Traditional Chinese medicine compound mouthwash for resisting dental plaque and preparation method thereof

Abstract

The invention provides traditional Chinese medicine compound mouthwash for resisting dental plaque and a preparation method thereof, and belongs to the technical field of oral care, and the traditional Chinese medicine compound mouthwash comprises the following raw material components in percentage by weight: 6-10% of honeysuckle flower extract, 1-5% of volatile oil clathrate compound, 0.03-0.06% of hydrogen peroxide, 1-5% of xylitol, 0.5-1% of surfactant, 0.1-0.3% of preservative, 0.1-0.8% of sodium dihydrogen phosphate, 0.2-1.2% of disodium hydrogen phosphate and the balance of water. The volatile oil clathrate compound is a clathrate compound of a carboxymethyl-beta-cyclodextrin / chitosan / Fe3O4 nano compound and mixed volatile oil of eupatorium fortunei and agastache rugosus. The nano-composite catalyzes trace hydrogen peroxide to generate hydroxyl radicals, the antibacterial effect of the traditional Chinese medicine components is synergistically enhanced, and the effect of inhibiting a dental plaque biofilm is excellent.

Description

Technical Field

[0001] The present invention relates to the technical field of oral care, and in particular to an anti-dental plaque Chinese medicinal compound mouthwash and a preparation method thereof. Background Art

[0002] Oral health is closely related to people's quality of life. Brushing teeth, as the main way of daily oral cleaning, can only remove some bacteria on the surface of the teeth and cannot thoroughly clean them. Mouthwash, as a common oral cleaning and care product, plays an important role in maintaining oral hygiene and preventing oral diseases.

[0003] Currently, most mouthwashes on the market contain chemical antibacterial agents, of which chlorhexidine is a commonly used one. Although chlorhexidine has certain antibacterial effects, long-term use can be harmful to the human body. Moreover, chlorhexidine has a better bactericidal effect on suspended bacteria, but its effectiveness is significantly reduced for bacteria attached to dental plaque biofilms. Dental plaque is a soft, unmineralized bacterial community wrapped in a matrix that adheres to each other or to the tooth surface, between teeth, or on the surface of restorations. It cannot be washed away or rinsed away by water. The bacteria in the dental plaque biofilm are wrapped in a protective matrix of extracellular polysaccharides (EPS), making it difficult for bactericides to penetrate. Bacteria that remain on the EPS surface are easily removed by saliva, making it impossible to remove bacteria associated with the dental plaque biofilm, affecting the prevention and treatment of oral diseases.

[0004] Traditional Chinese medicine mouthwashes are favored by some consumers for their natural and gentle properties. However, they also face challenges in their development and application. Certain components of traditional Chinese medicine, such as volatile oils, have poor solubility, making it difficult for the active ingredients in mouthwashes to fully dissolve. This results in low concentrations of active ingredients in the mouthwash, making it difficult to effectively inhibit oral bacteria. Furthermore, individual traditional Chinese medicine components still face the problem of being unable to penetrate EPS.

[0005] Hydrogen peroxide is an oxidizing substance. The hydroxyl radicals it produces can destroy key components of EPS, reduce EPS viscosity, and break through the bacterial barrier. However, in actual use, hydrogen peroxide takes effect relatively slowly, and to achieve the desired antibacterial effect, high concentrations of hydrogen peroxide are often required for treatment. However, high concentrations of hydrogen peroxide can damage oral tissues, causing irritation, pain, and other discomfort in the oral mucosa, which limits its widespread use in mouthwashes.

[0006] Existing oral rinses have many deficiencies in the treatment process and cannot meet people's demand for efficient and safe oral care products. Therefore, the development of an efficient and safe oral rinse has important practical significance and broad market prospects. Summary of the Invention

[0007] The object of the present invention is to provide an anti-plaque Chinese medicine compound mouthwash and a preparation method thereof, so as to solve the problems raised in the above background technology.

