Preparation method and application of moutan bark paeonol crystal

Abstract

The invention discloses a preparation method and application of moutan bark and paeonol crystals. The preparation method of the moutan bark and paeonol crystal provided by the invention comprises the following steps: (1) uniformly mixing crushed moutan bark and a sodium chloride aqueous solution in a distillation flask of a distillation device, and soaking the moutan bark; (2) connecting a distillation device, turning on a heater, simultaneously turning on a condensation pipe and an interlayer U-shaped pipe to feed and discharge water, setting a distillation temperature, a condensation water temperature of the condensation pipe and a condensation water temperature of the interlayer U-shaped pipe, heating and distilling, and collecting distillate after the distillation is finished; (3) cooling and crystallizing the distillate; and (4) carrying out suction filtration on the distillate after cooling crystallization to obtain white needle-like crystals, and drying to obtain paeonol crystals. According to the method, the volatility of the paeonol extraction crystal is reduced, the crystal stability is improved, the crystal product quality is improved, the surface area of the crystal is reduced, and meanwhile, the purity and the stability of the product are improved.

Description

Technical Field

[0001] The present invention relates to a method for preparing an active ingredient, and in particular to a method for preparing paeonol crystals from peony bark and its application. Background Art

[0002] Moutan bark is a common herbal medicine widely used in traditional Chinese medicine to treat blood stasis and related conditions, such as dysmenorrhea and blood-stasis skin diseases. Early research focused on the pharmacological effects and chemical composition of moutan bark as a whole. With advances in science and technology, researchers have become increasingly interested in studying the active ingredients in moutan bark. Studies have shown that paeonol, one of its main active ingredients, exhibits multiple pharmacological activities. Paeonol has significant antioxidant properties, neutralizing free radicals and alleviating cellular damage caused by oxidative stress. It also has anti-inflammatory effects, suppressing inflammatory responses and modulating the immune system. Paeonol also exhibits certain pharmacological activities in blood circulation. Studies have shown that paeonol can inhibit platelet aggregation and thrombosis, thus exerting antithrombotic effects. It can also dilate blood vessels, improve microcirculation, promote blood flow, and protect the cardiovascular system. In addition to cardiovascular research, paeonol has also been found to possess various pharmacological activities, including anti-tumor, antispasmodic, analgesic, and antibacterial properties.

[0003] In the study of paeonol, the improvement of extraction methods has also become one of the research focuses. Traditional extraction methods include steam distillation, alcohol extraction and ultrasonic-assisted extraction. In recent years, some new extraction technologies have also been developed, such as supercritical fluid extraction, microwave-assisted extraction and enzymatic hydrolysis. Steam distillation is the most commonly used method for extracting paeonol in laboratories and industries. It has the advantages of being environmentally friendly, natural and retaining active ingredients. Patent application with publication number CN108403791A provides a preparation of a peony bark extract with a high paeonol content. The raw material peony bark is extracted with water as a solvent by warm immersion or reflux extraction to obtain an extract; the obtained extract is added to a vacuum concentration-volatile oil collection system, and concentrated under vacuum to obtain a concentrated solution. At the same time, the volatile component paeonol produced during the vacuum concentration process is condensed and collected by a volatile oil collection device; the obtained paeonol is added to the concentrated solution to obtain a peony bark extract fluid extract. The paeonol content in the obtained peony bark extract is 1.9-7.7%, and the paeonol exists in the form of a mixed extract. Patent application publication number CN110551012A applies steam distillation to extract paeonol: the distillate is separated into volatile oil containing paeonol and aromatic water containing paeonol through an oil-water separator, and then total paeonol is obtained by cooling and crystallization. This method has a high yield for extracting paeonol, but the extraction process is cumbersome and may lead to loss or degradation of paeonol components. In addition, the large-scale use of organic solvents poses a safety hazard in industrial production, and the paeonol product contains residual organic solvents. Patent application publication number CN103787859A applies CO2 supercritical extraction to extract paeonol: peony bark powder is placed in anhydrous ethanol and ultrasonicated, then dried and mixed evenly with β-cyclodextrin in a mass ratio of 2-3:1, granulated, and sent to a supercritical extraction kettle to obtain high-purity paeonol after extraction. However, this method is costly and complex, making it unsuitable for industrial production. The melting point of the paeonol crystal product is 49-51°C and it is volatile. The scanning electron microscope image of the crystal shows that there are cavities on the crystal surface, which is caused by the volatilization of paeonol. Summary of the Invention

[0004] In view of this, the present invention provides a preparation method and application of paeonol crystals from peony bark.

[0005] The method for preparing paeonol crystals from peony bark provided by the present invention comprises the following steps:

[0006] (1) mixing the crushed peony bark and a sodium chloride aqueous solution in a distillation flask of a distillation apparatus to uniformly soak the peony bark;

[0007] (2) Connect the distillation apparatus, turn on the heater, and simultaneously open the water inlet and outlet of the condenser and the interlayer U-shaped tube. Set the distillation temperature, the condensed water temperature of the condenser, and the condensed water temperature of the interlayer U-shaped tube. Heat and distill. After the distillation is completed, collect the distillate.

[0008] (3) subjecting the distillate to cooling crystallization;

[0009] (4) filtering the distillate after the crystallization by cooling to obtain white needle-shaped crystals, and drying the crystals to obtain paeonol crystals;

[0010] The distillation device includes a heater 1, a distillation flask 2, a thermometer 3, a first bend 6, a condenser 9, a second bend 12, an interlayer U-shaped tube 19, and a third bend 23; wherein, the top opening of the distillation flask 2 is sealedly connected to the first end 5 of the first bend; the second end 8 of the first bend is sealedly connected to the first end 16 of the condenser; the second end 17 of the condenser is sealedly connected to the first end 11 of the second bend; the second end 13 of the second bend is sealedly connected to the first end of the interlayer U-shaped tube 19; the second end of the interlayer U-shaped tube 19 is sealedly connected to the first end 22 of the third bend.

