Antibacterial oral care toothpaste based on active ingredients of melia azedarach

Abstract

The present application relates to toothpaste technical field, specifically, it relates to the bacteriostatic oral care toothpaste based on active ingredient of mountain ardisia. It includes sorbitol, hydrated silicon stone, deionized water, polyethylene glycol-8, sodium lauryl sulfate, essence, polyquaternium-22, cellulose glue, sodium saccharin, hydroxypropyl guar gum, sodium methyl hydroxybenzoate and mountain ardisia extract;The bacteriostatic oral care toothpaste based on active ingredient of mountain ardisia, by introducing the mountain ardisia extract with specific chemical composition into the formula system, effectively solve the problem that the existing oral care product is not strong in specificity to periodontal pathogenic bacteria, and the bacteriostatic spectrum is relatively single;The mutual synergistic effect relationship exists between the extract, not only broaden the inhibition spectrum of periodontal pathogenic microorganism, also can reduce the oxidative stress and inflammatory response of gingival tissue, thereby maintaining oral cleaning, improve the comprehensive performance of oral care product and the mildness of use.

Description

Technical Field

[0001] This invention relates to the field of toothpaste technology, and more specifically, to an antibacterial oral care toothpaste based on the active ingredient of *Syzygium aromaticum*. Background Technology

[0002] Currently, chemical antibacterial ingredients are commonly used in the field of oral care to inhibit pathogens associated with gingivitis and periodontitis. These toothpastes often rely on synthetic additives or single-function ingredients. Although they have a certain antibacterial effect, they often cause an imbalance in the oral flora with long-term use and may also be accompanied by risks of irritation and drug resistance, affecting oral microecological health. In existing technologies, antibacterial agents or crude plant extracts are commonly used to enhance the antibacterial properties of toothpaste. However, their targeted antibacterial effects against specific pathogens of gingivitis and periodontitis, such as Prevotella intermedius and Fusobacterium nucleatum, are still insufficient. Furthermore, crude plant extracts often use common herbal ingredients such as Scutellaria baicalensis and Lonicera japonica, and their active ingredient composition is relatively simple. This not only reduces their specific inhibitory effect on periodontal pathogens, resulting in a narrow antibacterial spectrum, but also weakens the synergistic effect of plant ingredients in antioxidation and gum soothing. As a result, the overall care efficacy and safety of antibacterial oral care toothpaste are reduced.

[0003] Therefore, there is an urgent need for antibacterial oral care toothpaste based on the active ingredient of *Syzygium aromaticum*. Summary of the Invention

[0004] The purpose of this invention is to provide an antibacterial oral care toothpaste based on the active ingredient of *Syzygium aromaticum*, in order to solve the problems mentioned in the background art.

[0005] To achieve the above objectives, the present invention provides an antibacterial oral care toothpaste based on the active ingredient of *Syzygium aromaticum*, comprising the following raw materials: 15-25 wt% sorbitol, 15-25 wt% hydrated silica, 15-25 wt% deionized water, 1-5 wt% polyethylene glycol-8, 1-3 wt% sodium lauryl sulfate, 0.5-1.5 wt% fragrance, 0.1-1 wt% polyquaternium-22, 0.5-1.5 wt% cellulose gum, 0.1-0.5 wt% sodium saccharin, 0.1-1 wt% hydroxypropyl guar gum, 0.05-0.15 wt% Sodium methylparaben and 0.1-0.5 wt% of *Syzygium aromaticum* extract; wherein: the sodium lauryl sulfate can produce a synergistic effect with polyquaternium-22 in the oral environment to enhance the physical removal effect on dental plaque; the *Syzygium aromaticum* extract interacts with polyquaternium-22 and cellulose gum to form a composite carrier system that helps the active ingredients to be adsorbed and released slowly on the tooth and gingival surfaces, thereby synergistically enhancing the specific inhibitory efficacy against periodontal pathogens *Prevotella intermedius* and *Fusobacterium nucleatum*.

[0006] Furthermore, the *Syzygium aromaticum* extract includes the following extraction steps: S1.1 Material crushing and soaking: Take dried leaves of *Ligustrum lucidum* and crush them until they pass through a No. 3 sieve to obtain uniform powder raw material. Then, put the powder and 2.8-3.2 times its volume of 90% ethanol solution into a sealed extraction container and stir continuously at 30-50 r / min for 20-30 min at room temperature. This is beneficial to the full dispersion of raw material particles and also helps the ethanol solution to penetrate into the powder, causing the plant cell walls to swell gently and form a uniform suspension. S1.2, Staged Ultrasonic Extraction and Combination: The suspension is placed in an ultrasonic extraction device for three extractions to obtain three extracts, A, B and C. Then, these three extracts are mixed and combined according to their ethanol concentration. Based on the differences in component polarity, various functional substances in the extract can be initially enriched and integrated, thus obtaining a mixed extract with more comprehensive components and more concentrated activity. S1.3 Concentration and Extraction: The mixed extract is transferred to a rotary evaporator and concentrated under reduced pressure at a water bath temperature of 40-50℃ and a pressure below 0.09MPa until the solution volume is reduced to 5-10% of the original volume and no ethanol odor is emitted. This process gently and thoroughly removes 90% of the ethanol solvent from the mixture, while effectively avoiding the damage of heat-sensitive active ingredients to high temperatures. The final product is a brownish-brown, uniform, thick paste-like extract of *Syzygium aromaticum*.