[0008] To achieve the above object, the present invention provides the following technical solutions:

[0009] The invention discloses a traditional Chinese medicine composite mouthwash for resisting dental plaque. The mouthwash comprises the following raw materials, measured by weight percentage: 6-10% of honeysuckle flower extract, 1-5% of volatile oil inclusion compound, 0.03-0.06% of hydrogen peroxide, 1-5% of xylitol, 0.5-1% of surfactant, 0.1-0.3% of preservative, 0.1-0.8% of sodium dihydrogen phosphate, 0.2-1.2% of disodium hydrogen phosphate, and the balance being distilled water. The volatile oil inclusion compound is an inclusion compound of a carboxymethyl-β-cyclodextrin / chitosan / Fe3O4 nanocomposite and a mixed volatile oil of perilla and patches.

[0010] Specifically, the method for extracting the honeysuckle flower extract includes:

[0011] (1) Wash the honeysuckle flowers, dry them thoroughly, and crush them. After crushing, ultrasonically extract them with 50% ethanol at a material-liquid ratio of 1:15 (g:mL) for 1 h at an ultrasonic power of 250 W and an ultrasonic temperature of 40°C. After the ultrasonication, filter and collect the filtrate.

[0012] (2) The medicinal residue from the above step was added with 70% ethanol at a material-liquid ratio of 1:15 (g:mL), and refluxed at 70°C for 2 h. The two filtrates were combined;

[0013] (3) Adsorption with macroporous resin and elution of the target component with 50% ethanol;

[0014] (4) Concentrate under reduced pressure until there is no alcohol smell, and spray dry to obtain a light yellow powder.

[0015] The extraction method of the mixed volatile oil extract of Perilla frutescens and Patchouli includes washing Perilla frutescens and Patchouli thoroughly, drying, crushing, and mixing them, and then extracting them by steam distillation. The mass ratio of Perilla frutescens to Patchouli is 1:1, and the material-liquid ratio is 1:9 (g / mL). First, soak for 30 minutes, then extract for 3 hours, and collect the volatile oil.

[0016] Preferably, the total amount of the honeysuckle flower extract and the volatile oil inclusion complex is not less than 10 wt % of the total amount of raw materials.

[0017] Preferably, the surfactant comprises vitamin E polyethylene glycol succinate and the preservative comprises potassium sorbate.

[0018] The present invention also discloses a method for preparing a traditional Chinese medicine composite mouthwash for resisting dental plaque, comprising the following steps:

[0019] A1. The carboxymethyl-β-cyclodextrin / chitosan / Fe3O4 nanocomposite was added to distilled water and sonicated to dissolve. An ethanol solution of a mixed volatile oil of Perilla and Patchouli was added and sonicated. The mixture was then magnetically separated using a magnet. The separated product was repeatedly washed with ethanol and distilled water and dried to obtain a volatile oil inclusion complex.

[0020] A2. Add honeysuckle flower extract, volatile oil inclusion complex, hydrogen peroxide, xylitol, surfactant, preservative, disodium hydrogen phosphate, and sodium dihydrogen phosphate to distilled water, stir to dissolve, and allow to stand to defoam to produce a traditional Chinese medicine compound mouthwash.

[0021] Preferably, in step A1, the ratio of carboxymethyl-β-cyclodextrin / chitosan / Fe3O4 nanocomposite to the mixed volatile oil of Perilla frutescens and Patchouli is 25:1 (g:mL); in step A2, the pH value of the obtained traditional Chinese medicine composite mouthwash is 6.5-7.5.

[0022] Preferably, the preparation of the carboxymethyl-β-cyclodextrin / chitosan / Fe3O4 nanocomposite in step A1 comprises the following steps:

[0023] S1. Preparation of chitosan / Fe3O4 nanocomposite particles: chitosan was dissolved in an acetic acid solution to obtain solution A; Fe3O4 nanoparticles were weighed and dissolved in a citric acid solution and ultrasonically dispersed to obtain solution B; solution B was added to solution A under stirring and ultrasonically dispersed; glutaraldehyde solution was added to adjust the pH of the system to 9, the reaction was heated and stirred, and then magnetic separation was performed using a magnet. The separated product was repeatedly washed with ethanol and distilled water and dried to obtain chitosan / Fe3O4 nanocomposite particles;

[0024] S2. Dissolve carboxymethyl-β-cyclodextrin powder in phosphate buffer solution, add EDC (1-ethyl-(3-dimethylaminopropyl)carbodiimide hydrochloride) and NHS (N-hydroxysuccinimide), and react at room temperature in the dark to obtain solution C.

