CN113321820A

CN113321820A - Preparation method and application of novel antibacterial adhesive moisturizing hydrogel

Info

Publication number: CN113321820A
Application number: CN202110591185.8A
Authority: CN
Inventors: 林权; 杨欣婷; 贺亮; 马程远; 刘厚; 冯钰斌; 关琳
Original assignee: Jilin University
Current assignee: Jilin University
Priority date: 2021-05-28
Filing date: 2021-05-28
Publication date: 2021-08-31

Abstract

The invention provides a preparation method and application of novel antibacterial adhesive moisturizing hydrogel. The prepared multifunctional hydrogel has excellent adhesion and mechanical properties to various materials, and has excellent lasting antibacterial property and broad-spectrum antibacterial function within 100 h. Can be used as a film to be pasted on the surfaces of catheters and other instruments which need to be adhered and antibacterial, and can prevent bacteria from invading the instruments for a long time. The novel antibacterial adhesive hydrogel has great potential as a novel antibacterial adhesive tape for fixing the catheter, and has wide application prospect in the aspects of preventing urinary tract infection and the like.

Description

Preparation method and application of novel antibacterial adhesive moisturizing hydrogel

Technical Field

The invention belongs to the technical field of high polymer materials, and particularly relates to preparation of a novel hydrogel with antibacterial, adhesive and moisturizing functions and application of the hydrogel in ureteral sticking films and prevention of urinary tract infection.

Background

Ureters are one of the most implanted devices for treating urinary system diseases at present. After the ureter is implanted into a human body, external bacteria can be gathered on the ureter and cause urinary tract infection with a certain probability. According to previous studies, within one week of ureter implantation, the probability of bacteria accumulating in the ureter is 28% to 90%, with a probability of urinary tract infection occurring of 7% to 34%, while the bacteria accumulating in the ureter are mostly of extracorporeal origin and more than 95% of urinary tract infections are caused by a single bacterium. Therefore, a nurse is required to disinfect the exterior of the ureter every day, which causes a great burden on medical staff and also causes a certain pain to patients. Meanwhile, in the medical field, the materials for fixing the infusion tube or the catheter have the problems of poor air permeability and antibacterial property, easy allergy and the like. The hydrogel is a substance with a three-dimensional polymer network structure, and compared with other materials, the hydrogel has many unique characteristics, such as enough flexibility, elasticity, biocompatibility, high water content, stability to physiological environment and the like. The unique macroporous structure of the hydrogel brings good air permeability for the hydrogel material, and the hydrogel material with good biocompatibility is combined with the antibacterial component to prepare the hydrogel with biocompatibility, air permeability and antibacterial property, and the hydrogel can be widely applied to the medical field and daily life.

Considering that hydrogel adhesion and antibacterial properties are greatly affected by the water content of hydrogel, glycerol was added to the hydrogel. The glycerin as a liquid with good biocompatibility can form a large number of hydrogen bonds with water molecules in the hydrogel and other components in the hydrogel, so that the volatilization of the water molecules in the hydrogel is slowed down, and the mechanical property of the hydrogel is enhanced. So that the hydrogel can have the properties of adhesion, antibiosis, moisture retention and the like for a long time. Therefore, the novel antibacterial adhesive hydrogel can be well pasted on a catheter as a pasting film, has a good sterilization effect and has good property of preventing urinary tract infection.

Disclosure of Invention

The invention aims to provide a preparation method of a novel antibacterial adhesive moisturizing hydrogel and application of the hydrogel in ureter sticking films and prevention of urinary tract infection.

The method comprises the steps of firstly dissolving antibacterial macromolecules, acrylic acid, polydopamine, methylene bisacrylamide and a photoinitiator I2959 in a certain proportion into a binary mixed solvent of glycerol and water, and forming the hydrogel with the double-network structure by adopting a photopolymerization method after uniformly mixing. Abundant functional groups on the surface of the hydrogel, particularly benzene rings and hydroxyl groups provided by polydopamine, endow the hydrogel with good adhesiveness; the addition of the antibacterial polymer not only enables the hydrogel to have lasting antibacterial property, but also is combined with polyacrylic acid through electrostatic interaction to form a double network, so that the mechanical property of the hydrogel is greatly improved; in addition, glycerin is added into the hydrogel as a humectant, so that the hydrogel can keep excellent adhesiveness and antibacterial property for a long time. By combining the characteristics, the novel antibacterial adhesive hydrogel has great potential as a novel antibacterial adhesive tape for fixing the catheter, and has wide application prospect in the aspects of sticking a film on the catheter, preventing urinary tract infection and the like.