[0007] Furthermore, in step S1.2, the ultrasonic extraction device extraction includes the following steps: First, set the ultrasonic extraction device to a constant temperature of 25-28℃ and an ultrasonic power of 280-320W to perform the first extraction on the suspension for 18-22 minutes. After extraction, perform solid-liquid separation using medium-speed filter paper and collect the first clear extract, which is labeled as part A. Add the same volume and concentration of 90% ethanol solution as the first extraction to the separated solid residue. Under the same temperature and ultrasonic power conditions, repeat the second and third extractions. Each extraction time is 18-22 min. Collect the clear extracts by filtration and label them as part B and part C, respectively.

[0008] Furthermore, in S1.3, the *Syzygium aromaticum* extract includes at least privetin, rhubarb glycoside, ursolic acid, total polyphenols, and total flavonoids.

[0009] Furthermore, the content of privetin is 4.9-5.4%; the content of rhubarb glycoside is 0.9-1.1%; the content of ursolic acid is 0.4-0.5%; the content of total polyphenols is 14.5-15.8%; and the content of total flavonoids is 7.9-8.5%.

[0010] Firstly, through fractional ultrasonic extraction and gradient enrichment with ethanol, multiple active ingredients such as privetin, rhubarb glycoside, ursolic acid, total polyphenols, and total flavonoids can be efficiently obtained, forming a synergistic antibacterial network in the toothpaste system. Simultaneously, this extract, along with polyquaternium-22 and cellulose gum, constructs a composite carrier with adhesive sustained-release properties in the oral cavity through electrostatic adsorption and colloidal complexation, enhancing the targeted retention time on the tooth surface and gingival sulcus, thereby strengthening the specific inhibition of Prevotella intermedius and Fusobacterium nucleatum. Furthermore, through the synergistic antioxidant and anti-inflammatory mechanisms of polyphenols and flavonoids, it reduces gingival tissue inflammation while scavenging free radicals. In addition, this extract, along with polyquaternium-22 and cellulose gum in the formula, forms a sustained-release composite system through intermolecular interactions. This system enhances the adsorption and retention of active ingredients on the tooth and gingival surfaces, thus prolonging the specific antibacterial effect against periodontal pathogens. Combined with the physical cleaning efficacy of sodium lauryl sulfate, it comprehensively improves oral care.

[0011] Furthermore, the toothpaste is prepared using a pre-assembly-step integration process, which includes the following steps: S2.1 Construction of functional composite carrier system: A portion of polyquaternium-22, hydroxypropyl guar gum, cellulose gum, and a portion of deionized water were added to a closed mixing tank with stirring and temperature control functions. Under medium-speed stirring at 25-35℃ and 200-400r / min, a clear and viscous cationic polymer mixed solution was formed. Then, the stirring speed was reduced to 50-100r / min, and the extract of *Syzygium aromaticum* was added dropwise under light-protected conditions. The active substances in the extract spontaneously embedded themselves into the three-dimensional network structure formed by the polymer molecular chains through electrostatic attraction, hydrogen bonding, and hydrophobic interaction, forming an encapsulated composite gel. S2.2 Preparation of stabilized paste base: Sorbitol, hydrated silica, polyethylene glycol-8 and the remaining deionized water are added to a vacuum paste-making machine and subjected to high-speed shearing at 40-45℃ and 600-800r / min for 20-30min to fully wet, disperse and homogenize the powder and liquid, forming a dense and smooth base paste. S2.3 Step-by-step integration and functional coupling: The composite gel is transferred to the base paste and mixed continuously for 15-25 minutes at a medium speed of 300-400 r / min at 40-45℃ to fully integrate the gel network with the paste matrix. Then, sodium lauryl sulfate and the remaining polyquaternium-22 are added and stirred for another 10-15 minutes at the same temperature and speed to further stabilize the system through ionic interaction. Finally, the fragrance, sodium saccharin and sodium methylparaben are added, the stirring is switched to low speed and a vacuum is turned on, and the mixture is homogenized and degassed at 100-150 r / min for 5-10 minutes to obtain the final product paste.

[0012] Furthermore, in step S2.1, the amount of polyquaternium-22 used accounts for 30%-50% of the total amount of polyquaternium-22 used, and the amount of deionized water used accounts for 30%-40% of the total amount of deionized water used.

[0013] Furthermore, the toothpaste is used to inhibit pathogenic microorganisms related to gingivitis and periodontitis, and in daily oral hygiene.

[0014] Compared with the prior art, the beneficial effects of the present invention are as follows: 1. This antibacterial oral care toothpaste based on the active ingredient of *Syzygium aromaticum* effectively solves the problems of existing oral care products having weak targeting of periodontal pathogens and relatively limited antibacterial spectrum by introducing *Syzygium aromaticum* extract with specific chemical composition into the formulation system. The extract is rich in privetin, rhubarb glycoside, ursolic acid, as well as total polyphenols and total flavonoids and other active substances. These components have a synergistic effect, which not only broadens the inhibition spectrum against periodontal pathogens, but also reduces oxidative stress and inflammatory response of gingival tissue. Thus, while maintaining oral hygiene, it improves the overall efficacy and gentleness of oral care products.

