Preparation method of degradable silk fibroin Yimei pulling wire with antibacterial function

Abstract

The invention discloses a preparation method of a degradable silk fibroin Yimei guy wire with an antibacterial function, and in the preparation process, a regenerated silk fibroin aqueous solution is promoted to be integrally formed into the silk fibroin Yimei guy wire through ultrasonic treatment, alcohol steam fumigation, heating and other treatments. The lifting line has the advantages of stable structure and performance, excellent biocompatibility, excellent flexibility, and good shape retention performance, mechanical performance and anti-swelling performance. Besides, by adding calcium ions, glycerol and polyethylene glycol, the secondary structure of the silk fibroin Yimei pulling wire can be remarkably regulated and controlled, and the degradation rate and the mechanical property of the silk fibroin Yimei pulling wire are influenced, so that the controllable degradation period and the controllable mechanical property are realized. And meanwhile, a water-soluble antibacterial substance is added into a regenerated silk fibroin aqueous solution to prepare a mixed solution, so that the antibacterial function of the silk fibroin Yimei guy wire can be realized. The silk fibroin Yimei guy can keep the face improvement effect of a patient for a long time, and does not generate toxic or side effects in the use process.

Description

Technical Field

[0001] The invention belongs to the technical field of biomedical materials and relates to a method for preparing a degradable antibacterial silk fibroin medical beauty lifting thread. Background Art

[0002] In the past few decades, barbed sutures have been widely used. This type of suture has many advantages such as no knotting, uniform tension distribution and strong anchoring effect. Barbed sutures are now used in many surgical fields such as urology, obstetrics, plastic surgery and orthopedics. The fishbone suture is a special design of barbed sutures. Its barbs are arranged in parallel and symmetrically. It is an efficient medical lifting line with significant three-dimensional support and gripping effect. It can effectively avoid the problem of suture slippage. Its deep lifting time is long and safe and stable.

[0003] At present, the fishbone-type medical beauty lifting thread is mainly made of polymer materials such as polydioxanone (PDO), polypropylene (PP), and polycaprolactone (PCL), but this type of medical beauty lifting thread has many side effects in actual application. A survey study published in the British Association of Aesthetic Plastic Surgeons Journal (ASJ) showed that when barbed sutures made of polymer materials such as PDO are used for facial lifting, the total probability of postoperative complications is 34%, of which 35 patients had transient erythema, infection, and skin depression. Even if there are no complications after surgery, the facial improvement effect of the patient does not last more than 1 year. The main cause of these problems is that the biocompatibility and functionality of polymer materials are poor, the tissue rejection reaction is strong, and the degradation rate is fast, which seriously affects the effect of fishbone-type medical beauty lifting thread in plastic surgery.

[0004] Regenerated silk fibroin is a water-soluble natural polymer protein obtained by degumming, dissolving and dialyzing natural silk. Regenerated silk fibroin contains 18 kinds of amino acids, and there are mainly two secondary structures in the crystalline region, namely SILK I (irregular structure) and SILKⅡ (β-folding). Changes in various physical and chemical conditions such as shear force, alcohol solution, high temperature, and ultrasound can effectively induce the transformation of the regenerated silk fibroin SILK I structure to the SILKⅡ structure. Regenerated silk fibroin materials with a high proportion of SILKⅡ structure (β-folding) have the characteristics of high strength and high modulus, long degradation cycle and anti-swelling. As a biomaterial, regenerated silk fibroin has excellent mechanical properties, biocompatibility and biodegradability. The regenerated silk fibroin material implanted in the body has controllable degradation performance, and the selectable degradation cycle ranges from several days to several years. Regenerated silk fibroin-based biomaterials have extremely wide applications in tissue repair and medical device implantation due to their controllable performance, low inflammatory response and easy implantation.

[0005] The patent application with publication number CN 114569282 A discloses a magnesium fishbone wire and its preparation method, but it has the disadvantages of low mechanical properties and too fast degradation rate; the patent application with publication number CN 113440190A discloses a cosmetic lifting wire and its preparation method, the main base material of which is polycaprolactone and polyethylene glycol, but the polycaprolactone wire is soft and the lifting effect is weak; the patent application with publication number CN 112315623A discloses a self-fixing plastic surgery lifting wire, the main material of which is polydioxanone, because its degradation process will release monomers, residual catalysts and material fragments, so there will be many side effects and immune reactions after implantation. In summary, the current medical beauty lifting wires generally have problems such as unsatisfactory mechanical properties, obvious tissue rejection reaction, too fast degradation and lack of antibacterial function.