[0011] Preferably, in step (1), the crushed peony bark is peony bark powder passed through an 80-100 mesh sieve; the mass percentage concentration of the sodium chloride aqueous solution is 4%-6%; the material-liquid ratio of the peony bark to the sodium chloride aqueous solution is 1g / 10mL-1g / 20mL; and the soaking time is 18h-24h.

[0012] Preferably, the distillation temperature is 100°C-102°C; the condensed water temperature of the condenser is 60°C-62°C; the condensed water temperature of the interlayer U-tube is 55°C-58°C, and the heating distillation time is 2.5h-2.8h.

[0013] Preferably, the distillate in step (3) is a distillate at 35°C-40°C; and the cooling crystallization is performed by cooling the temperature to 2°C-4°C for 20h-24h according to a cooling rate curve.

[0014] Preferably, the conditions for the filtration in step (4) are a temperature of 20-25°C and a pressure of 0.04-0.06 MPa; and the drying temperature is 20-25°C.

[0015] The paeonol crystals from the peony bark prepared by the method also fall within the protection scope of the present invention.

[0016] The present invention also provides a toothpaste, which is prepared from the following ingredients in parts by mass: 0.3-0.5 parts of paeonol crystals, 45-50 parts of abrasives, 1.5-2.5 parts of foaming agents, 1.5-2.5 parts of thickeners, 20-25 parts of moisturizers, 0.5-1.0 parts of flavoring agents, 0.2-0.5 parts of xylitol, 0.3-0.5 parts of methylparaben, 0.4-0.8 parts of Xanthoceras sorbifolia oil, and the remainder being water;

[0017] Preferably, the paeonol crystals are effective anti-inflammatory factors; the abrasive is composed of calcium hydrogen phosphate dihydrate and hydrated silica, the foaming agent is composed of sodium lauryl sulfate and sodium N-lauroyl sarcosine, the thickener is composed of sodium carboxymethyl cellulose and sodium hydroxyethyl cellulose, the moisturizer is composed of sorbitol and glycerin, the flavoring agent is menthol, the sweetener is xylitol and edible saccharin, and the preservative is methylparaben.

[0018] Preferably, the mass ratio of the friction agent hydrated silica to dihydrated calcium phosphate is (0-1): (8-9); the mass ratio of the foaming agent sodium N-lauroyl sarcosinate to sodium lauryl sulfate is (0-1): (4-6); the mass ratio of the thickener sodium hydroxyethyl cellulose to sodium carboxymethyl cellulose is (0-1): (3-5); the mass ratio of the moisturizing agent sorbitol to glycerin is 1: (1.0-1.2).

[0019] Preferably, the toothpaste is made of the following ingredients by mass: 0.3-0.5 parts of paeonol crystals, 40-42 parts of calcium hydrogen phosphate dihydrate, 3-5 parts of hydrated silica, 1.5-2.0 parts of sodium lauryl sulfate, 0.5-1.0 parts of sodium N-lauroyl sarcosinate, 1.5-2.0 parts of sodium carboxymethyl cellulose, 0.4-0.8 parts of sodium hydroxyethyl cellulose, 10-12 parts of sorbitol, 10-13 parts of glycerol, 0.2-0.5 parts of xylitol, 0.5-1.0 parts of menthol, 0.3-0.5 parts of methylparaben, 0.4-0.8 parts of Xanthoceras sorbifolia oil and 20-25 parts of water.

[0020] The preparation method of the toothpaste comprises the following steps:

[0021] (1) Glycerin, Xanthoceras sorbifolia oil, menthol and sodium carboxymethyl cellulose are mixed to obtain glue A;

[0022] (2) adding methylparaben to water, heating to 80-85°C to fully dissolve for 3-5 minutes, cooling to 50-55°C, adding xylitol, sorbitol, sodium lauryl sulfate, sodium N-lauroyl sarcosinate and paeonol crystals to obtain aqueous solution B;

[0023] (3) mixing the glue solution A with the aqueous solution B, stirring at 50-55° C. for 5-10 minutes to obtain solution C;

[0024] (4) Adding powdered calcium hydrogen phosphate dihydrate and hydrated silica to the liquid C to prepare toothpaste.

[0025] Beneficial effects:

[0026] (1) Paeonol exists in the cell tissue of peony bark and is wrapped by the cell wall. The addition of sodium chloride in the soaking solution, the osmotic pressure generated by the salt and repeated freezing and thawing both promote the destruction of the cell wall structure, which is conducive to the exudation of paeonol and the improvement of the paeonol extraction rate.

[0027] (2) The present invention innovatively utilizes a sandwich U-shaped tube to control the temperature of the interlayer circulating water, thereby controlling the temperature of the distillate in the U-shaped tube, thereby ensuring that paeonol exists in a liquid state and preventing the temperature from falling below the melting point, which would cause paeonol to precipitate. This allows the paeonol liquid to overflow from the outlet end through the U-shaped tube water phase, while the oil phase remains on the surface of the U-shaped tube water phase, achieving a one-time separation of oil and paeonol.

[0028] (3) The distillate crystallization method selected by the present invention is cooling crystallization according to the optimized cooling curve to achieve secondary separation of paeonol. The entire crystallization process maintains the solution supersaturation approximately constant, which is conducive to crystal growth, obtains large-particle paeonol crystals, and improves the purity and stability of the crystal product.

[0029] (4) The entire extraction process of the present invention is simple and easy to control, and no organic solvent is used throughout the process. It is a green and efficient separation and extraction method that conforms to the concept of energy conservation and environmental protection.

[0030] The method for preparing paeonol proposed in the present invention improves the industrial adaptability of paeonol extraction, reduces the volatility of paeonol extracted crystals, improves crystal stability, enhances crystal product quality, and reduces the surface area of ​​the crystals. Increasing the crystal size not only helps reduce the surface area of ​​the crystals, but also helps improve the purity of the product.

