac nanoparticle coatings had no cytotoxicity.

[0098] (4) Anticoagulant performance test

[0099] Figure 5 This is the semi-in vivo blood circulation result of the PLGA-loaded shellac nanoparticle coating prepared in the present invention. The result shows that the PLGA-loaded shellac nanoparticle coating prepared in the present invention also has good anti-coagulation performance.

[0100] 2. Antibacterial property test of HA-loaded shellac nanoparticle gel prepared in Example 4

[0101] Figure 6 The antibacterial (Staphylococcus aureus (positive)) performance of the HA-loaded shellac nanoparticle gel layer prepared in Example 4 of the present invention was shown. The results showed that the gel with a shellac nanoparticle concentration of 12.5 mg / mL had a good antibacterial effect.

[0102] Finally, it should be noted that the above specific implementation methods are only used to illustrate the technical solutions of the present invention and are not limiting. Although the present invention has been described in detail with reference to examples, those skilled in the art should understand that the technical solutions of the present invention can be modified or replaced by equivalents without departing from the spirit and scope of the technical solutions of the present invention, which should all be included in the scope of the claims of the present invention.

Claims

1. Use of shellac in the preparation of antibacterial products.

2. The use according to claim 1, characterized in that The antibacterial product is an antibacterial coating or an antibacterial gel.

3. An antibacterial coating containing shellac nanoparticles, characterized in that: The invention comprises shellac nanoparticles and a polymer carrier for loading the shellac nanoparticles.

4. The antibacterial coating according to claim 3, characterized in that The polymer carrier is polylactic acid-glycolic acid copolymer, hydroxypropyl methylcellulose, methylcellulose, triethyl citrate, polyethylene glycol, polyvinyl alcohol, ethyl cellulose, polylactic acid, polyglycolic acid, polylactide, polyglycolide, copolymer of polylactide and polyglycolide, polyhydroxymethylacrylate, fibrin, silicone, polysiloxane, polydimethylsiloxane, polyvinyl halide and copolymer, cellulose ether, cellulose triacetate, chitosan, and copolymers and / or mixtures of the above polymers.

5. The antibacterial coating according to claim 3 or 4, characterized in that: The weight ratio of the polymer carrier to the shellac nanoparticles is 1:0.1 to 1:2.

0.

6. The antibacterial coating according to claim 3, characterized in that The shellac nanoparticles are prepared by an anti-solvent precipitation method.

7. An antibacterial gel containing shellac nanoparticles, characterized in that: The invention comprises shellac nanoparticles and a high molecular gel matrix for loading the shellac nanoparticles.

8. The antibacterial gel according to claim 7, characterized in that The polymer gel matrix is hyaluronic acid, carbomer, hydroxypropyl methylcellulose, chitosan, xanthan gum, sodium polyacrylate, polyvinyl pyrrolidone, polyethylene glycol, and copolymers and / or mixtures of the above polymers.

9. The antibacterial gel according to claim 7, characterized in that The shellac nanoparticles are prepared by an anti-solvent precipitation method.

10. Use of the shellac according to claim 1, the antibacterial coating according to any one of claims 3 to 6, or the antibacterial gel according to any one of claims 7 to 9 in the preparation of antibacterial medical materials or medical devices.