[0006] Therefore, it is of great significance to develop a biodegradable antibacterial silk protein medical lifting thread. Summary of the invention

[0007] The purpose of the present invention is to provide a method for preparing a biodegradable antibacterial silk fibroin medical lifting thread to solve the problems of poor biocompatibility and strong tissue rejection reaction of existing polymer material barbed sutures.

[0008] The technical solution of the present invention is:

[0009] A method for preparing a degradable antibacterial silk fibroin medical beauty lifting thread comprises the following steps:

[0010] (1) Modeling and designing the overall shape of the fishbone-shaped medical beauty lifting thread, using a 3D printer to print a fishbone thread positive mold, mixing polydimethylsiloxane and a polydimethylsiloxane initiator and pouring them on the surface of the fishbone thread positive mold, and vacuum drying to obtain a fishbone thread negative mold;

[0011] (2) degumming, dissolving and dialyzing natural silk to obtain a regenerated silk fibroin aqueous solution, centrifuging to remove impurities, and concentrating the regenerated silk fibroin aqueous solution using polyethylene glycol to obtain a high-concentration regenerated silk fibroin aqueous solution;

[0012] (3) adding calcium chloride, glycerol and hyaluronic acid to the high-concentration regenerated silk fibroin aqueous solution, mixing them evenly to obtain a mixed solution, adding a water-soluble antibacterial substance to the mixed solution, ultrasonically treating the mixed solution to obtain a regenerated silk fibroin gel precursor solution, pouring the regenerated silk fibroin gel precursor solution into the fishbone wire negative mold, placing the mold in a vacuum drying oven, standing, demolding, and obtaining a regenerated silk fibroin gel;

[0013] (4) placing the regenerated silk fibroin gel in a vacuum dryer, using diphenylethanol to fumigate at high temperature, taking it out, and obtaining the silk fibroin medical lifting thread;

[0014] (5) ultrasonically washing the silk fibroin medical beauty lifting thread, drying it, and making an indicator line at the center line of the silk fibroin medical beauty lifting thread;

[0015] (6) The silk fibroin medical lifting thread is sterilized with ethylene oxide, and then packaged and stored to obtain the degradable antibacterial silk fibroin medical lifting thread.

[0016] Furthermore, in step (1), the printing temperature is 200-210°C, the time is 30 minutes, the material of the fishbone line positive mold is PCL, the mass ratio of the polydimethylsiloxane to the polydimethylsiloxane initiator is 10:1, the polydimethylsiloxane initiator is a platinum catalyst, and the vacuum drying temperature is 60-80°C, and the time is 2-4 hours.

[0017] Furthermore, in step (1), the specification of the fishbone wire is 0.500mm-0.599mm.

[0018] Furthermore, in step (2), the centrifugal speed is 10000 r / min, the number of times is 3 times, the time of each centrifugation is 10 min, the mass fraction of the polyethylene glycol is 15-20 wt % and the mass fraction of the high concentration regenerated silk fibroin aqueous solution is 10-20 wt %.

[0019] Furthermore, in step (3), the mass fraction of calcium chloride is 20wt%, the mass fraction of glycerol is 20wt%, the mass fraction of hyaluronic acid is 20wt%, the mass ratio of the high concentration of regenerated silk fibroin to the calcium chloride is 60:1, the mass ratio of the high concentration of regenerated silk fibroin to the glycerol and hyaluronic acid is 5-10:1-3, the concentration of the water-soluble antibacterial substance is 1-3mg / mL, the mass ratio of the water-soluble antibacterial substance to the mixed solution is 1:10, the frequency of the ultrasound is 80Hz, the time is 30-50s, the vacuum degree of the vacuum drying oven is -0.085MPa, the temperature is 40-50℃, and the time is 3-4h.

[0020] Furthermore, in step (3), the water-soluble antibacterial substance is any one or more combinations of tannic acid, gentamicin, minocycline hydrochloride, vancomycin, and curcumin.

[0021] Furthermore, in step (4), the high temperature fumigation temperature is 60° C. and the time is 4-6 hours.