[0025] S3. The chitosan / Fe3O4 nanocomposite particles obtained in step S1 are dissolved in an acetic acid solution to obtain a solution D. Solution D is mixed with solution C obtained in step S2, dispersed ultrasonically, and stirred for reaction at room temperature. The mixture is then magnetically separated, and the separated product is washed with a phosphate buffer solution and dried to obtain a carboxymethyl-β-cyclodextrin / chitosan / Fe3O4 nanocomposite.

[0026] Preferably, in step S1, the molecular weight of chitosan is 30 to 40 kDa, the degree of deacetylation is not less than 90%, the particle size of Fe3O4 nanoparticles is 15 to 25 nm, and the mass ratio of chitosan:Fe3O4 nanoparticles is 1:(0.12 to 0.2); in step S2, the molar ratio of EDC:NHS:carboxymethyl-β-cyclodextrin is 1:1:(0.1 to 0.2); in step S3, the mass ratio of carboxymethyl-β-cyclodextrin in solution C:chitosan / Fe3O4 nanocomposite particles in solution D is 1:(0.6 to 1), and the degree of substitution of carboxymethyl-β-cyclodextrin in the carboxymethyl-β-cyclodextrin / chitosan / Fe3O4 nanocomposite is 4 to 8%.

[0027] The beneficial effects of the above technical solution of the present invention are as follows:

[0028] The present invention uses traditional Chinese medicine as the main bactericidal agent. The chlorogenic acid in the honeysuckle extract exerts antibacterial and anti-inflammatory effects through multiple mechanisms such as inhibiting bacterial growth, scavenging free radicals, and regulating inflammatory factors, and has broad-spectrum antibacterial activity. The luteolin in the honeysuckle extract has strong anti-biofilm activity. In the biofilm, luteolin reduces the expression of pathogenic genes of Streptococcus mutans, such as genes encoding surface adhesins and EPS production enzymes, thereby significantly reducing the number of bacteria and EPS. In addition, luteolin also reduces the production of water-insoluble glucans in the biofilm, disrupting the formation of the biofilm. The volatile oils in perilla and patchouli can interfere with the aggregation behavior of bacteria, reduce the quorum sensing effect, slow down their replication rate, and thus inhibit the formation of bacterial biofilms. At the same time, the volatile oils have antioxidant and anti-inflammatory properties, which can reduce stomatitis and remove endotoxins in bacteria. Replacing chemical antibacterial agents with traditional Chinese medicine ingredients avoids the side effects of chemical antibacterial agents, such as oral flora imbalance, increased drug resistance, or irritation to the oral mucosa, and is more in line with the development trends of "green health" and "prevention first". In addition, the present invention avoids the use of alcohol, reduces oral irritation, and can be used for a long time.

[0029] The present invention prepares a carboxymethyl-β-cyclodextrin / chitosan / Fe3O4 nanocomposite, which has the following effects:

[0030] (1) The solubilizing effect of carboxymethyl-β-cyclodextrin was used to increase the solubility of volatile oils from Perilla frutescens and Patchouli in mouthwash, thereby enhancing their efficacy.

[0031] (2) Chitosan has pH response function. After food ferments in the mouth, a slightly acidic environment is formed, which promotes the dissolution of chitosan and releases Fe3O4 nanoparticles. Fe3O4 nanoparticles have peroxidase-like properties and can catalyze low-dose hydrogen peroxide in mouthwash to generate a large number of hydroxyl radicals. Hydroxyl radicals can destroy the extracellular polysaccharides (EPS) in bacterial biofilms, which are the structural basis of biofilms. By degrading EPS, hydroxyl radicals weaken the physical barrier of the biofilm, exposing bacteria to the external environment, making them easier to remove. They work synergistically with the bactericidal ingredients of traditional Chinese medicine to further improve the bactericidal effect and effectively inhibit the formation of dental plaque.