[0031] The toothpaste formula of the present invention adds high-purity paeonol crystals as a functional ingredient, which has high purity and is conducive to effectively exerting anti-inflammatory effects. At the same time, the addition of Xanthoceras sorbifolia oil, which contains nervonic acid, helps to slow the proliferation of periodontal nerve cells and synergizes with paeonol to achieve the dual effects of anti-inflammatory and promoting nerve cell proliferation in the periodontium. BRIEF DESCRIPTION OF THE DRAWINGS

[0032] For purposes of illustration and not limitation, the present invention will now be described with reference to preferred embodiments thereof, particularly with reference to the accompanying drawings, in which:

[0033] Figure 1 This is a schematic diagram of the device for extracting paeonol crystals according to the present invention;

[0034] In the figure: 1. heater; 2. distillation flask; 3. thermometer; 4. first bracket; 5. first end of first bend; 6. first bend; 7. first clamp; 8. second end of first bend; 9. condenser; 10. condensate inlet and outlet; 11. first end of second bend; 12. second bend; 13. second end of second bend; 14. second bracket; 15. second clamp; 16. first end of condenser; 17. second end of condenser; 18. rubber stopper; 19. sandwich U-shaped tube; 20. water outlet of sandwich U-shaped tube; 21. water inlet of sandwich U-shaped tube; 22. first end of third bend; 23. third bend; 24. second end of third bend; 25. container.

[0035] Figure 2 This is the cooling rate curve of paeonol.

[0036] Figure 3 This is a diagram showing the effect of the solid-liquid ratio on the extraction rate of paeonol.

[0037] Figure 4 This is a graph showing the effect of distillation time on the extraction rate of paeonol.

[0038] Figure 5 This is a diagram showing the effect of raw material particle size on the extraction rate of paeonol.

[0039] Figure 6 Response surface diagram and contour diagram for the interaction between liquid-to-solid ratio and distillation time.

[0040] Figure 7 Response surface diagram and contour diagram of the interaction between liquid-to-material ratio and raw material particle size.

[0041] Figure 8 Response surface and contour plots for the interaction between distillation time and raw material particle size.

[0042] Figure 9 The liquid phase spectrum of paeonol, where (a) is the liquid phase spectrum of paeonol standard, and (b) is the liquid phase spectrum of the sample.

[0043] Figure 10 The infrared spectra of paeonol are shown in Figure 1, where (a) is the infrared spectrum of the paeonol standard and (b) is the infrared spectrum of the sample.

[0044] Figure 11 The XRD spectra of paeonol are shown in Figure 2, where (a) is the XRD spectrum of the paeonol standard and (b) is the XRD spectrum of the sample.

[0045] Figure 12 This is a picture of paeonol under an optical microscope.

[0046] Figure 13 This is a scanning electron micrograph of paeonol.

[0047] Figure 14The effect of different concentrations of paeonol on inflammatory factors TNF-α, IL-6, and IL-1β. DETAILED DESCRIPTION

[0048] The specific embodiments do not limit the scope of protection of the present invention. Those skilled in the art will appreciate that various modifications, combinations, sub-combinations, and substitutions may occur depending on design requirements and other factors. Any modifications, equivalent substitutions, and improvements made within the spirit and principles of the present invention are intended to be included within the scope of protection of the present invention.

[0049] The technical solutions of the present invention will be further described in detail below with reference to specific examples. Unless otherwise specified, the raw materials and reagents used in the following examples are all commercially available products or can be prepared by known methods.

[0050] Figure 1 Schematic diagram of the distillation apparatus for the Paeonia lactiflora crystals of the present invention. Figure 1 As shown, the distillation apparatus includes a heater 1, a distillation flask 2, a thermometer 3, a first curved pipe 6, a condenser 9, a second curved pipe 12, a sandwich U-shaped tube 19, and a third curved pipe 23. The top opening of the distillation flask 2 is sealedly connected to the first end 5 of the first curved pipe; the second end 8 of the first curved pipe is sealedly connected to the first end 16 of the condenser; the second end 17 of the condenser is sealedly connected to the first end 11 of the second curved pipe; the second end 13 of the second curved pipe is sealedly connected to the first end of the sandwich U-shaped tube 19; and the second end of the sandwich U-shaped tube 19 is sealedly connected to the first end 22 of the third curved pipe. A first clamp 7 is fixed to one side of the first bracket 4 and holds the distillation flask 2. A second clamp 15 is fixed to one side of the second bracket 11 and holds the sandwich U-shaped tube 19.

[0051] The steam distillation device is mainly composed of a distillation flask 2, a condenser 9 and an interlayer U-shaped tube 19. The process of extracting paeonol from peony bark is as follows: first, the crushed peony bark is soaked in a sodium chloride solution and placed together in the distillation flask 2. The high-temperature water vapor is in full contact with the raw material, so that the paeonol in the peony bark evaporates together with the water vapor due to its volatility to form a mixed vapor. Based on Dalton's law of partial pressures, when the sum of the vapor pressures of the two reaches the external atmospheric pressure, they form an azeotropic mixture, and the paeonol is brought out into the first bend 6 at a temperature lower than its own boiling point; then the mixed vapor enters the condenser 9, is cooled and condensed into a liquid, and flows into the interlayer U-shaped tube 19 through the second bend 12. The interlayer U-shaped tube 19 will separate the water-insoluble impurities such as oil and fat brought out by the steam from the paeonol distillate and ensure that the paeonol will not precipitate prematurely, thereby greatly improving the purity and yield of the paeonol. Finally, it passes through the third bend 23 and flows out from the distillate outlet of the second end 24 of the third bend. The distillate is collected and placed in the container 25. The distillate is then cooled to precipitate a large amount of paeonol, which is then filtered and dried to obtain paeonol crystals. This device uses water vapor as a carrier, preventing paeonol from decomposing at high temperatures while efficiently separating the target components through volatility differences. This ensures the purity and extraction rate of paeonol, making it an effective technology for extracting volatile components from natural products.