[0015] 2. This antibacterial oral care toothpaste based on the active ingredient of *Syzygium aromaticum* solves the problems of easy loss and short duration of action of active ingredients in the oral environment through a "pre-assembly-step integration" method. First, *Syzygium aromaticum* extract, along with some polyquaternium-22 and colloidal components, is pre-formed into a functional composite gel carrier, which effectively encapsulates the active substances. Then, in the step integration stage, the carrier is coupled with the paste base and cleaning components, ultimately constructing a three-dimensional network with adhesion and sustained-release properties in the toothpaste system. This not only prolongs the retention time of active ingredients on the tooth surface and gingival sulcus, but also creates a temporal synergy with the cleaning efficacy of sodium lauryl sulfate. It first adsorbs and inhibits pathogenic bacteria, and then removes them through physical friction, thereby achieving a long-lasting and coordinated effect of antibacterial, cleaning, and tissue care. Attached Figure Description

[0016] Figure 1This is a flowchart of the extraction steps of the *Syzygium serratum* extract according to the present invention; Figure 2 This is a flowchart of the pre-assembly-step integration process of the present invention. Figure 3 This is a colony distribution diagram of Prevotella intermedius in this invention; Figure 4 This is a colony distribution diagram of *Fusobacterium nucleatum* according to the present invention; Figure 5 This is a line graph showing the inhibition rate of dental plaque biofilm formation according to the present invention. Figure 6 Line graph showing the clearance efficiency of this invention against Porphyromonas gingivalis; Figure 7 This is a bar chart showing the 24-hour sustained release rate of the active ingredient (privetin) of this invention. Detailed Implementation

[0017] The technical solutions in the embodiments of the present invention will be clearly and completely described below with reference to the accompanying drawings. Obviously, the described embodiments are only some embodiments of the present invention, and not all embodiments. Based on the embodiments of the present invention, all other embodiments obtained by those skilled in the art without creative effort are within the scope of protection of the present invention. Example

[0018] The dried leaves of *Hedysarum heterotropoides* were pulverized and passed through a No. 3 sieve. Three times the volume of 90% ethanol was added for ultrasonic extraction at room temperature, repeated three times. The extracts were combined and concentrated under reduced pressure to obtain a *Hedysarum heterotropoides* extract containing 5.167% privetin, 0.993% arbutin, 0.454% ursolic acid, 15.15% total polyphenols, and 8.28% total flavonoids. The following components were weighed: 20 wt% sorbitol, 20 wt% hydrated silica, 20 wt% deionized water, 83 wt% polyethylene glycol, 1.5 wt% sodium lauryl sulfate, 1 wt% fragrance, 0.5 wt% polyquaternium-22, 1 wt% cellulose gum, 0.3 wt% sodium saccharin, 0.5 wt% hydroxypropyl guar gum, 0.1 wt% sodium methylparaben, and 0.25 wt% of the above *Hedysarum heterotropoides* extract.

[0019] First, 30% of polyquaternium-22, hydroxypropyl guar gum, and cellulose gum were mixed with 35% of deionized water at 30°C and 300 rpm to form a gel. Then, *Syzygium aromaticum* extract was added dropwise and a composite gel was prepared under light-protected conditions. Next, the remaining materials (excluding sodium lauryl sulfate, remaining polyquaternium-22, fragrance, sodium saccharin, and sodium methylparaben) were dispersed at 42°C and 700 rpm for 25 minutes in a vacuum toothpaste mixer to form a base paste. The composite gel was then added to the paste, and the mixture was stirred at 42°C and 350 rpm for 20 minutes. Sodium lauryl sulfate and remaining polyquaternium-22 were added, and the mixture was stirred for another 12 minutes. Finally, fragrance, sodium saccharin, and sodium methylparaben were added, and the mixture was vacuum degassed at 120 rpm for 8 minutes to obtain the toothpaste. Example

[0020] Dried leaves of *Hedysarum heterotropoides* were pulverized and passed through a No. 3 sieve. 2.8 times their volume of 90% ethanol were added for ultrasonic extraction at room temperature, repeated three times. The extracts were combined and concentrated under reduced pressure to obtain *Hedysarum heterotropoides* extract containing 4.9% ligustrazine, 1.1% arbutin, 0.4% ursolic acid, 15.8% total polyphenols, and 7.9% total flavonoids. The following components were weighed: 15 wt% sorbitol, 25 wt% hydrated silica, 15 wt% deionized water, 81 wt% polyethylene glycol, 3 wt% sodium lauryl sulfate, 0.5 wt% fragrance, 0.1 wt% polyquaternium-22, 1.5 wt% cellulose gum, 0.1 wt% sodium saccharin, 1 wt% hydroxypropyl guar gum, 0.05 wt% sodium methylparaben, and 0.5 wt% of the above *Hedysarum heterotropoides* extract.

[0021] First, add 30% of polyquaternium-22, all of hydroxypropyl guar gum, all of cellulose gum, and 30% of deionized water to a mixing tank and stir at 25°C and 200 rpm to form a gel. Then, under light protection and low-speed stirring at 50 rpm, add all of the *Ligusticum striatum* extract dropwise, continuing to stir until a homogeneous composite gel is formed. Next, add the remaining deionized water, sorbitol, hydrated silica, and polyethylene glycol-8 to a vacuum ointment machine, set the temperature to 40°C, and perform high-speed stirring at 600 rpm. Rapid shear dispersion for 30 minutes to form the base paste; then the composite gel is added to the base paste and mixed at 40℃ and 300r / min for 25 minutes to fully integrate the two. Then all sodium lauryl sulfate and the remaining 70% polyquaternium-22 are added and stirred for 15 minutes at the same temperature and speed. Finally, all the fragrance, sodium saccharin and sodium methylparaben are added, the stirring is switched to a low speed of 100r / min and the vacuum system is turned on. After degassing for 10 minutes, the final toothpaste product is obtained. Example

[0022] Dried leaves of *Hedysarum heterotropoides* were pulverized and passed through a No. 3 sieve. 3.2 times their volume of 90% ethanol were added, and the mixture was ultrasonically extracted at room temperature, repeated three times. The extracts were combined and concentrated under reduced pressure to obtain a *Hedysarum heterotropoides* extract containing 5.4% ligustrazine, 0.9% arbutin, 0.5% ursolic acid, 14.5% total polyphenols, and 8.5% total flavonoids. The following ingredients were weighed: 25 wt% sorbitol, 15 wt% hydrated silica, 25 wt% deionized water, 85 wt% polyethylene glycol, 1 wt% sodium lauryl sulfate, 1.5 wt% fragrance, 1 wt% polyquaternium-22, 0.5 wt% cellulose gum, 0.5 wt% sodium saccharin, 0.1 wt% hydroxypropyl guar gum, 0.15 wt% sodium methylparaben, and 0.1 wt% of the above *Hedysarum heterotropoides* extract.