[0032] (3) After chitosan is coupled with carboxymethyl-β-cyclodextrin, the solubility of chitosan in water is improved. After chitosan is coated with Fe3O4 nanoparticles, the dispersion stability of Fe3O4 nanoparticles in aqueous solution is improved. At the same time, the polycationic properties of chitosan can adhere to the negatively charged bacterial biofilm, thereby improving the targeting effect of volatile oil and Fe3O4 nanoparticles, prolonging their action time, and providing more efficient and long-lasting protection. DETAILED DESCRIPTION

[0033] The preferred embodiments of the present invention are described below. It should be understood that the preferred embodiments described herein are only used to illustrate and explain the present invention, and are not used to limit the present invention.

[0034] If specific experimental procedures or conditions are not specified in this protocol, the procedures or conditions described in the literature in this field can be followed. Reagents or instruments used without manufacturer's information are commercially available.

[0035] Example

[0036] The invention discloses an anti-dental plaque Chinese medicine composite mouthwash, which comprises the following raw material components, measured by weight percentage: 6-10% of honeysuckle flower extract, 1-5% of volatile oil inclusion compound, 0.03-0.06% of hydrogen peroxide, 1-5% of xylitol, 0.5-1% of surfactant, 0.1-0.3% of preservative, 0.1-0.8% of sodium dihydrogen phosphate, 0.2-1.2% of disodium hydrogen phosphate, and the balance is distilled water.

[0037] The volatile oil inclusion compound is an inclusion compound of carboxymethyl-β-cyclodextrin / chitosan / Fe3O4 nanocomposite and mixed volatile oils of Perilla frutescens and Patchouli, the surfactant includes vitamin E polyethylene glycol succinate, the preservative includes potassium sorbate, and the total amount of honeysuckle extract and volatile oil inclusion compound is not less than 10wt% of the total amount of raw materials.

[0038] A method for preparing an anti-plaque Chinese medicine compound mouthwash comprises the following steps:

[0039] A1. The carboxymethyl-β-cyclodextrin / chitosan / Fe3O4 nanocomposite was added to distilled water and ultrasonically dissolved. An ethanol solution of a mixed volatile oil of Perilla and Patchouli was added and ultrasonically included. The ratio of the carboxymethyl-β-cyclodextrin / chitosan / Fe3O4 nanocomposite to the mixed volatile oil of Perilla and Patchouli was 25:1 (g:mL); magnetic separation was then performed using a magnet, and the isolate was repeatedly washed with ethanol and distilled water and dried to obtain a volatile oil inclusion complex.

[0040] A2. Add honeysuckle flower extract, volatile oil inclusion complex, hydrogen peroxide, xylitol, surfactant, preservative, disodium hydrogen phosphate, and sodium dihydrogen phosphate to distilled water, stir to dissolve, and allow to stand to defoam. This produces a traditional Chinese medicine compound mouthwash with a pH of 6.5 to 7.5.

[0041] Specifically, the preparation of carboxymethyl-β-cyclodextrin / chitosan / Fe3O4 nanocomposite includes the following steps:

[0042] S1. Preparation of chitosan / Fe3O4 nanocomposite particles: 2 g of chitosan (molecular weight 30-40 kDa, degree of deacetylation not less than 90%) was dissolved in 100 mL of 2% acetic acid solution to obtain solution A; 0.24 g to 0.4 g of Fe3O4 nanoparticles (particle size 15-25 nm) were weighed and dissolved in 100 mL of 20 mg / mL citric acid solution and ultrasonically dispersed to obtain solution B; solution B was added to solution A under stirring and ultrasonically dispersed; 20 mL of 5% glutaraldehyde solution was added, the pH value of the system was adjusted to 9 with sodium hydroxide, and the reaction was stirred at 60°C for 2 h, followed by magnetic separation using a magnet. The separated material was repeatedly washed with ethanol and distilled water and dried to obtain chitosan / Fe3O4 nanocomposite particles;

[0043] S2. Dissolve 0.77 g to 1.54 g of carboxymethyl-β-cyclodextrin powder in 50 mL of 0.01 mol / L pH 7.4 phosphate buffer solution. Add 0.95 g of EDC and 0.57 g of NHS. Incubate at room temperature in the dark for 1 h to obtain Solution C.