[0022] Furthermore, in step (5), the power of the ultrasonic washing is 40-60 Hz, the time is 30-90 min, and the drying time is 12 h.

[0023] Furthermore, in step (6), the concentration of ethylene oxide is 500 mg / L, the sterilization temperature is 37-50° C., the time is 3-4 h, and the relative humidity is 60-80%.

[0024] Furthermore, in step (6), after the silk fibroin medical beauty lifting thread is sterilized and taken out, it is placed for 24 hours and then packaged and stored.

[0025] The present invention provides a method for preparing a degradable antibacterial silk fibroin medical beauty lifting thread, which adopts an integrated casting molding process, and induces the secondary structure of the regenerated silk fibroin to change from a random coil to a β-fold under physical and chemical conditions, during which a liquid-solid phase transition occurs, thereby obtaining a high-strength and high-modulus silk fibroin medical beauty lifting thread. Its advantages are: this product has excellent biocompatibility, excellent mechanical properties, good anti-swelling properties and morphology retention ability, stable facial improvement and maintenance effects, and can significantly reduce the inflammatory response and other side effects of the implanted part, providing patients with a better use experience, and is conducive to the further application of silk fibroin-based biomaterials in the fields of tissue repair, facial beauty, etc. BRIEF DESCRIPTION OF THE DRAWINGS

[0026] Figure 1 This is a modeling design diagram of the overall morphology of the fishbone-shaped medical beauty lifting thread in the preparation method of the degradable antibacterial silk fibroin medical beauty lifting thread described in the present invention;

[0027] Figure 2 This is a structural diagram of the degradable antibacterial functional silk fibroin medical beauty lifting thread prepared in Example 1 of the method for preparing a degradable antibacterial functional silk fibroin medical beauty lifting thread described in the present invention;

[0028] Figure 3 It is a microstructure analysis diagram of the degradable antibacterial functional silk fibroin medical lifting thread prepared in each embodiment of the preparation method of the degradable antibacterial functional silk fibroin medical lifting thread described in the present invention;

[0029] Figure 4 This is a degradation performance analysis diagram of the degradable antibacterial functional silk fibroin medical lifting thread prepared in each embodiment of the preparation method of the degradable antibacterial functional silk fibroin medical lifting thread described in the present invention;

[0030] Figure 5This is a comparison chart of the antibacterial effects of the degradable antibacterial functional silk fibroin medical beauty lifting thread (loaded with tannic acid) and the lifting thread not loaded with tannic acid prepared in each embodiment of the preparation method of the degradable antibacterial functional silk fibroin medical beauty lifting thread described in the present invention. DETAILED DESCRIPTION

[0031] The purpose of the present invention is to provide a method for preparing a degradable antibacterial silk fibroin medical beauty lifting thread, which adopts a casting process and is easy to operate.

[0032] The above method comprises the following steps:

[0033] (1) Modeling and designing the overall shape of the fishbone-shaped medical aesthetic lifting thread, using a 3D printer to print a fishbone thread positive mold, pouring polydimethylsiloxane (PDMS) and a polydimethylsiloxane initiator on the surface of the fishbone thread positive mold, and obtaining a fishbone thread negative mold;

[0034] (2) degumming, dissolving and dialyzing natural silk to obtain a regenerated silk fibroin aqueous solution, centrifuging to remove impurities, and concentrating the regenerated silk fibroin aqueous solution using polyethylene glycol (PEG) to obtain a high-concentration regenerated silk fibroin aqueous solution;

[0035] (3) adding calcium chloride, glycerol and hyaluronic acid to a high concentration of regenerated silk fibroin aqueous solution, adding a water-soluble antibacterial substance after mixing evenly, then subjecting the solution to ultrasonic treatment, pouring the regenerated silk fibroin gel precursor solution after ultrasonic treatment into a fishbone wire negative mold, placing it in a vacuum drying oven, and allowing it to stand until it becomes a gel;

[0036] (4) demolding the gelled regenerated silk fibroin, placing it in a vacuum dryer, and fumigating it with diphenylethanol at high temperature;

[0037] (5) The silk fibroin medical lifting thread after fumigation is taken out, ultrasonically cleaned, and dried. To facilitate the surgical operation, an indicator line is made at the center line of the lifting thread;

[0038] (6) Sterilize the product with ethylene oxide and then package and store it.