The preparation method of the novel adhesive, antibacterial and temperature-tolerant hydrogel comprises the following specific steps:

(1) dopamine hydrochloride was dissolved in a NaOH solution at pH 11 to a solution concentration of 10 mg/mL. The dopamine was polymerized to polydopamine by stirring at room temperature for 5 h.

(2) Preparing a mixed solution with the volume ratio of water to glycerol of 4: 1-3: 2, putting 6.6mL of the mixed solution into a round-bottom flask, adding 0.1-0.3 g of electropositive antibacterial polymer, continuously stirring for 3 hours at room temperature, after the mixed solution becomes a uniform solution, adding 0.3-1.2mL of polydopamine solution, and after the solution is uniformly mixed; sequentially adding 1.5-3mL of Acrylic Acid (AA), 4.0-6.0 mg of crosslinking monomer and 20-60mg of photoinitiator I2959, and uniformly stirring in a dark place; and then pouring the obtained mixed solution into a polytetrafluoroethylene mold, and irradiating for 20min under the irradiation of an ultraviolet lamp with the wavelength of 365nm and the power of 35W to form the adhesive antibacterial moisturizing functional hydrogel.

In the method, the electropositive antibacterial polymer is a natural or synthetic polymer bacteriostatic agent with positive charges, such as polylysine, quaternary ammonium salt chitosan or antibacterial polypeptide.

In the method, if the electropositive antibacterial polymer is selected to be the quaternary ammonium salt chitosan, the grafting ratio of the quaternary ammonium salt is 90-98%.

In the above method, the crosslinking monomer is N, N' -Methylenebisacrylamide (MBA) or polyethylene glycol diacrylate (PEGDA) crosslinking agent.

The invention has the following advantages: 1. the hydrogel disclosed by the invention has excellent adhesiveness and mechanical property, has stronger adhesiveness and mechanical strength aiming at different organic and inorganic surfaces, can be used as an excellent adhesive tape for fixing a catheter, and is very convenient to replace; 2. the hydrogel has relatively durable antibacterial property and broad-spectrum antibacterial function within 100 hours; 3. the hydrogel can be used as a film to be pasted on the surfaces of catheters and other instruments which need to be adhered and antibacterial, so that external bacteria can be prevented from invading the catheters and other instruments for a long time; 4. the water content of the hydrogel can reach more than 60% for a long time, and the adhesiveness and antibacterial property of the hydrogel can be maintained for a long time, so that the hydrogel can be ensured not to be replaced for a long time; 5. the scanning electron microscope image of the hydrogel after freeze-drying shows that the hydrogel is a loose porous structure, has good air permeability and prevents the skin contacting with the hydrogel from generating phenomena such as allergy and the like; 6. the hydrogel has wide raw material source, easy storage and good biocompatibility, and is favorable for commercialization of products; 7. the hydrogel preparation operation process is simple and convenient, and is green and pollution-free; 8. the invention is suitable for the surface antibiosis of the fixed object surface of the catheter and the like, and has wide application prospect.

Drawings

FIG. 1: phase transition diagram of the multifunctional hydrogel dressing prepared for example 1. By comparing the front and back changes of the substances in the inclined reagent bottle, the hydrogel precursor is in a brown liquid state and is changed into a light brown gel state after being polymerized by ultraviolet light.

FIG. 2: scanning electron micrographs of the multifunctional hydrogel dressing prepared in example 1 after lyophilization. From the figure, we can clearly see the loose and porous structure in the hydrogel, so that the hydrogel has good air permeability and prevents the occurrence of allergy.

FIG. 3: the adhesive figures of the multifunctional hydrogel dressing prepared for example 1 with different materials. We can see that the prepared hydrogel can be adhered to the surfaces of different substances and has stronger adhesiveness.

FIG. 4: is a graph of in vitro antibiotic experiments of the antibiotic adhesive hydrogel prepared in example 1. The percentage in the figure is the mass fraction of the electropositive antibacterial polymer, and the growth curve diagram of escherichia coli and staphylococcus aureus of a control group and a PAA-QCS-PDA hydrogel group at 37 ℃ can be seen as the antibacterial ring is larger and larger along with the increase of the concentration of the antibacterial polymer, which indicates that the hydrogel provided by the invention has good antibacterial performance.