[0044] S3. Dissolve 0.7 g to 1.54 g of the chitosan / Fe3O4 nanocomposite particles from step S1 in 50 mL of 2% acetic acid solution to obtain solution D. Mix solution D with solution C from step S2, disperse ultrasonically, and react with stirring at room temperature for 24 h. Then, separate magnetically, wash the separated material with 0.01 mol / L pH 7.4 phosphate buffer solution, and dry it to obtain a carboxymethyl-β-cyclodextrin / chitosan / Fe3O4 nanocomposite, wherein the degree of substitution of the carboxymethyl-β-cyclodextrin is 4 to 8%.

[0045] Example 1

[0046] The preparation method of the anti-plaque Chinese medicine composite mouthwash of the above embodiment is adopted, wherein, in terms of weight percentage, it comprises the following components:

[0047] Honeysuckle extract 10%, volatile oil inclusion compound 5%, hydrogen peroxide 0.03%, xylitol 2%, vitamin E polyethylene glycol succinate 1%, potassium sorbate 0.3%, sodium dihydrogen phosphate 0.1%, disodium hydrogen phosphate 0.6%, and the balance is distilled water.

[0048] Example 2

[0049] The preparation method of the anti-plaque Chinese medicine composite mouthwash of the above embodiment is adopted, wherein the following components are included in weight percentage:

[0050] Honeysuckle flower extract 10%, volatile oil inclusion compound 1%, hydrogen peroxide 0.06%, xylitol 5%, vitamin E polyethylene glycol succinate 0.5%, potassium sorbate 0.2%, sodium dihydrogen phosphate 0.2%, disodium hydrogen phosphate 1.2%, and the balance is distilled water.

[0051] Example 3

[0052] The preparation method of the anti-plaque Chinese medicine composite mouthwash of the above embodiment is adopted, wherein the following components are included in weight percentage:

[0053] Honeysuckle flower extract 6%, volatile oil inclusion compound 5%, hydrogen peroxide 0.05%, xylitol 3%, vitamin E polyethylene glycol succinate 1%, potassium sorbate 0.1%, sodium dihydrogen phosphate 0.4%, disodium hydrogen phosphate 0.2%, and the balance is distilled water.

[0054] Example 4

[0055] The preparation method of the anti-plaque Chinese medicine composite mouthwash of the above embodiment is adopted, wherein, in terms of weight percentage, it comprises the following components:

[0056] Honeysuckle flower extract 8%, volatile oil inclusion compound 3%, hydrogen peroxide 0.04%, xylitol 1%, vitamin E polyethylene glycol succinate 0.8%, potassium sorbate 0.2%, sodium dihydrogen phosphate 0.8%, disodium hydrogen phosphate 0.4%, and the balance is distilled water.

[0057] Comparative Example 1

[0058] The difference from Example 1 is that the honeysuckle flower extract is not added.

[0059] Comparative Example 2

[0060] The difference from Example 1 is that no hydrogen peroxide was added.

[0061] Comparative Example 3

[0062] The difference between this embodiment and Example 1 is that no volatile oil inclusion compound is added.

[0063] Comparative Example 4

[0064] The difference from Example 1 is that volatile oil included in the mixture by carboxymethyl-β-cyclodextrin is added, and the inclusion ratio is 8:1 (g:mL).

[0065] Comparative Example 5

[0066] The difference from Example 1 is that volatile oil that has not been encapsulated by the carboxymethyl-β-cyclodextrin / chitosan / Fe3O4 nanocomposite is added, and the amount of hydrogen peroxide added is 1.5%.

[0067] Comparative Example 6

[0068] Chlorhexidine mouthwash, in percentage by weight, comprises the following components:

[0069] Chlorhexidine 0.12%, metronidazole 0.05%, xylitol 2%, vitamin E polyethylene glycol succinate 1%, potassium sorbate 0.3%, sodium dihydrogen phosphate 0.1%, disodium hydrogen phosphate 0.6%, and the balance is distilled water.