[0039] In order to make the above-mentioned objects, features and advantages of the present invention more clearly understood, the technical solutions of the present invention are further described below in conjunction with specific embodiments. However, the present invention is not limited to the embodiments listed, and should also include any other known changes within the scope of the rights claimed by the present invention.

[0040] The term "one embodiment" or "embodiment" as used herein refers to a specific feature, structure, or characteristic that may be included in at least one implementation of the present invention. The term "in one embodiment" that appears in different places in this specification does not necessarily refer to the same embodiment, nor does it refer to a separate or selective embodiment that is mutually exclusive with other embodiments.

[0041] Example 1

[0042] The following example shows a method for preparing a degradable antibacterial silk fibroin medical lifting thread, and the specific steps are as follows:

[0043] Step 1: Model and design the overall shape of the fishbone-shaped medical beauty lifting line. The specification of the fishbone-shaped medical beauty lifting line is No. 2 (0.52mm). Print the fishbone line positive mold through a 3D printer. The printing temperature is 200℃, the printing material is PCL, and the printing time is 30min. Mix 20mL PDMS and 2mL PDMS initiator (10:1), stir evenly, let it stand for 1h to remove bubbles, and then pour it on the surface of the fishbone line positive mold. After pouring, place it in a vacuum drying oven to wait for the fishbone line negative mold to be formed. The temperature of the vacuum drying oven is 60℃. After standing for 4h, take it out and demold it to obtain the fishbone line negative mold.

[0044] Step 2: Degumming the natural silk in alkaline water for 30 minutes, washing, air-drying and storing. At 60°C, dissolve the degummed silk with 9.8mol / L lithium bromide solution, and obtain the regenerated silk fibroin lithium bromide solution after 4 hours. After the mixed solution is cooled, it is placed in a dialysis bag (molecular weight cutoff 14kDa) for 3 days to obtain a regenerated silk fibroin protein aqueous solution. Centrifuge the regenerated silk fibroin protein aqueous solution to remove impurities at a centrifugal speed of 10000r / min. Take the supernatant after centrifugation, continue centrifugation, centrifuge 3 times, 10 minutes each time, and store in a 4°C refrigerator after centrifugation. Use 20wt% PEG (molecular weight 20kDa) to concentrate the regenerated silk fibroin to obtain a 15wt% concentration of regenerated silk fibroin protein aqueous solution.

[0045] Step 3: Add 20wt% glycerol and 20wt% hyaluronic acid to the 15wt% regenerated silk fibroin aqueous solution at a mass ratio of 10:1, and then add 20wt% calcium chloride solution at a mass ratio of 60:1 to prepare a mixed solution. Add 3mg / mL tannic acid to the mixed solution at a mass ratio of 1:10, oscillate, and mix evenly. Ultrasonicate the mixed solution with an ultrasonic power of 80Hz and an ultrasonic time of 30s. After ultrasound, cast the regenerated silk fibroin gel precursor solution into a PDMS fishbone wire mold, place it in a vacuum drying oven, and evacuate the vacuum to -0.085MPa. The temperature of the vacuum drying oven is set to 40°C, and the treatment time is 4h. Wait for it to gel to obtain a regenerated silk fibroin gel.

[0046] Step 4: Evenly apply vaseline on the surface of the regenerated silk fibroin gel, demould, and obtain the gel-state silk fibroin medical beauty lifting thread. Put the gel-state silk fibroin medical beauty lifting thread into a vacuum dryer and fumigate with diphenylethanol at a fumigation temperature of 60°C for 6 hours.

[0047] Step 5: Ultrasonic wash the fumigated silk protein medical lifting thread at a power of 40Hz for three times, each time for 30 minutes, to completely remove the residual organic solvent on the surface. Finally, use dust-free paper to absorb the moisture on the surface of the silk protein medical lifting thread, air-dry it in a fume hood for 12 hours, and make an indicator line at the center line of the silk protein medical lifting thread.

[0048] Step 6: Use ethylene oxide to sterilize the product, the sterilization temperature is 40°C, the sterilization time is 4h, the ethylene oxide concentration is 500mg / L, and the relative humidity is 60%.