[0052] Example 1: Method for extracting high-purity paeonol by steam distillation and application of paeonol in preparing toothpaste

[0053] (1) Method for extracting high-purity paeonol using steam distillation

[0054] The method for extracting high-purity paeonol by steam distillation in this experimental example comprises the following steps:

[0055] (1) Take an appropriate amount of clean and disease-free dry peony bark (purchased from Xuzhou Feixianran Biotechnology Co., Ltd.), grind it with a high-speed grinder, and pass it through an 80-mesh sieve. Weigh 100 g of the sieved peony bark powder, 60 g of sodium chloride, and 1500 mL of distilled water. First, dissolve the sodium chloride in distilled water. Then, mix the peony bark powder and the sodium chloride aqueous solution evenly in a distillation flask of a distillation apparatus and soak them at room temperature for 18 h.

[0056] (2) Add enough distilled water to the sandwich U-shaped tube 19 so that the liquid level at the left end of the sandwich U-shaped tube 19 is flush with the water outlet at the right end, and then press Figure 1 Connect the distillation apparatus as shown.

[0057] (3) Turn on the distillation heater 1, and simultaneously open the water inlet and outlet of the condenser 9 and the interlayer U-shaped tube 19, set the distillation temperature to 100°C, the condensed water temperature of the condenser to 60°C, and the condensed water temperature of the interlayer U-shaped tube 19 to 55°C, and heat the distillation for 2.5 hours. After the distillation is completed, collect all the distillate from the distillate outlet of the second end 24 of the third bend tube.

[0058] (4) The distillate was cooled to 40°C at room temperature and then transferred into a jacketed crystallizer (500 mL capacity, purchased from Tianjin Bozhao Chemical Technology Co., Ltd.) for crystallization according to the set cooling rate curve, such as Figure 2 As shown, the temperature was lowered for 20 h and the distillate dropped to 4°C.

[0059] (5) The distillate after cooling and crystallization was filtered using a circulating water multi-purpose vacuum pump at a filtration temperature of 25°C and a filtration pressure of 0.04 MPa to obtain white needle-shaped paeonol crystals. The crystals were dried to a constant weight at room temperature to obtain needle-shaped paeonol crystals with a white to slightly yellow color and a slightly bitter taste. The crystals weighed 1.054 g, the extraction rate was 1.054%, and the purity was 99.14%.

[0060]

[0061] Where ω is the extraction rate of paeonol; m 原 is the mass of the raw material, which is 100g; m 产 It is the mass of extracted paeonol.

[0062] The specific method for purity determination is the following liquid chromatography method.

[0063] (2) Application of Paeonol Crystals in the Preparation of Toothpaste

[0064] The raw materials and sources of paeonol toothpaste are shown in the following table:

[0065]

[0066]

[0067] The application of the paeonol prepared in this embodiment in preparing toothpaste comprises the following steps:

[0068] (1) 12 g of glycerol, 0.8 g of menthol and 2.0 g of sodium carboxymethyl cellulose (CMC) were mixed to obtain glue A.

[0069] (2) 0.3 g of methylparaben was added to 24.6 g of water, heated to 80°C for full dissolution for 5 min, cooled to 50°C, and 0.25 g of xylitol, 0.25 g of saccharin, 10 g of sorbitol, 2 g of sodium lauryl sulfate, 0.5 g of sodium N-lauroyl sarcosinate, 0.4 g of Xanthoceras sorbifolia oil, and 0.3 g of paeonol were added to obtain aqueous solution B.

[0070] (3) Mix the glue solution A with the aqueous solution B, stir at 50°C for 10 minutes, and obtain solution C.

[0071] (4) 42 g of calcium hydrogen phosphate dihydrate powder and 5 g of hydrated silica were added to liquid C to prepare a toothpaste mixture. The mixture was stirred at a low speed (200 rpm) for 15 min using a toothpaste vacuum mixer. The vacuum was then turned on and the vacuum degree was controlled to 0.06 MPa. The mixture was stirred and homogenized for 10 min to obtain a toothpaste paste.

[0072] (5) The toothpaste paste was centrifuged and degassed at 3000 rpm for 10 min and then transferred to an aging tank. The toothpaste paste was aged for 120 min to cool to room temperature before packaging.

[0073] Toothpaste stability, pH determination and efficacy experiments:

[0074] (1) Stability test method

[0075] Take 2 tubes of toothpaste, store one at room temperature and the other at -8±1℃ for 8 hours, place it at a constant temperature of 45±1℃ for 8 hours, return it to room temperature, open the lid and observe whether the paste overflows from the tube, turn the tube upside down and observe whether there is liquid dripping from the tube within 10 seconds; compare the aroma and color with the paste stored at room temperature.

[0076] (2) pH determination method

[0077] Take 5g of toothpaste from a tube, place it in a 50mL beaker, add 20mL of pre-boiled and cooled distilled water, stir evenly, and read the reading within 10 minutes at 20℃.

[0078] The stability and pH test results are shown in the following table:

[0079] (3) Toothpaste efficacy experiment

[0080]

[0081] By intervening in the lipopolysaccharide (LPS) (1 mg / mL)-induced mouse mononuclear macrophage leukemia cell (hereinafter referred to as RAW264.7 cells, purchased from Shanghai Fuheng Biotechnology Co., Ltd.) inflammation model (this model is established by lipopolysaccharide (LPS) stimulating cells), it was found that the expression of three pro-inflammatory cytokines, TNF-α, IL-6 and IL-1β, showed significant dose-dependent regulatory characteristics. Figure 14Experimental data showed that as the concentration of paeonol increased from 35μg / mL to 45μg / mL, the expression levels of the three inflammatory factors decreased in a step-by-step manner, with the 45μg / mL group showing the greatest inhibitory effect (TNF-α, IL-6, and IL-1β). When the concentration continued to increase to 50-55μg / mL, the levels of inflammatory factors increased, but were still lower than those in the LPS control group. This biphasic dose effect may suggest that the anti-inflammatory mechanism of paeonol is subject to complex concentration threshold regulation: within the optimal concentration range (45μg / mL), it exerts its maximum anti-inflammatory effect by effectively inhibiting the activation of key inflammatory signaling pathways such as NF-κB; at higher concentrations, it may activate compensatory regulatory mechanisms or induce mild cellular stress responses, resulting in a partial offset of the anti-inflammatory effect.