Detailed Description

Example 1:

(2) Preparing a mixed solution with the volume ratio of water to glycerol of 4: 1-3: 2, putting 6.6mL of the mixed solution into a round-bottom flask, adding 0.1-0.3 g of quaternary ammonium salt chitosan, continuously stirring for 3 hours at room temperature, after the mixed solution becomes a uniform solution, adding 0.3-1.2mL of polydopamine solution, and after the solution is uniformly mixed; sequentially adding 1.5-3mL of Acrylic Acid (AA), 4.0-6.0 mg of N, N' -Methylene Bisacrylamide (MBA) and 20-60mg of photoinitiator I2959, and uniformly stirring in a dark place; and then pouring the obtained mixed solution into a polytetrafluoroethylene mold, and irradiating for 20min under the irradiation of an ultraviolet lamp with the wavelength of 365nm and the power of 35W to form the hydrogel with the adhesive antibacterial function.

Example 2:

(2) Preparing a mixed solution with the volume ratio of water to glycerol of 4: 1-3: 2, putting 6.6mL of the mixed solution into a round-bottom flask, adding 0.1-0.3 g of polylysine, continuously stirring for 3 hours at room temperature, after the mixed solution becomes a uniform solution, adding 0.3-1.2mL of polydopamine solution, and after the solution is uniformly mixed; sequentially adding 1.5-3mL of Acrylic Acid (AA), 4.0-6.0 mg of N, N' -Methylene Bisacrylamide (MBA) and 20-60mg of photoinitiator I2959, and uniformly stirring in a dark place; and then pouring the obtained mixed solution into a polytetrafluoroethylene mold, and irradiating for 20min under the irradiation of an ultraviolet lamp with the wavelength of 365nm and the power of 35W to form the hydrogel with the adhesive antibacterial function.

Example 3:

(2) Preparing a mixed solution with the volume ratio of water to glycerol of 4: 1-3: 2, putting 6.6mL of the mixed solution into a round-bottom flask, adding 0.1-0.3 g of antibacterial polypeptide, continuously stirring at room temperature for 3 hours, after the mixed solution becomes a uniform solution, adding 0.3-1.2mL of polydopamine solution, and after the solution is uniformly mixed; sequentially adding 1.5-3mL of Acrylic Acid (AA), 4.0-6.0 mg of polyethylene glycol diacrylate (PEGDA) and 20-60mg of photoinitiator I2959, and uniformly stirring in a dark place; and then pouring the obtained mixed solution into a polytetrafluoroethylene mold, and irradiating for 20min under the irradiation of an ultraviolet lamp with the wavelength of 365nm and the power of 35W to form the hydrogel with the adhesive antibacterial function.

Claims

1. A preparation method of novel antibacterial adhesive moisturizing hydrogel is characterized by comprising the following steps: the method comprises the following specific steps:

(1) dissolving dopamine hydrochloride in a NaOH solution with the pH value of 11 to ensure that the concentration of the solution is 10 mg/mL; stirring for 5h at room temperature to polymerize dopamine into polydopamine;

2. The method for preparing a novel antibacterial adhesive moisturizing functional hydrogel as claimed in claim 1, wherein the method comprises the following steps: the electropositive antibacterial polymer in the step (1) is a natural or synthetic polymer bacteriostatic agent with positive charges, such as polylysine, quaternary ammonium salt chitosan or antibacterial polypeptide.

3. The method for preparing a novel antibacterial adhesive moisturizing functional hydrogel as claimed in claim 1, wherein the method comprises the following steps: if the electropositive antibacterial polymer selected in the step (1) is quaternary ammonium salt chitosan, the grafting ratio of the quaternary ammonium salt is 90-98%.

4. The method for preparing a novel antibacterial adhesive moisturizing functional hydrogel as claimed in claim 1, wherein the method comprises the following steps: the crosslinking monomer in the step (1) is N, N' -Methylene Bisacrylamide (MBA) or polyethylene glycol diacrylate (PEGDA) crosslinking agent.

5. The hydrogel prepared by the preparation method of any one of the novel antibacterial adhesive moisturizing functional hydrogels of claims 1-4, which is characterized in that: the hydrogel has good adhesion to various materials, and has excellent lasting antibacterial performance and broad-spectrum antibacterial function within 100 h; can be used as a film to be pasted on the inner sides of catheters and other instruments which need to be adhered and antibacterial, and can prevent bacteria from invading the instruments for a long time.

6. The hydrogel prepared by the preparation method of any one of the novel antibacterial adhesive moisturizing functional hydrogels of claims 1-4, which is characterized in that: the hydrogel can be used as an antibacterial adhesive tape to be adhered to the outer side of the catheter, so that bacteria invading from the outside are killed, and the probability of urinary tract infection is reduced.