[0070] MTT (thiazolyl blue) method was used to detect the viability of dental plaque biofilm cells in vitro:

[0071] Experiment 1: In vitro inhibition of early dental plaque biofilm cell activity by mouthwash

[0072] (1) Dental plaque collected from the teeth of participants who had not used antibiotics within three months was diluted with sterile saline at a ratio of 1:50 and inoculated into a culture medium. Subsequently, 2 mL of saline (control group) and 2 mL of the mouthwash of Examples 1 to 4 and Comparative Examples 1 to 6 (test group) were added to 100 mL of the culture medium. The culture medium of the control group and the test group was added to a 24-well plate, with three parallel wells in each group, and the plates were incubated at 37°C and 5% CO2 for 48 h to form a biofilm.

[0073] (2) The culture medium with the biofilm was transferred to a new 24-well plate, and then 1 mL of MTT dye (0.5 mg / mL MTT in PBS) was added to each well. After incubation at 37°C and 5% CO2 for 1 h, the culture medium was transferred to a new 24-well plate, 1 mL of DMSO (dimethyl sulfoxide) was added to dissolve the crystals, and the plate was incubated at room temperature in the dark for 20 min. 200 μL of the solution from each well was transferred to a 96-well plate, and the absorbance (A) value at 540 nm was measured using a microplate reader. Deionized water was used as the blank group, and the cell survival rate was calculated [(A value of the experimental group - A value of the blank group) / (A value of the control group - A value of the blank group) × 100%].

[0074] Table 1 Results of in vitro inhibition test of early dental plaque biofilm cell activity by mouthwash

[0075] Group Cell survival rate / % control group 100 Example 1 8.3 Example 2 10.7 Example 3 13.1 Example 4 12.6 Comparative Example 1 38.4 Comparative Example 2 32.2 Comparative Example 3 35.8 Comparative Example 4 30.5 Comparative Example 5 25.6 Comparative Example 6 15.9

[0076] Note: The cell survival rate of the control group was taken as 100%.

[0077] Experiment 2: In vitro inhibition of mature dental plaque biofilm cell activity by mouthwash

[0078] The difference from step (1) of the first experiment is that the dental plaque collected from the teeth of participants who had not used antibiotics within three months was diluted with sterile saline at a ratio of 1:50 and inoculated into the culture medium, and incubated at 37°C and 5% CO2 for 48 hours to form a biofilm; 2 mL of saline (control group) and 2 mL of the mouthwash of Examples 1 to 4 and Comparative Examples 1 to 6 (test group) were added to 100 mL of culture medium; the culture medium of the control group and the test group were added to a 24-well plate, with three parallel wells in each group, and incubated at 37°C and 5% CO2 for 48 hours.

[0079] Step (2) is the same as in Experiment 1.

[0080] Table 2 Results of in vitro test on the inhibition of mature dental plaque biofilm cell activity by mouthwash

[0081]

[0082]

[0083] Note: The cell survival rate of the control group was taken as 100%.

[0084] The MTT assay is based on the reduction of MTT to insoluble blue-purple formazan crystals by succinate dehydrogenase in the mitochondria of living cells, while dead cells are unable to undergo this reaction. By dissolving the formazan in DMSO (dimethyl sulfoxide) and measuring its absorbance at a specific wavelength, the number of living cells can be indirectly reflected, thereby evaluating the inhibitory effect on biofilms.

[0085] Dental plaque index test:

[0086] 110 volunteers aged 18-35 were divided into 11 groups of 10 each. They underwent full mouth cleaning (to remove tartar and plaque) and rinsed with 20 mL of the mouthwashes of Examples 1-4 and Comparative Examples 1-6 for 3 minutes every morning and evening after brushing. The control group used tap water for the test, which lasted for 1 month. Each volunteer was given a soft-bristled toothbrush and non-antibacterial toothpaste, and was advised to avoid flossing or interdental brushes during the cleaning period.

[0087] One month later, stain the plaque using a plaque stain. Place 1 mL of stain in a disposable cup and evenly apply to all tooth surfaces with a cotton swab. Examine the buccal, labial, and lingual surfaces of six designated teeth. The average score for all six surfaces is used as the individual plaque index. Record the test results according to the following criteria.