[0082] (3) Process optimization

[0083] 1. Single-factor experiment

[0084] (1) The effect of material-liquid ratio on the extraction rate of paeonol is shown in Table 1 and Figure 3 As shown in the figure, when the solid-liquid ratio (ratio of peony bark powder to sodium chloride aqueous solution) is lower than 1:17.5 (g / mL), the paeonol extraction rate increases with the increase in the solid-liquid ratio. When the solid-liquid ratio increases from 1:17.5 to 1:20 (g / mL), the paeonol extraction rate decreases with the increase in the solid-liquid ratio. This may be because the viscosity of the system increases with the increase in the solid-liquid ratio, which reduces the solubility of peony bark and thus reduces the dissolution of paeonol.

[0085] Table 1 Effects of different material-liquid ratios on paeonol

[0086]

[0087] (2) The effect of distillation time on the extraction rate of paeonol is shown in Table 2 and Figure 4 As shown in the figure, the extraction rate of paeonol increases with increasing distillation time, but the extraction rate begins to decrease after the distillation time exceeds 2.5 hours. This may be due to the prolonged heating time and the significant dilution of paeonol in the distillate, which affects the recrystallization yield. Prolonged heating of the medicinal material causes gelatinization of the residue, which adsorbs and entraps paeonol, hindering filtration and leading to a decrease in the extraction rate of paeonol.

[0088] Table 2 Effect of different distillation times on paeonol

[0089]

[0090] (3) The effect of raw material particle size on the extraction rate of paeonol is shown in Table 3 and Figure 5As shown in the figure, when the raw material particle size is greater than 0.1 cm, the extraction rate of paeonol decreases with increasing raw material particle size. This is because paeonol needs to travel a longer diffusion path to be released from the interior of the large particles into the solvent during the extraction process. The increase in the medicinal material particle size also leads to a decrease in the solid-liquid interfacial area. During the extraction process, paeonol needs to diffuse from the interface between the medicinal material solid phase and the solvent into the solution. Larger particles have a smaller solid-liquid interfacial area, which limits the contact area between the active ingredient and the solvent, thereby slowing the dissolution and diffusion rate of paeonol and causing a decrease in the extraction rate.

[0091] Table 3 Effect of different raw material particle sizes on paeonol

[0092]

[0093] 2. Response Surface Experiment

[0094] (1) Based on the results of the single-factor experiment, a three-factor three-level response surface optimization experiment was conducted. The factors and levels selected for the response surface experiment are shown in Table 4, and the experimental design and results are shown in Table 5.

[0095] Table 4 Experimental factor level table

[0096]

[0097] Table 5 Box-Behnken test design and results

[0098]

[0099]

[0100] (2) According to the test results obtained in Table 5, the fitting analysis was performed using Design Expert 13.0 software to obtain the quadratic polynomial regression equation:

[0101] Y=1.01-0.0304A+0.0500B-0.2446C-0.0028AB-0.0150AC-0.0103BC-0.1096A 2 -

[0102] 0.0503B 2 -0.1360C 2

[0103] The variance analysis of the above equation is shown in Table 6.

[0104] Table 6 Analysis of variance table of paeonol extraction rate

[0105]

[0106]

[0107] Note: **. Extremely significant difference (P < 0.01); *. Significant difference (P < 0.05).

[0108] As shown in Table 6, the P value of the lack-of-fit term is 0.0652, which means the lack-of-fit term is not significant. The P value of the model is less than 0.0001, which means the model is highly significant. According to the comparison of F values, the influence of each factor on the final yield can be concluded. The influence of raw material particle size (C) > distillation time (B) > liquid-to-material ratio (A). The influence of liquid-to-material ratio, distillation time and raw material particle size on the extraction rate of paeonol all reached an extremely significant level (P < 0.01). The quadratic term A 2 、B 2 、C 2 The correlation coefficient R 2 =0.9949, the model fits the actual test to a high degree, and 99.49% of the response value changes can be explained by the fitted model. In addition, after precise correction, the coefficient of determination R 2 Adj reached 0.9882, which is consistent with R 2 The values ​​of are quite similar, which shows that the model has extremely high accuracy and versatility. In summary, it can be seen that the regression equation obtained after analyzing the experimental data can be applied to the analysis and prediction of the yield of paeonol extracted from peony bark by steam distillation.

[0109] (3) The influence of liquid-to-material ratio, distillation time and raw material particle size on the interaction was analyzed by regression model, and response surface diagram and contour map were drawn. Figure 6-Figure 8 The significance of the influence of each factor on the response value and the strength of the interaction between the factors can be judged by the change trend of the three-dimensional graph surface and the shape of the contour line. Figure 6-8 The slopes of the response surface shown are relatively gentle, so the effects of the distillation time, raw material particle size and liquid-to-material ratio on the extraction rate of paeonol are not significant. The change rate of the height of the contour map shows that the effect of raw material particle size and distillation time on the extraction rate of paeonol is greater than the effect of liquid-to-material ratio on the extraction rate.

[0110] (4) Verification of the optimal extraction process: Design Expert 13.0 software optimized and predicted the final experimental data, and the optimal parameters of the process formula were obtained as follows: solid-liquid ratio (g / mL) of 1:17.291, distillation time of 2.797h, and raw material particle size of 0.158cm. Under these conditions, the theoretical extraction rate of paeonol was 1.136%. Taking into account the actual situation, the above conditions were modified, and the final optimized conditions were: solid-liquid ratio (g / mL) of 1:17.5, distillation time of 2.8h, and raw material particle size of 0.15cm. Three parallel experiments were carried out under these conditions, and the actual extraction rate of paeonol was 1.138%, which was close to the theoretical predicted value, indicating that the optimization area obtained by contour superposition of the quadratic polynomial mathematical model meets the design goal.