[0049] Example 2

[0050] The following example shows a method for preparing a degradable antibacterial silk fibroin medical lifting thread, and the specific steps are as follows:

[0051] Step 1: Design the overall shape of the fishbone-shaped medical beauty lifting line through blender software. The specification of the fishbone-shaped medical beauty lifting line is No. 2 (0.52mm). Print the fishbone line positive mold through a 3D printer. The printing temperature is 210℃, the printing material is PCL, and the printing time is 30min. Mix 30mL PDMS and 3mL PDMS initiator (10:1), stir evenly, let stand for 1h to remove bubbles, and then pour it on the surface of the fishbone line positive mold. After pouring, place it in a vacuum drying oven to wait for the fishbone line negative mold to be formed. The temperature of the vacuum drying oven is 60℃. After standing for 4h, take it out and demold it to obtain the fishbone line negative mold.

[0052] Step 2: Degumming natural silk in alkaline water for 60 minutes, washing, air-drying and storing. At 60°C, dissolve the degummed silk with 9.8mol / L lithium bromide solution, and obtain regenerated silk fibroin lithium bromide solution after 4 hours. After the mixed solution is cooled, it is placed in a dialysis bag (molecular weight cutoff 14kDa) for 3 days to obtain a regenerated silk fibroin protein aqueous solution. Centrifuge the regenerated silk fibroin protein aqueous solution to remove impurities at a centrifugal speed of 10000r / min. Take the supernatant after centrifugation and continue centrifugation for 3 times, 10 minutes each time. Store in a refrigerator at 4°C after centrifugation. Use 20wt% PEG (molecular weight 20kDa) to concentrate the regenerated silk fibroin to obtain a 20wt% concentration of regenerated silk fibroin protein aqueous solution.

[0053] Step 3: Add 20wt% glycerol and 20wt% hyaluronic acid to the 20wt% regenerated silk fibroin aqueous solution at a mass ratio of 5:1, and then add 20wt% calcium chloride solution at a mass ratio of 60:1 to prepare a mixed solution. Add 2mg / mL tannic acid to the mixed solution at a mass ratio of 1:10, oscillate, and mix evenly. Ultrasonicate the mixed solution with an ultrasonic power of 80Hz and an ultrasonic time of 40s. After ultrasound, cast the regenerated silk fibroin gel precursor solution into a PDMS fishbone wire mold, place it in a vacuum drying oven, and evacuate the vacuum to -0.085MPa. The temperature of the vacuum drying oven is set to 45°C, and the treatment time is 3h. Wait for it to gel and obtain a regenerated silk fibroin gel.

[0054] Step 4: Evenly apply vaseline on the surface of the regenerated silk fibroin gel, demould, and obtain the gel-state silk fibroin medical beauty lifting thread. Put the gel-state silk fibroin medical beauty lifting thread into a vacuum dryer and fumigate with diphenylethanol at a fumigation temperature of 60°C for 5 hours.

[0055] Step 5: Ultrasonic wash the fumigated silk protein medical lifting thread at a power of 40Hz for three times, each time for 30 minutes, to completely remove the residual organic solvent on the surface. Finally, use dust-free paper to absorb the moisture on the surface of the silk protein medical lifting thread, air-dry it in a fume hood for 12 hours, and make an indicator line at the center line of the silk protein medical lifting thread.

[0056] Step 6: Use ethylene oxide to sterilize the product, the sterilization temperature is 45°C, the sterilization time is 3h, the ethylene oxide concentration is 500mg / L, and the relative humidity is 80%.

[0057] Example 3

[0058] The following example shows a method for preparing a degradable antibacterial silk fibroin medical lifting thread, and the specific steps are as follows:

[0059] Step 1: Design the overall shape of the fishbone-shaped medical beauty lifting line through blender software. The specification of the fishbone-shaped medical beauty lifting line is No. 2 (0.52mm). Print the fishbone line positive mold through a 3D printer. The printing temperature is 210℃, the printing material is PCL, and the printing time is 30min. Mix 400mL PDMS and 4mL PDMS initiator (10:1), stir evenly, let stand for 1h to remove bubbles, and then pour it on the surface of the fishbone line positive mold. After pouring, place it in a vacuum drying oven to wait for the fishbone line negative mold to be formed. The temperature of the vacuum drying oven is 80℃. After standing for 2h, take it out and demold it to obtain the fishbone line negative mold.