[0088] Table 3 Dental plaque scoring criteria

[0089]

[0090]

[0091] Table 4 Dental plaque index test results

[0092] Group Plaque index control group 4.1 Example 1 0.4 Example 2 0.6 Example 3 1.0 Example 4 0.9 Comparative Example 1 3.1 Comparative Example 2 2.3 Comparative Example 3 2.5 Comparative Example 4 2.2 Comparative Example 5 1.9 Comparative Example 6 1.8

[0093] By comparing the test data of Examples 1 to 4 and Comparative Examples 1 to 6 in Table 1, it can be seen that in the early stage of dental plaque biofilm formation, the cell survival rates of Examples 1 to 4 and Comparative Example 6 are relatively low, indicating that they have a good inhibitory effect on the early stage dental plaque biofilm; the cell survival rates of Comparative Examples 1 to 5 are slightly higher, indicating that the inhibitory effect on the early stage dental plaque biofilm is slightly weaker.

[0094] By comparing the test data of Examples 1 to 4 and Comparative Examples 1 to 6 in Table 2, it can be seen that after the dental plaque biofilm matures, the cell survival rate of Examples 1 to 4 is low, indicating that they have a good inhibitory effect on mature dental plaque biofilm, and the antibacterial cell survival rate of Comparative Examples 1 to 6 is high, indicating that after the dental plaque film matures, the antibacterial effect of Comparative Examples 1 to 6 is significantly weakened.

[0095] By comparing the test data of Examples 1 to 4 and Comparative Examples 1 to 6 in Table 4, it can be seen that Examples 1 to 4 have better effects on inhibiting dental plaque.

[0096] Combining Tables 1, 2 and 4, it can be seen that destroying the EPS in the dental plaque biofilm is very important for the antibacterial effect of antibacterial agents. Simple Chinese herbal antibacterial ingredients or chemical antibacterial ingredients cannot effectively destroy the EPS in the dental plaque biofilm, resulting in the antibacterial ingredients being unable to contact the bacteria in the biofilm, which in turn leads to poor antibacterial effect; and the hydroxyl free radicals produced by hydrogen peroxide catalytic oxidation play a key role in destroying EPS. Therefore, the synergistic effect of hydrogen peroxide and Chinese herbal antibacterial ingredients can significantly enhance the antibacterial effect of mouthwash.

[0097] The carboxymethyl-β-cyclodextrin / chitosan / Fe3O4 nanocomposite prepared by the present invention can not only improve the solubility of volatile oil, but also provide a catalyst for catalyzing the oxidation of hydrogen peroxide to hydroxyl radicals, thereby reducing the added concentration of hydrogen peroxide and reducing oral irritation. The addition of chitosan can also increase the adhesion of volatile oil and Fe3O4 nanoparticles on dental plaque biofilms, release volatile oils in a targeted manner, cooperate with hydroxyl radicals to destroy dental plaque biofilms, clear the bacterial protective barrier for antibacterial ingredients, and at the same time prevent the effective ingredients from being washed away too quickly by saliva, prolong the action time, and produce a significant inhibitory effect on dental plaque biofilms.

[0098] Finally, it should be noted that the above embodiments are only used to illustrate the technical solution of the present invention and are not limiting. Other modifications or equivalent substitutions made to the technical solution of the present invention by ordinary technicians in this field should be included in the scope of the claims of the present invention as long as they do not depart from the spirit and scope of the technical solution of the present invention.

Claims

1. A traditional Chinese medicine compound mouthwash for resisting dental plaque, characterized in that: The invention comprises the following raw material components in weight percentage: 6-10% of honeysuckle flower extract, 1-5% of volatile oil inclusion compound, 0.03-0.06% of hydrogen peroxide, 1-5% of xylitol, 0.5-1% of surfactant, 0.1-0.3% of preservative, 0.1-0.8% of sodium dihydrogen phosphate, 0.2-1.2% of disodium hydrogen phosphate, and the balance is distilled water. The volatile oil inclusion compound is an inclusion compound of carboxymethyl-β-cyclodextrin / chitosan / Fe3O4 nanocomposite and mixed volatile oils of perilla and patches.