[0023] First, add 50% of the amount of polyquaternium-22, all of the hydroxypropyl guar gum, all of the cellulose gum, and 40% of the amount of deionized water into a sealed mixing tank. Stir at 35°C and 400 rpm to form a homogeneous gel. Then, adjust the speed to 100 rpm and slowly add all of the *Syzygium aromaticum* extract under light-protected conditions, continuing to stir until an encapsulated composite gel is formed. Separately, place the remaining deionized water, sorbitol, hydrated silica, and polyethylene glycol-8 into a vacuum ointment-making machine, set the temperature to 45°C, and stir at 800 rpm. High-speed shear dispersion at a rotation speed of r / min for 20 min is used to form a smooth paste base. Then, the composite gel is transferred to the paste base and mixed at 45℃ and 400 r / min for 15 min to achieve system integration. Then, all sodium lauryl sulfate and the remaining 50% of polyquaternium-22 are added, and stirring is continued for 10 min under the same conditions. Finally, all the fragrance, sodium saccharin and sodium methylparaben are added, the stirring speed is reduced to 150 r / min and vacuum is turned on. After homogenization and degassing for 5 min, the finished toothpaste is obtained. Example

[0024] The dried leaves of *Hedysarum heterotropoides* were pulverized and passed through a No. 3 sieve. Three times the volume of 90% ethanol was added for ultrasonic extraction at room temperature, repeated three times. The extracts were combined and concentrated under reduced pressure to obtain a *Hedysarum heterotropoides* extract containing 5.0% privetin, 1.05% arbutin, 0.45% ursolic acid, 15.2% total polyphenols, and 8.0% total flavonoids. The following components were weighed: 18 wt% sorbitol, 22 wt% hydrated silica, 18 wt% deionized water, 84 wt% polyethylene glycol, 2 wt% sodium lauryl sulfate, 1.2 wt% fragrance, 0.8 wt% polyquaternium-22, 0.8 wt% cellulose gum, 0.4 wt% sodium saccharin, 0.8 wt% hydroxypropyl guar gum, 0.12 wt% sodium methylparaben, and 0.3 wt% of the above *Hedysarum heterotropoides* extract.

[0025] First, add 40% of polyquaternium-22, all of hydroxypropyl guar gum, all of cellulose gum, and 38% of deionized water to a mixing tank equipped with a stirrer. Stir at 32°C and 350 rpm to prepare a gel solution. Then, adjust the speed to 80 rpm and add all of the *Ligusticum striatum* extract dropwise at a uniform rate in a light-protected environment, stirring to form a stable functional composite gel. Simultaneously, mix the remaining deionized water with sorbitol, hydrated silica, and polyethylene glycol-8 in a vacuum ointment-making machine at a set temperature of 43°C. The mixture was sheared and dispersed at 750 rpm for 22 minutes to form a uniform base paste. Then, the composite gel was combined with the base paste and mixed at 43°C and 380 rpm for 18 minutes. All of the sodium lauryl sulfate and the remaining 60% of polyquaternium-22 were added and stirred continuously for 13 minutes. Finally, all of the fragrance, sodium saccharin and sodium methylparaben were added, and the mixture was stirred at a low speed of 130 rpm and vacuumed for 7 minutes to obtain the antibacterial oral care toothpaste.

[0026] Experimental Example 1 The purpose of this experimental group is to detect the antibacterial oral care toothpaste of the present invention against gingival pathogens.

[0027] Experimental objective: Experimental group A used the antibacterial oral care toothpaste provided in Example 1, while control group A used a blank toothpaste that did not contain the extract of *Syzygium aromaticum* but had the same other matrix components.

[0028] Test Method: Following the quantitative bactericidal test method specified in section 2.2.11.3.2 of the 2002 edition of the "Disinfection Technical Specifications", 1.0 g of the test sample and the blank control sample were dissolved in 20 mL of sterile phosphate buffer and thoroughly mixed to prepare a 1:20 test solution. The test solution was then mixed with an equal volume of Prevotella intermedius or Fusobacterium nucleatum suspension. The mixture was incubated at 20°C for 1 min. After terminating the reaction with a neutralizing agent, viable bacteria were counted, and the inhibition rate was calculated. The inhibition rate was calculated using the following formula: Inhibition Rate (%) = (Average Colony Count of Control Group A - Average Colony Count of Test Group A) / Average Colony Count of Control Group A × 100%; where the average colony count of Control Group A refers to the viable bacterial concentration (cfu / mL) obtained after culturing the bacterial suspension without the test sample under the same conditions, and the average colony count of Test Group A refers to the concentration of surviving colonies (cfu / mL) in the bacterial suspension after adding the test sample and incubating for a specific time.

[0029] Table 1. Detection indicators of anti-gingival pathogenic bacteria activity in Experiment Example 1 according to Figure 3 , Figure 4As shown in Table 1, the toothpaste containing *Syzygium styracifolium* extract reduced the number of *Prevotella intermedius* and *Fusobacterium nucleatum* platelets to below the detection limit (<10 CFU / mL) after 1 minute of action, with an inhibition rate exceeding 99.97%. In contrast, the blank control group and the control group without extract showed dense colony growth. This indicates that the present invention, by pre-assembling *Syzygium styracifolium* extract rich in active ingredients such as privetin, rhubarb glycoside, and polyphenols with polyquaternium-22 and cellulose gum to construct a sustained-release composite system, not only achieves rapid and efficient specific inhibition of periodontal pathogens, but also that the composite carrier effectively enhances the retention and sustained release of active ingredients at the oral site of action, thereby achieving a significant antibacterial effect within a short time.