[0111] Determination of paeonol content and structure:

[0112] (1) Paeonol extracted under the optimal process conditions was selected for subsequent determination.

[0113] (2) A UV-visible spectrophotometer is usually used to verify whether a sample contains paeonol. In this process, the sample solution is transferred to a UV absorption cell and then scanned by the instrument. By observing the absorption spectrum of the sample, a characteristic absorption peak of paeonol is found at 274nm. The experimental results are compared with the UV absorption spectrum of known paeonol to confirm that the absorption peak of the sample is consistent with the standard paeonol absorption spectrum, thereby proving the presence of paeonol in the sample.

[0114] (3) Liquid chromatography:

[0115] Pretreatment: Weigh 5 mg of sample to 25 mL, mix well, filter through 0.22 μm microporous membrane, and measure on the instrument.

[0116] Chromatographic conditions: chromatographic column: C18 column (250 mm × 4.6 mm, 5 μm); mobile phase: methanol: water (40:60, V / V); detection wavelength: 274 nm; flow rate: 1.2 mL / min; injection volume: 10 μL; column temperature: 25 ° C; detector: DAD detector.

[0117] Calculation formula:

[0118] The paeonol content was calculated according to the formula:

[0119]

[0120] Where:

[0121] W——the content of target substance in the sample, in g / 100g;

[0122] C——the concentration of the target substance in the sample solution, in mg / L;

[0123] C0——the concentration of target substance in blank control, in mg / L;

[0124] V——constant volume, unit: mL;

[0125] N——dilution multiple;

[0126] m——the sampling volume of the test sample, in mL.

[0127] Experimental results: The liquid chromatography spectra of paeonol sample and standard are as follows: Figure 9 As shown, the test results show that the sample contains paeonol, which is consistent with the UV results. Through calculation, it can be concluded that the purity of paeonol in the tested sample is 99.57%.

[0128] (4) Fourier transform infrared spectroscopy (ATR): The prepared paeonol was identified by infrared spectroscopy, such as Figure 10 Compared with the standard spectrum, the spectrum Figure 1 In the infrared spectrum, 4000-1500 cm -1 The region is the characteristic frequency region, >1500cm -1 In the spectrum of paeonol, 1375.22 cm -1 The absorption peak at 1508.50cm is produced by the symmetrical bending vibration of -CH3; -1 and 1206.20cm -1 The peak at is caused by the vibration of the aromatic C=C double bond of paeonol and the para-substituted benzene ring, which is consistent with the structural characteristics of paeonol.

[0129] (5) X-ray diffraction (XRD): XRD analysis was performed using an X-ray diffractometer. The sample powder was tightly packed in a rectangular aluminum cell and exposed to an X-ray beam. The scanning area of ​​the diffraction angle 2θ was 5-40°. Figure 11 As shown, paeonol has obvious diffraction peaks at 2θ diffraction angles of 11.80°, 16.48°, 21.06°, 23.66°, 24.30°, 25.64°, and 27.42°, indicating that paeonol is a crystalline material.

[0130] Morphological determination of paeonol:

[0131] (1) Paeonol extracted under the optimal process conditions was selected for subsequent determination.

[0132] (2) Optical microscope: Use an Industrial Digital Camera to observe the sample morphology. Place the sample on a glass slide and add a few drops of distilled water to disperse the sample. Eyepiece 10× / 20, objective lens 10× / 0.25. Figure 12 It can be seen that paeonol is needle-shaped crystals.

[0133] (3) Scanning electron microscope: Figure 13 These are pictures of paeonol under a scanning electron microscope. Through the pictures under the microscope at different magnifications, it can be observed that paeonol is a needle-shaped crystal. When magnified to a certain extent, many loose holes can be observed on the paeonol crystals. This may be because paeonol evaporates slightly during the storage and measurement process.

[0134] Example 2: Method for extracting high-purity paeonol by steam distillation and application of paeonol in preparing toothpaste

[0135] (1) Method for extracting high-purity paeonol using steam distillation

[0136] The method for extracting high-purity paeonol by steam distillation in this experimental example comprises the following steps:

[0137] (1) Take an appropriate amount of clean and disease-free dry peony bark, grind it with a high-speed grinder, and pass it through an 80-mesh sieve. Weigh 100 g of the sieved peony bark powder, 90 g of sodium chloride, and 1800 mL of distilled water. First dissolve the sodium chloride in distilled water, then mix the peony bark powder and the sodium chloride aqueous solution in a distillation flask and soak them at room temperature for 20 h.

[0138] (2) Add enough distilled water to the sandwich U-shaped tube 19 so that the liquid level at the left end of the sandwich U-shaped tube 19 is flush with the water outlet at the right end, and then press Figure 1 Connect the distillation apparatus as shown.

[0139] (3) Turn on the distillation heater 1, and at the same time, open the water inlet and outlet of the condenser tube 9 and the interlayer U-shaped tube 19, set the distillation temperature to 100°C, the condensed water temperature of the condenser tube 9 to 60°C, and the condensed water temperature of the interlayer U-shaped tube 19 to 58°C, heat the distillation for 2.6 hours, and collect all the distillate after the distillation is completed.

[0140] (4) The distillate is cooled to 40°C at room temperature and then transferred into a jacketed crystallizer for cooling crystallization according to the set cooling rate curve, such as Figure 2 As shown, the temperature was lowered for 20 h and the distillate dropped to 4°C.

[0141] (5) The distillate after cooling and crystallization was filtered to obtain white needle-shaped paeonol crystals, which were dried at room temperature to constant weight. The obtained paeonol needle-shaped crystals were white to slightly yellow in color and slightly bitter in taste. The weight was 1.081 g, the extraction rate was 1.081%, and the purity was 99.36%.