[0060] Step 2: Degumming natural silk in alkaline water for 30 minutes, washing, air-drying and storing. At 60°C, dissolve the degummed silk with 9.8 mol / L lithium bromide solution, and obtain regenerated silk fibroin lithium bromide solution after 4 hours. After the mixed solution is cooled, it is placed in a dialysis bag (molecular weight cutoff 14kDa) for 3 days to obtain a regenerated silk fibroin protein aqueous solution. Centrifuge the regenerated silk fibroin protein aqueous solution to remove impurities at a centrifugal speed of 10000r / min. Take the supernatant after centrifugation and continue centrifugation for 3 times, 10 minutes each time. Store in a refrigerator at 4°C after centrifugation. Use 15wt% PEG (molecular weight 10kDa) to concentrate the regenerated silk fibroin to obtain a 10wt% concentration of regenerated silk fibroin protein aqueous solution.

[0061] Step 3: Add 20wt% glycerol and 20wt% hyaluronic acid to the 10wt% regenerated silk fibroin aqueous solution at a mass ratio of 10:3, and then add 20wt% calcium chloride solution at a mass ratio of 60:1 to prepare a mixed solution. Add 1mg / mL tannic acid to the mixed solution at a mass ratio of 1:10, oscillate, and mix evenly. Ultrasonicate the mixed solution with an ultrasonic power of 80Hz and an ultrasonic time of 50s. After ultrasound, cast the regenerated silk fibroin gel precursor solution into a PDMS fishbone wire mold, place it in a vacuum drying oven, and evacuate the vacuum to -0.085MPa. The temperature of the vacuum drying oven is set to 40°C, and the treatment time is 4h. Wait for it to gel to obtain a regenerated silk fibroin gel.

[0062] Step 4: Evenly apply vaseline on the surface of the regenerated silk fibroin gel, demould, and obtain the gel-state silk fibroin medical beauty lifting thread. Put the gel-state silk fibroin medical beauty lifting thread into a vacuum dryer and fumigate with diphenylethanol at a fumigation temperature of 60°C for 4 hours.

[0063] Step 5: Ultrasonic wash the fumigated silk protein medical lifting thread at a power of 60Hz for three times, each time for 30 minutes, to completely remove the residual organic solvent on the surface. Finally, use dust-free paper to absorb the moisture on the surface of the silk protein medical lifting thread, air-dry it in a fume hood for 12 hours, and make an indicator line at the center line of the silk protein medical lifting thread.

[0064] Step 6: Use ethylene oxide to sterilize the product, the sterilization temperature is 50°C, the sterilization time is 4h, the ethylene oxide concentration is 500mg / L, and the relative humidity is 70%.

[0065] See also Figure 1 , Figure 1 This is a modeling design diagram of the overall shape of the fishbone-shaped medical beauty lifting thread in the preparation method of a degradable antibacterial silk fibroin medical beauty lifting thread described in the present invention. Figure 1As shown in the figure, the overall shape of the medical lifting line is fishbone-shaped, and the barbs are designed with blunt angles, which effectively avoids the stimulation of facial tissue during the lifting process. At the same time, the barbs have a serrated structure, which can increase the grip effect of the lifting line. There is a black indicator line mark at the center line of the lifting line to facilitate surgical operations.

[0066] See also Figure 2 , Figure 2 This is a structural diagram of the degradable antibacterial silk fibroin medical lifting thread prepared in Example 1 of the preparation method of the degradable antibacterial silk fibroin medical lifting thread described in the present invention. Figure 2 As shown, the silk fibroin medical lifting thread has excellent flexibility after ultrasound, gelation, fumigation, drying and sterilization. It can still maintain a stable morphological structure after stretching, winding and bending, and has excellent mechanical properties.

[0067] See also Figure 3 , Figure 3 This is a microstructure analysis diagram of the degradable antibacterial silk fibroin medical lifting thread prepared in each embodiment of the preparation method of the degradable antibacterial silk fibroin medical lifting thread described in the present invention. Figure 3 As shown in the figure, the silk protein medical lifting thread was frozen with liquid nitrogen, dried in a freeze dryer for 24 hours, and then taken out. A high-power scanning electron microscope was used to analyze the obvious nanowire structure, which is a microscopic manifestation of high β-folding content. The freeze-dried sample of silk protein fishbone thread was analyzed by XRD. The X-ray diffraction spectrum showed peaks at 20.7 and 24.3, which is a typical manifestation of SILKⅡ type crystalline structure. Infrared analysis showed that the characteristic peaks were mainly amide I (1600-1700cm -1 ) and amide II (1500-1600cm -1 ).