[0030] Experimental Example 2 The purpose of this experimental group is to investigate the effects of different ingredient ratios on antibacterial oral care toothpaste, and to test the inhibition rate of dental plaque biofilm formation, the clearance efficiency of Porphyromonas gingivalis, and the 24-hour sustained release rate of active ingredients in a simulated tooth surface environment.

[0031] Experimental Objective: Experimental groups A, B, C, and D adopted the component ratios of krill oil provided in Examples 1-4, respectively; the control group consisted of control groups A, B, C, D, E, and F, wherein: Control group A Weigh out 20wt% of sorbitol, 20wt% of hydrated silica, 20wt% of deionized water, 83wt% of polyethylene glycol, 1.5wt% of sodium lauryl sulfate, 1wt% of fragrance, 0.5wt% of polyquaternium-22, 1wt% of cellulose gum, 0.3wt% of sodium saccharin, 0.5wt% of hydroxypropyl guar gum, 0.1wt% of sodium methylparaben, and 0.3wt% of triclosan. All water-soluble ingredients (including all deionized water, sorbitol, polyethylene glycol-8, sodium saccharin, and sodium methylparaben) were added to a vacuum toothpaste maker and stirred until dissolved at 40°C and 500 rpm. Then, hydrated silica, cellulose gum, and hydroxypropyl guar gum were added sequentially, and the mixture was sheared and dispersed at 800 rpm for 30 minutes. Subsequently, sodium lauryl sulfate, polyquaternium-22, and triclosan were added and mixed at 400 rpm for 20 minutes. Finally, the fragrance was added, and the mixture was vacuum degassed for 10 minutes under low-speed stirring at 150 rpm to obtain the comparison toothpaste.

[0032] Control group B Weigh out 20wt% sorbitol, 20wt% hydrated silica, 20wt% deionized water, 3wt% polyethylene glycol-8, 1.5wt% sodium lauryl sulfate, 1wt% fragrance, 1wt% cellulose gum, 0.3wt% sodium saccharin, 0.5wt% hydroxypropyl guar gum, 0.1wt% sodium methylparaben, and 0.25wt% Scutellaria baicalensis water extract. Add all deionized water, sorbitol, and polyethylene glycol-8 to a toothpaste-making machine and stir at 600 rpm at 45°C. Then, add hydrated silica, cellulose gum, and hydroxypropyl guar gum sequentially, and shear at high speed for 25 min to form a paste base. Next, add the Scutellaria baicalensis water extract directly to the paste base and mix at 400 rpm for 15 min. Finally, add sodium lauryl sulfate, fragrance, sodium saccharin, and sodium methylparaben, stir at 200 rpm, and degas under vacuum for 8 min to obtain a comparative toothpaste.

[0033] Control group C Take 0.25 wt% of the *Syzygium aromaticum* extract obtained by the same method as in Example 1, and weigh out 20 wt% of sorbitol, 20 wt% of hydrated silica, 20 wt% of deionized water, 83 wt% of polyethylene glycol, 1.5 wt% of sodium lauryl sulfate, 1 wt% of fragrance, 0.5 wt% of polyquaternium-22, 1 wt% of cellulose gum, 0.3 wt% of sodium saccharin, 0.5 wt% of hydroxypropyl guar gum, and 0.1 wt% of sodium methylparaben. All solid powders (hydrated silica, cellulose gum, hydroxypropyl guar gum) and all liquid components (deionized water, sorbitol, polyethylene glycol-8) were added to a vacuum toothpaste maker at one time. The temperature was set to 42°C, and the mixture was sheared and mixed at a high speed of 700 r / min for 30 min. Then, the extract of *Syzygium aromaticum*, sodium lauryl sulfate, polyquaternium-22, fragrance, sodium saccharin, and sodium methylparaben were added all at once. The speed was reduced to 400 r / min and the mixture was mixed for another 20 min. Finally, the mixture was degassed under vacuum at a speed of 150 r / min for 10 min to obtain the comparison toothpaste.

[0034] Control group D Take 0.25 wt% of the *Syzygium aromaticum* extract obtained by the same method as in Example 1, and weigh out 20 wt% of sorbitol, 20 wt% of hydrated silica, 20 wt% of deionized water, 3 wt% of polyethylene glycol-8, 1.5 wt% of sodium lauryl sulfate, 1 wt% of fragrance, 1 wt% of cellulose gum, 0.3 wt% of sodium saccharin, 0.5 wt% of hydroxypropyl guar gum, and 0.1 wt% of sodium methylparaben. First, hydroxypropyl guar gum, cellulose gum, and 35% deionized water were stirred at 30°C and 300 rpm to form a gel solution. Then, *Syzygium aromaticum* extract was added dropwise and mixed evenly. Next, the remaining materials (except sodium lauryl sulfate, fragrance, sodium saccharin, and sodium methylparaben) were dispersed at 42°C and 700 rpm for 25 min in a vacuum toothpaste-making machine to form a basic paste. Subsequently, the gel solution containing the extract was added to the paste and mixed at 42°C and 350 rpm for 20 min. Sodium lauryl sulfate was then added and stirring was continued for 12 min. Finally, fragrance, sodium saccharin, and sodium methylparaben were added, and the mixture was vacuum degassed at 120 rpm for 8 min to obtain the comparative toothpaste.