[0142]

[0143] Where ω is the extraction rate of paeonol; m 原 is the mass of the raw material, which is 100g; m 产 It is the mass of extracted paeonol.

[0144] The determination method of paeonol is the same as that in Example 1.

[0145] (2) Application of large-particle, high-purity paeonol in the preparation of toothpaste

[0146] The application of the paeonol prepared in this embodiment in preparing toothpaste comprises the following steps:

[0147] (1) 13 g of glycerol, 0.9 g of menthol and 1.5 g of sodium carboxymethyl cellulose (CMC) were mixed to obtain glue A.

[0148] (2) 0.4 g of methylparaben was added to 25 g of water, heated to 80°C for full dissolution for 5 min, cooled to 50°C, and 0.5 g of xylitol, 0.25 g of saccharin, 10 g of sorbitol, 2 g of sodium lauryl sulfate, 0.5 g of sodium N-lauroyl sarcosinate, 0.5 g of Xanthoceras sorbifolia oil, and 0.3 g of paeonol were added to obtain aqueous solution B.

[0149] (3) Mix the glue solution A with the aqueous solution B, stir at 50°C for 10 minutes, and obtain solution C.

[0150] (4) 41 g of calcium hydrogen phosphate dihydrate powder and 6 g of hydrated silica were added to liquid C to prepare a toothpaste mixture. The mixture was stirred at a low speed (200 rpm) for 15 min using a toothpaste vacuum mixer. The vacuum was then turned on and the vacuum degree was controlled to 0.06 MPa. The mixture was stirred and homogenized for 10 min to obtain a toothpaste paste.

[0151] (5) The toothpaste paste was centrifuged and degassed at 3000 rpm for 10 min and then transferred to an aging tank. The toothpaste paste was aged for 120 min to cool to room temperature before packaging.

[0152] (6) The toothpaste efficacy determination method was the same as in Example 1, and the determination results were not significantly different from those in Example 1.

[0153] Example 3: Method for extracting high-purity paeonol by steam distillation and application of paeonol in preparing toothpaste

[0154] (1) Method for extracting high-purity paeonol using steam distillation

[0155] The method for extracting high-purity paeonol by steam distillation in this experimental example comprises the following steps:

[0156] (1) Take an appropriate amount of clean and disease-free dry peony bark, grind it with a high-speed grinder, and pass it through a 100-mesh sieve. Weigh 100 g of the sieved peony bark powder, 90 g of sodium chloride, and 1500 mL of distilled water. First, dissolve the sodium chloride in distilled water. Then, mix the peony bark powder and the sodium chloride aqueous solution in a distillation flask and soak them at room temperature for 24 h.

[0157] (2) Add enough distilled water to the sandwich U-shaped tube 19 so that the liquid level at the left end of the sandwich U-shaped tube 19 is flush with the water outlet at the right end, and then press Figure 1 Connect the distillation apparatus as shown.

[0158] (3) Turn on the distillation heater 1, and at the same time, open the water inlet and outlet of the condenser tube 9 and the interlayer U-shaped tube 19, set the distillation temperature to 100°C, the condensed water temperature of the condenser tube 9 to 62°C, and the condensed water temperature of the interlayer U-shaped tube 19 to 56°C, heat the distillation for 2.5 hours, and collect all the distillate after the distillation is completed.

[0159] (4) The distillate is cooled to 40°C at room temperature and then transferred into a jacketed crystallizer for cooling crystallization according to the set cooling rate curve, such as Figure 2 As shown, the temperature was lowered for 24 h and the distillate dropped to 2°C.

[0160] (5) The distillate after cooling and crystallization was filtered to obtain white needle-shaped paeonol crystals, which were dried at room temperature to constant weight to obtain paeonol needle-shaped crystals. The color was white to slightly yellow, and the taste was slightly bitter. The weight was 1.131 g, the extraction rate was 1.131%, and the purity was 99.87%.

[0161]

[0162] Where ω is the extraction rate of paeonol; m 原 is the mass of the raw material, which is 100g; m 产 It is the mass of extracted paeonol.

[0163] The determination method of paeonol is the same as that in Example 1.

[0164] (2) Application of large-particle, high-purity paeonol in the preparation of toothpaste

[0165] The application of the paeonol prepared in this embodiment in preparing toothpaste comprises the following steps:

[0166] (1) Glue A was prepared by mixing 14 g of glycerol, 0.8 g of menthol, 1.5 g of sodium carboxymethyl cellulose (CMC), and 0.5 g of sodium hydroxyethyl cellulose (HEC).

[0167] (2) 0.5 g of methylparaben was added to 24 g of water, heated to 85°C for full dissolution for 5 min, cooled to 55°C, and 0.35 g of xylitol, 0.25 g of saccharin, 11 g of sorbitol, 2.5 g of sodium lauryl sulfate, 0.6 g of Xanthoceras sorbifolia oil, and 0.4 g of paeonol were added to obtain aqueous solution B.

[0168] (3) Mix the glue solution A with the aqueous solution B, stir at 55°C for 10 min, and obtain solution C.

[0169] (4) Add 47 g of calcium hydrogen phosphate dihydrate powder to liquid C to prepare a toothpaste mixture. After stirring the mixture at a low speed (200 rpm) for 15 min using a toothpaste vacuum mixer, turn on the vacuum and control the vacuum degree to 0.06 MPa. Continue stirring and homogenizing for 10 min to obtain a toothpaste paste.

[0170] (5) The toothpaste paste was centrifuged and degassed at 3000 rpm for 10 min and then transferred to an aging tank. The toothpaste paste was aged for 120 min to cool to room temperature before packaging.

[0171] (6) The toothpaste efficacy determination method was the same as in Example 1, and the determination results were not significantly different from those in Example 1.