2. The anti-plaque Chinese medicine compound mouthwash according to claim 1, characterized in that: The total amount of the honeysuckle flower extract and the volatile oil inclusion compound is not less than 10wt% of the total amount of the raw materials.

3. The anti-plaque Chinese medicine compound mouthwash according to claim 1, characterized in that: Surfactants include vitamin E polyethylene glycol succinate.

4. The anti-plaque Chinese medicine compound mouthwash according to claim 1, characterized in that: Preservatives include potassium sorbate.

5. A method for preparing an anti-plaque Chinese medicine compound mouthwash, comprising: The following steps are involved: A1. The carboxymethyl-β-cyclodextrin / chitosan / Fe3O4 nanocomposite was added to distilled water and sonicated to dissolve. An ethanol solution of a mixed volatile oil of Perilla and Patchouli was added and sonicated. The mixture was then magnetically separated using a magnet. The separated product was repeatedly washed with ethanol and distilled water and dried to obtain a volatile oil inclusion complex. A2. Add honeysuckle flower extract, volatile oil inclusion complex, hydrogen peroxide, xylitol, surfactant, preservative, disodium hydrogen phosphate, and sodium dihydrogen phosphate to distilled water, stir to dissolve, and allow to stand to defoam to produce a traditional Chinese medicine compound mouthwash.

6. The method for preparing the Chinese medicinal compound mouthwash according to claim 5, wherein: In step A1, the ratio of carboxymethyl-β-cyclodextrin / chitosan / Fe3O4 nanocomposite to the mixed volatile oil of Perilla frutescens and Patchouli is 25:1 (g:mL); in step A2, the pH value of the obtained traditional Chinese medicine composite mouthwash is 6.5-7.

5.

7. The method for preparing the Chinese medicinal compound mouthwash according to claim 5, wherein: The preparation of the carboxymethyl-β-cyclodextrin / chitosan / Fe3O4 nanocomposite in step A1 comprises the following steps: S1. Preparation of chitosan / Fe3O4 nanocomposite particles: chitosan was dissolved in an acetic acid solution to obtain solution A; Fe3O4 nanoparticles were weighed and dissolved in a citric acid solution and ultrasonically dispersed to obtain solution B; solution B was added to solution A under stirring and ultrasonically dispersed; glutaraldehyde solution was added to adjust the pH of the system to 9, the reaction was heated and stirred, and then magnetic separation was performed using a magnet. The separated product was repeatedly washed with ethanol and distilled water and dried to obtain chitosan / Fe3O4 nanocomposite particles; S2. Dissolve carboxymethyl-β-cyclodextrin powder in phosphate buffer solution, add EDC and NHS, and react at room temperature in the dark to obtain solution C; S3. The chitosan / Fe3O4 nanocomposite particles obtained in step S1 are dissolved in an acetic acid solution to obtain a solution D. Solution D is mixed with solution C obtained in step S2, dispersed ultrasonically, and stirred for reaction at room temperature. The mixture is then magnetically separated, and the separated product is washed with a phosphate buffer solution and dried to obtain a carboxymethyl-β-cyclodextrin / chitosan / Fe3O4 nanocomposite.

8. The method for preparing the Chinese medicinal compound mouthwash according to claim 7, wherein: In step S1, the molecular weight of chitosan is 30-40 kDa, the degree of deacetylation is not less than 90%, the particle size of Fe3O4 nanoparticles is 15-25 nm, and the mass ratio of chitosan to Fe3O4 nanoparticles is 1:(0.12-0.2).

9. The method for preparing the Chinese medicinal compound mouthwash according to claim 7, wherein: In step S2, the molar ratio of EDC:NHS:carboxymethyl-β-cyclodextrin is 1:1:(0.1-0.2).

10. The method for preparing the Chinese medicinal compound mouthwash according to claim 7, wherein: In step S3, the mass ratio of carboxymethyl-β-cyclodextrin in solution C to chitosan / Fe3O4 nanocomposite particles in solution D is 1:(0.6-1), and the degree of substitution of carboxymethyl-β-cyclodextrin in the carboxymethyl-β-cyclodextrin / chitosan / Fe3O4 nanocomposite is 4-8%.

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