[0035] Control group E The dried leaves of *Heliotropium indicum* were pulverized and passed through a No. 3 sieve. Ten times the volume of pure water was added, and the mixture was heated to 90°C and refluxed for one extraction for 2 hours. The extract was then filtered and concentrated to obtain an aqueous extract. 0.25 wt% of this aqueous extract (based on its dry matter content) was weighed, along with the following components: 20 wt% sorbitol, 20 wt% hydrated silica, 20 wt% deionized water, 83 wt% polyethylene glycol, 1.5 wt% sodium lauryl sulfate, 1 wt% fragrance, 0.5 wt% polyquaternium-22, 1 wt% cellulose gum, 0.3 wt% sodium saccharin, 0.5 wt% hydroxypropyl guar gum, and 0.1 wt% sodium methylparaben. The preparation process is the same as the pre-assembly-step integration method in Example 1. First, 30% of polyquaternium-22, hydroxypropyl guar gum, cellulose gum and 35% of deionized water are used to make a gel solution. Water extract is added dropwise to form a composite gel. Then it is integrated with the base paste made from the remaining materials. The subsequent steps are exactly the same as in Example 1 to obtain the comparative toothpaste.

[0036] control group F Take 0.25 wt% of the *Syzygium aromaticum* extract obtained by the same method as in Example 1, and weigh out 20 wt% of sorbitol, 20 wt% of hydrated silica, 20 wt% of deionized water, 83 wt% of polyethylene glycol, 1.5 wt% of cocamidopropyl betaine, 1 wt% of fragrance, 0.5 wt% of polyquaternium-22, 1 wt% of cellulose gum, 0.3 wt% of sodium saccharin, 0.5 wt% of hydroxypropyl guar gum, and 0.1 wt% of sodium methylparaben. The preparation process adopted the same pre-assembly-step integration method as in Example 1. First, 30% of polyquaternium-22, hydroxypropyl guar gum, cellulose gum and 35% of deionized water were used to make a gel solution, and then the extract of *Syzygium aromaticum* was added dropwise to form a composite gel. Then, the remaining materials (except for cocamidopropyl betaine, the remaining polyquaternium-22, fragrance, sodium saccharin and sodium methylparaben) were used to make a base paste. Then, the composite gel and the paste were mixed, cocamidopropyl betaine and the remaining polyquaternium-22 were added and stirred. Finally, fragrance and other excipients were added and degassed to obtain the comparative toothpaste.

[0037] Test methods: Based on the invention, tests were conducted on the toothpaste's inhibition rate of dental plaque biofilm formation, its clearance efficiency against *Porphyromonas gingivalis*, and its 24-hour sustained-release rate of the active ingredient in a simulated tooth surface environment. The specific test methods are as follows: Inhibition rate of dental plaque biofilm formation: Based on the method for establishing an in vitro model of oral microbial biofilm, toothpaste samples from the experimental and control groups were prepared into a 1:20 (w / v) test solution using sterile simulated saliva. The test solution and freshly cultured mixed dental plaque flora (including Porphyromonas gingivalis, Streptococcus mutans, etc.) were co-inoculated into 24-well plates covered with hydroxyapatite sheets and incubated at 37°C under anaerobic conditions for 48 hours to form a mature biofilm. After incubation, the culture medium was discarded, and the biofilm was gently rinsed with phosphate buffer. The biofilm was stained three times to remove non-adhesive bacteria; an appropriate amount of crystal violet staining solution was added to each well, and after staining at room temperature for 20 min, the wells were repeatedly rinsed with deionized water until the eluent was colorless, and then 95% ethanol was added to dissolve the dye bound to the biofilm; the absorbance (OD value) of each well was measured at 590 nm using an ELISA reader; the culture wells without any toothpaste sample were used as negative controls (100% biofilm formation); the biofilm formation inhibition rate (%) = [1 – (OD value of experimental group / OD value of negative control group)] × 100%.

[0038] The clearance efficiency against *Porphyromonas gingivalis* was determined using a modified suspension bactericidal test. Standard strains of *Porphyromonas gingivalis* were revived and cultured to the logarithmic growth phase in brain and heart broth supplemented with heme and vitamin K. The bacterial suspension concentration was adjusted to approximately 1 × 10^7 CFU / mL with sterile physiological saline. Each group of toothpaste samples was mixed with sterile phosphate buffer at a ratio of 1:20 (w / v) and vortexed to prepare a homogeneous test solution. 0.5 mL of the test solution was mixed with an equal volume of the bacterial suspension in a sterile centrifuge tube and placed in a 37°C water bath for 2 minutes. Immediately after contact, 4 mL of a diluent containing a neutralizing agent was added to terminate the reaction. Mix thoroughly by vortexing; then perform a series of 10-fold serial dilutions, and spread 0.1 mL of the bacterial suspension at an appropriate dilution onto pre-reduced Brucella blood agar plates, and incubate in an anaerobic environment at 37°C for 5-7 days; count the colonies on the plates and convert them to the number of viable bacteria per milliliter of the original bacterial suspension (CFU / mL); use the bacterial suspension in contact with blank buffer containing no active ingredients in toothpaste as the initial bacterial count control; clearance efficiency (%) = [(average CFU / mL of initial bacterial count control – average CFU / mL of experimental group) / average CFU / mL of initial bacterial count control] × 100%.