[0068] See also Figure 4 , Figure 4 This is a degradation performance analysis diagram of the degradable antibacterial silk fibroin medical lifting thread prepared in each embodiment of the preparation method of the degradable antibacterial silk fibroin medical lifting thread described in the present invention. Figure 4 As shown in the figure, the silk fibroin medical lifting thread was placed in phosphate buffer solution (PBS) and protein XIV solution (ProteaseXIV) to simulate the in vivo degradation process, and the experimental environment temperature was maintained at 37°C. The quality changes of the samples were detected within 35 days, and the statistical results showed that the regenerated silk fibroin lifting thread with high β-folding content after regulation by glycerol and calcium ions had a higher quality residual rate and stronger resistance to degradation.

[0069] See also Figure 5 , Figure 5This is a comparison chart of the antibacterial effects of the degradable antibacterial silk fibroin medical lifting thread (loaded with tannic acid) and the non-loaded tannic acid lifting thread prepared in each embodiment of the preparation method of the degradable antibacterial silk fibroin medical lifting thread described in the present invention. Figure 5 As shown, according to GB / T 20944.3-2008, the prepared samples were placed in PBS for 24 hours of shaking, sample group 1 was the blank group, and sample group 2 was the drug-loaded pulling wire group, and the inhibitory effects on Escherichia coli (E.coil) and Staphylococcus aureus (S.aureus) were characterized. The results showed that the inhibition rates of the loaded tannic acid pulling wire on Escherichia coli and Staphylococcus aureus were 81.78±1.73% and 92.32±0.41%, respectively, which met the antibacterial effect requirements specified in the national standard (>50%).

[0070]

[0071]

[0072] Table 1

[0073] Please refer to Table 1, which is a comparison table between the present invention and various thread lifting patents. As shown in Table 1, the drug release rate and degradation rate of the method of the present invention are both controllable.

[0074] In summary, the preparation method of a degradable antibacterial silk fibroin medical beauty lifting thread described in the present invention, during the preparation process, the regenerated silk fibroin aqueous solution is integrated into a silk fibroin medical beauty lifting thread through treatments such as ultrasound, alcohol vapor fumigation, and heating. The formed silk fibroin medical beauty lifting thread has a stable structure and performance, excellent biocompatibility, excellent flexibility, and good shape retention, mechanical properties, and anti-swelling properties. In addition, by adding calcium ions, glycerol, and polyethylene glycol (PEG), the secondary structure of the silk fibroin medical beauty lifting thread can be significantly regulated, affecting the degradation rate and mechanical properties of the silk fibroin medical beauty lifting thread, thereby achieving a controllable degradation cycle and controllable mechanical properties. At the same time, water-soluble antibacterial substances such as tannic acid are added to the regenerated silk fibroin aqueous solution to configure a mixed solution, which can realize the antibacterial function of the silk fibroin medical beauty lifting thread. The silk fibroin medical beauty lifting thread can maintain the patient's facial improvement effect for a long time, and does not produce toxic side effects during use.