[0039] 24-hour sustained-release rate of active ingredients in a simulated tooth surface environment: An in vitro simulated oral retention and release model was used. Appropriate amounts of each toothpaste sample were accurately weighed and evenly coated onto the surface of a hydroxyapatite disc pretreated with a simulated tooth surface smear layer, forming a film of a specified thickness. The disc containing the sample was fixed in a flow cell and kept at a constant temperature of 37°C. Simulated saliva (pH 6.8) was used as the release medium and continuously pumped into the flow cell at a flow rate of 1.0 mL / min. Effluent was collected at time points of 0.5, 1, 2, 4, 8, 12, and 24 hours. The concentration of representative active ingredients (such as privetin) in the collected effluent at each time point was determined by high-performance liquid chromatography (HPLC). The cumulative release amount at each time point was calculated. The 24-hour sustained-release rate (%) was defined as the percentage of the cumulative release amount at 24 hours relative to the total labeled content of the active ingredient in the toothpaste sample.

[0040] Specific testing indicators are shown in Table 2.

[0041] Table 2. Detection indicators of each sample in Experiment Example 2 Dental plaque biofilm formation inhibition rate (%) Elimination efficiency (%) of Porphyromonas gingivalis 24-hour sustained-release rate of active ingredient (privetin) (%) Experimental group A 92.5 99.2 85.4 Experimental group B 89.8 98.7 82.1 Experimental group C 90.3 98.9 83.6 Experimental group D 91.6 99.0 84.8 Control group A 88.1 99.5 Not applicable (chemically synthesized ingredients) Control group B 65.4 72.8 31.5 (baicalin) Control group C 78.2 90.1 45.7 Control group D 82.5 92.3 58.9 Control group E 71.6 85.4 68.2 control group F 90.8 98.5 84.0 according to Figures 5-7 As shown in Table 2, the summary of the above comparative data is as follows: First, through a horizontal comparison between the experimental group and multiple control groups, it was demonstrated that the specific *Scutellaria baicalensis* extract and its extraction process used in this invention are the core of achieving a highly efficient and broad-spectrum antibacterial effect. Specifically, the embodiments of this invention (experimental group AD) showed significantly better performance than control group B (65.4%, 72.8%), which used conventional *Scutellaria baicalensis* water extract, in two key indicators: the inhibition rate of dental plaque biofilm (89.8%-92.5%) and the clearance efficiency against *Porphyromonas gingivalis* (98.7%-99.2%). This result directly confirms the problem pointed out in the background art, namely, that the use of common herbal crude extracts leads to a narrow antibacterial spectrum and insufficient efficacy. The *Scutellaria baicalensis* extract obtained by this invention through ethanol fractional ultrasonic extraction and gradient enrichment process, rich in privetin, rhubarb glycoside, ursolic acid, polyphenols, and flavonoids, forms a synergistic antibacterial network, thereby enhancing the targeted inhibition ability against periodontal pathogenic biofilms and specific pathogenic bacteria. Secondly, the comparative test results highlight the key role of the "pre-assembly-step integration" preparation process of this invention in the long-term sustained release of active ingredients. The 24-hour sustained release rate of privetin in experimental group A (85.4%) far exceeded that of control group C (45.7%), which did not use this process, and control group D (58.9%), which did not use polyquaternium-22 to construct the composite carrier. Moreover, even when using the same pre-assembly process as this invention, the sustained release rate using the water extract (control group E) (68.2%) was still significantly lower than that of the experimental group using the specific extract of this invention. This indicates that the step of pre-preparing the active ingredients of *Ligusticum striatum* with some polyquaternium-22 and colloids into a composite gel carrier effectively solves the technical problems of easy loss and short action time of plant active ingredients in the oral environment. The three-dimensional network structure formed by this process can enhance the adsorption and retention of active substances on the tooth surface and gingival sulcus, thereby prolonging the residence and action time of active ingredients in the oral cavity. Finally, the combined data from each control group demonstrated that the synergistic effect of the various technical features in the present invention is the foundation for achieving comprehensive nursing efficacy. For example, although control group A, which was replaced solely with the chemical antibacterial agent triclosan, showed similar cleaning efficiency, it lacked the gentleness and multi-effect synergy of natural ingredients and could not provide sustained-release function of active ingredients. Control group F, which only changed the foaming agent system, had similar indicators to experimental group A, but the synergistic effect of sodium lauryl sulfate and polyquaternium-22 had specific value in improving physical cleaning effect. Therefore, the present invention systematically integrates the specific composition of the *Syzygium aromaticum* extract, the sustained-release carrier constructed with polyquaternium-22 and other ingredients through a specific process, and the cleaning efficacy of sodium lauryl sulfate, ultimately achieving a balance between high-efficiency antibacterial, long-lasting sustained release, and physical cleaning, thereby improving the comprehensive efficacy and gentleness of oral care products.

[0042] The foregoing has shown and described the basic principles, main features, and advantages of the present invention. Those skilled in the art should understand that the present invention is not limited to the above embodiments. The embodiments and descriptions in the specification are merely preferred examples and are not intended to limit the invention. Various changes and modifications can be made to the invention without departing from its spirit and scope, and all such changes and modifications fall within the scope of the present invention as claimed. The scope of protection of the present invention is defined by the appended claims and their equivalents.

Claims

1. An antibacterial oral care toothpaste based on the active ingredient of *Syzygium aromaticum*, characterized in that, Including the following raw materials: Sorbitol, hydrated silica, deionized water, polyethylene glycol-8, sodium lauryl sulfate, fragrance, polyquaternium-22, cellulose gum, sodium saccharin, hydroxypropyl guar gum, sodium methylparaben, and *Hedysarum heterotropoides* extract; among which: Sodium lauryl sulfate can synergistically enhance the physical removal effect on dental plaque by interacting with polyquaternium-22 in the oral environment. The extract of *Syzygium aromaticum* interacts with polyquaternium-22 and cellulose gum to form a composite carrier system that helps the active ingredients to be adsorbed and released slowly on the tooth and gingival surfaces, thereby synergistically enhancing the specific inhibitory efficacy against periodontal pathogens *Prevotella intermedius* and *Fusobacterium nucleatum*.

2. The antibacterial oral care toothpaste based on the active ingredient of *Syzygium aromaticum* according to claim 1, characterized in that, The amount of sorbitol used is 15-25 wt%; the amount of hydrated silica used is 15-25 wt%; the amount of deionized water used is 15-25 wt%; the amount of polyethylene glycol-8 used is 1-5 wt%; the amount of sodium lauryl sulfate used is 1-3 wt%; the amount of fragrance used is 0.5-1.5 wt%; the amount of polyquaternium-22 used is 0.1-1 wt%; the amount of cellulose gum used is 0.5-1.5 wt%; the amount of sodium saccharin used is 0.1-0.5 wt%; the amount of hydroxypropyl guar gum used is 0.1-1 wt%; the amount of sodium methylparaben used is 0.05-0.15 wt%; and the amount of *Syzygium aromaticum* extract used is 0.1-0.5 wt%.

3. The antibacterial oral care toothpaste based on the active ingredient of *Syzygium aromaticum* according to claim 1, characterized in that, The extract of *Syzygium aromaticum* includes the following extraction steps: S1.1 Take dried leaves of *Syzygium serratum* and crush them to pass through a No. 3 sieve to obtain uniform powder raw material. Then, put it together with 90% ethanol solution into a sealed extraction container and stir to allow the plant cell walls to swell gently and form a uniform suspension. S1.2 The suspension is placed in an ultrasonic extraction device for three extractions to obtain three extracts, A, B and C. Then, these three extracts are mixed and collected according to their ethanol concentration to obtain a mixed extract. S1.3 Concentration and Extraction: The mixed extract was transferred to a rotary evaporator and concentrated under reduced pressure at a water bath temperature of 40-50℃ and a pressure of less than 0.09MPa until the solution volume was reduced to 5-10% of the original volume and no ethanol odor was released, resulting in a brownish-brown, uniform, thick paste-like extract of *Syzygium styracifolium*.

4. The antibacterial oral care toothpaste based on the active ingredient of *Syzygium aromaticum* according to claim 3, characterized in that, In step S1.1, the amount of 90% ethanol solution used is 2.8-3.2 times the volume of the powdered raw material; the sealed extraction container is continuously stirred at a speed of 30-50 r / min for 20-30 min at room temperature.

5. The antibacterial oral care toothpaste based on the active ingredient of *Syzygium aromaticum* according to claim 3, characterized in that, In step S1.2, the ultrasonic extraction device extraction includes the following steps: First, set the ultrasonic extraction device to a constant temperature of 25-28℃ and an ultrasonic power of 280-320W to perform the first extraction on the suspension for 18-22 minutes. After extraction, perform solid-liquid separation using medium-speed filter paper and collect the first clear extract, which is labeled as part A. Add the same volume and concentration of 90% ethanol solution as the first extraction to the separated solid residue. Under the same temperature and ultrasonic power conditions, repeat the second and third extractions. Each extraction time is 18-22 min. Collect the clear extracts by filtration and label them as part B and part C, respectively.

6. The antibacterial oral care toothpaste based on the active ingredient of *Syzygium aromaticum* according to claim 3, characterized in that, In S1.3, the extract of *Syzygium aromaticum* includes at least privetin, rhubarb glycoside, ursolic acid, total polyphenols, and total flavonoids.

7. The antibacterial oral care toothpaste based on the active ingredient of *Syzygium aromaticum* according to claim 6, characterized in that, The content of privetin is 4.9-5.4%; the content of rhubarb glycoside is 0.9-1.1%; the content of ursolic acid is 0.4-0.5%; the content of total polyphenols is 14.5-15.8%; and the content of total flavonoids is 7.9-8.5%.

8. The antibacterial oral care toothpaste based on the active ingredient of *Syzygium aromaticum* according to claim 1, characterized in that, The toothpaste is prepared using a pre-assembly-step integration process, which includes the following steps: S2.1 Add a portion of polyquaternium-22, hydroxypropyl guar gum, cellulose gum, and a portion of deionized water to a sealed mixing tank with stirring and temperature control functions. Stir at a medium speed of 200-400 r / min at 25-35℃ to form a cationic polymer mixed solution. Then, reduce the stirring speed to 50-100 r / min and add the extract of Scutellaria barbata dropwise under light-protected conditions to form an encapsulated composite gel. S2.2 Add sorbitol, hydrated silica, polyethylene glycol-8 and the remaining deionized water to a vacuum ointment maker and disperse at high speed at 40-45℃ and 600-800r / min for 20-30min to form a dense and smooth base ointment. S2.3 Transfer the composite gel to the base paste and mix continuously for 15-25 minutes at a medium speed of 300-400 r / min at 40-45℃. Then, add sodium lauryl sulfate and the remaining polyquaternium-22 and continue stirring for 10-15 minutes. Next, add the fragrance, sodium saccharin and sodium methylparaben. Turn on the vacuum and homogenize and degas at a speed of 100-150 r / min for 5-10 minutes to obtain the final product paste.

9. The antibacterial oral care toothpaste based on the active ingredient of *Syzygium aromaticum* according to claim 1, characterized in that, In step S2.1, the amount of polyquaternium-22 used accounts for 30%-50% of the total amount of polyquaternium-22 used, and the amount of deionized water used accounts for 30%-40% of the total amount of deionized water used.

10. The antibacterial oral care toothpaste based on the active ingredient of *Syzygium aromaticum* according to claim 1, characterized in that, The antibacterial oral care teeth described in claims 1-7 are used to inhibit pathogenic microorganisms related to gingivitis and periodontitis, and in daily oral hygiene care.

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