[0075] It should be noted that the above embodiments are only used to illustrate the technical solutions of the present invention rather than to limit it. Although the present invention has been described in detail with reference to the preferred embodiments, those skilled in the art should understand that the technical solutions of the present invention may 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. A method for preparing a degradable antibacterial silk fibroin medical beauty lifting thread, characterized in that: The following steps are involved: (1) Modeling and designing the overall shape of the fishbone-shaped medical beauty lifting thread, using a 3D printer to print a fishbone thread positive mold, mixing polydimethylsiloxane and a polydimethylsiloxane initiator and pouring them on the surface of the fishbone thread positive mold, and vacuum drying to obtain a fishbone thread negative mold; (2) degumming, dissolving and dialyzing natural silk to obtain a regenerated silk fibroin aqueous solution, centrifuging to remove impurities, and concentrating the regenerated silk fibroin aqueous solution using polyethylene glycol to obtain a high-concentration regenerated silk fibroin aqueous solution; (3) adding calcium chloride, glycerol and hyaluronic acid to the high-concentration regenerated silk fibroin aqueous solution, mixing them evenly to obtain a mixed solution, adding a water-soluble antibacterial substance to the mixed solution, ultrasonically treating the mixed solution to obtain a regenerated silk fibroin gel precursor solution, pouring the regenerated silk fibroin gel precursor solution into the fishbone wire negative mold, placing the mold in a vacuum drying oven, standing, demolding, and obtaining a regenerated silk fibroin gel; (4) placing the regenerated silk fibroin gel into a vacuum dryer, using diphenylethanol to fumigate at high temperature, taking it out, and obtaining the silk fibroin medical lifting thread; (5) ultrasonically washing the silk fibroin medical beauty lifting thread, drying it, and making an indicator line at the center line of the silk fibroin medical beauty lifting thread; (6) The silk fibroin medical lifting thread is sterilized with ethylene oxide, and then packaged and stored to obtain the degradable antibacterial silk fibroin medical lifting thread.

2. The method for preparing a degradable antibacterial silk fibroin medical beauty lifting thread according to claim 1, characterized in that: In step (1), the printing temperature is 200-210°C, the time is 30 minutes, the material of the fishbone line positive mold is PCL, the mass ratio of the polydimethylsiloxane to the polydimethylsiloxane initiator is 10:1, the polydimethylsiloxane initiator is a platinum catalyst, the vacuum drying temperature is 60-80°C, and the time is 2-4 hours.

3. The method for preparing a degradable antibacterial silk fibroin medical beauty lifting thread according to claim 1, characterized in that: In step (1), the specification of the fishbone wire is 0.500mm-0.599mm.

4. The method for preparing a degradable antibacterial silk fibroin medical beauty lifting thread according to claim 1, characterized in that: In step (2), the centrifugal speed is 10000 r / min, the number of times is 3, the time of each centrifugation is 10 min, the mass fraction of polyethylene glycol is 15-20 wt % and the mass fraction of the high concentration regenerated silk fibroin aqueous solution is 10-20 wt %.

5. The method for preparing a degradable antibacterial silk fibroin medical beauty lifting thread according to claim 1, characterized in that: In step (3), the mass fraction of calcium chloride is 20wt%, the mass fraction of glycerol is 20wt%, the mass fraction of hyaluronic acid is 20wt%, the mass ratio of the high concentration of regenerated silk fibroin to the calcium chloride is 60:1, the mass ratio of the high concentration of regenerated silk fibroin to the glycerol and hyaluronic acid is 5-10:1-3, the concentration of the water-soluble antibacterial substance is 1-3mg / mL, the mass ratio of the water-soluble antibacterial substance to the mixed solution is 1:10, the frequency of the ultrasound is 80Hz, the time is 30-50s, the vacuum degree of the vacuum drying oven is -0.085MPa, the temperature is 40-50℃, and the time is 3-4h.

6. The method for preparing a degradable antibacterial silk fibroin medical beauty lifting thread according to claim 1, characterized in that: In step (3), the water-soluble antibacterial substance is any one or more combinations of tannic acid, gentamicin, minocycline hydrochloride, vancomycin, and curcumin.

7. The method for preparing a degradable antibacterial silk fibroin medical beauty lifting thread according to claim 1, characterized in that: In step (4), the high temperature fumigation temperature is 60° C. and the time is 4-6 hours.

8. The method for preparing a degradable antibacterial silk fibroin medical beauty lifting thread according to claim 1, characterized in that: In step (5), the power of the ultrasonic washing is 40-60 Hz, the time is 30-90 min, and the drying time is 12 h.

9. The method for preparing a degradable antibacterial silk fibroin medical beauty lifting thread according to claim 1, characterized in that: In step (6), the concentration of ethylene oxide is 500 mg / L, the sterilization temperature is 37-50° C., the time is 3-4 h, and the relative humidity is 60-80%.

10. The method for preparing a degradable antibacterial silk fibroin medical beauty lifting thread according to claim 1, characterized in that: In step (6), after the silk fibroin medical beauty lifting thread is sterilized and taken out, it is placed for 24 hours and then packaged and stored.

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