[0172] Example 4: Method for extracting high-purity paeonol by steam distillation and application of paeonol in preparing toothpaste

[0173] (1) Method for extracting high-purity paeonol using steam distillation

[0174] The method for extracting high-purity paeonol by steam distillation in this experimental example comprises the following steps:

[0175] (1) Take an appropriate amount of clean and disease-free dry peony bark, grind it with a high-speed grinder, and pass it through a 90-mesh sieve. Weigh 100 g of the sieved peony bark powder, 100 g of sodium chloride, and 2000 mL of distilled water. First, dissolve the sodium chloride in the distilled water. Then, mix the peony bark powder and the sodium chloride aqueous solution in a distillation flask and soak them at room temperature for 24 h.

[0176] (2) Add enough distilled water to the sandwich U-shaped tube 19 so that the liquid level at the left end of the sandwich U-shaped tube 19 is flush with the water outlet at the right end, and then press Figure 1 Connect the distillation apparatus as shown.

[0177] (3) Turn on the distillation heater 1, and at the same time, open the water inlet and outlet of the condenser tube 9 and the interlayer U-shaped tube 19, set the distillation temperature to 102°C, the condensed water temperature of the condenser tube 9 to 62°C, and the condensed water temperature of the interlayer U-shaped tube 19 to 58°C, and heat the distillation for 2.8 hours. After the distillation is completed, collect all the distillates.

[0178] (4) The distillate is cooled to 40°C at room temperature and then transferred into a jacketed crystallizer for cooling crystallization according to the set cooling rate curve, such as Figure 2 As shown, the temperature was lowered for 24 h and the distillate dropped to 2°C.

[0179] (5) The distillate after cooling and crystallization was filtered to obtain white needle-shaped paeonol crystals, which were dried at room temperature to constant weight to obtain paeonol needle-shaped crystals. The color was white to slightly yellow, and the taste was slightly bitter. The weight was 1.136 g, the extraction rate was 1.136%, and the purity was 99.48%.

[0180]

[0181] Where ω is the extraction rate of paeonol; m 原 is the mass of the raw material, which is 100g; m 产 It is the mass of extracted paeonol.

[0182] The determination method of paeonol is the same as that in Example 1.

[0183] (2) Application of large-particle, high-purity paeonol in the preparation of toothpaste

[0184] The application of the paeonol prepared in this embodiment in preparing toothpaste comprises the following steps:

[0185] (1) 13 g of glycerol, 0.5 g of menthol, 1.5 g of sodium carboxymethyl cellulose (CMC), and 0.8 g of sodium hydroxyethyl cellulose (HEC) were mixed to obtain glue A;

[0186] (2) 0.4 g of methylparaben was added to 22 g of water, heated to 85°C for full dissolution for 5 min, cooled to 55°C, and 0.35 g of xylitol, 0.25 g of saccharin, 12 g of sorbitol, 1.5 g of sodium lauryl sulfate, 1 g of sodium N-lauroyl sarcosinate, 0.7 g of Xanthoceras sorbifolia oil, and 0.4 g of paeonol were added to obtain aqueous solution B.

[0187] (3) Mix the glue solution A with the aqueous solution B, stir at 55°C for 10 min, and obtain solution C.

[0188] (4) Add 42 g of powdered calcium hydrogen phosphate dihydrate and 3 g of hydrated silica to liquid C to prepare a toothpaste mixture. After stirring the mixture at a low speed (200 rpm) for 15 min using a toothpaste vacuum mixer, the vacuum is turned on and the vacuum is controlled to 0.06 MPa. Stirring and homogenization are continued for 10 min to obtain a toothpaste paste.

[0189] (5) The toothpaste paste was centrifuged and degassed at 3000 rpm for 10 min and then transferred to an aging tank. The toothpaste paste was aged for 120 min to cool to room temperature before packaging.

[0190] (6) The toothpaste efficacy determination method was the same as in Example 1, and the determination results were not significantly different from those in Example 1.

[0191] Example 5: Method for extracting high-purity paeonol by steam distillation and application of paeonol in preparing toothpaste

[0192] (1) Method for extracting high-purity paeonol using steam distillation

[0193] The method for extracting high-purity paeonol by steam distillation in this experimental example comprises the following steps:

[0194] (1) Take an appropriate amount of clean and disease-free dry peony bark, grind it with a high-speed grinder, and pass it through a 90-mesh sieve. Weigh 100 g of the sieved peony bark powder, 70 g of sodium chloride, and 1750 mL of distilled water. First, dissolve the sodium chloride in distilled water. Then, mix the peony bark powder and the sodium chloride aqueous solution in a distillation flask and soak them at room temperature for 24 h.

[0195] (2) Add enough distilled water to the sandwich U-shaped tube 19 so that the liquid level at the left end of the sandwich U-shaped tube 19 is flush with the water outlet at the right end, and then press Figure 1 Connect the distillation apparatus as shown.

[0196] (3) Turn on the distillation heater 1, and at the same time, open the water inlet and outlet of the condenser 9 and the interlayer U-shaped tube 19, set the distillation temperature to 102°C, the condensed water temperature of the condenser to 62°C, and the condensed water temperature of the interlayer U-shaped tube 19 to 55°C, and heat the distillation for 2.8 hours. After the distillation is completed, collect all the distillates.

[0197] (4) The distillate is cooled to 40°C at room temperature and then transferred into a jacketed crystallizer for cooling crystallization according to the set cooling rate curve, such as Figure 2 As shown, the temperature was lowered for 20 h and the distillate dropped to 4°C.

[0198] (5) The distillate after cooling and crystallization was filtered to obtain white needle-shaped paeonol crystals, which were dried at room temperature to constant weight. The obtained paeonol needle-shaped crystals were white to slightly yellow in color and slightly bitter in taste. The weight was 1.141 g, the extraction rate was 1.141%, and the purity was 99.91%.

[0199]

[0200] Where ω is the extraction rate of paeonol; m 原 is the mass of the raw material, which is 100g; m 产 It is the mass of extracted paeonol.

[0201] The determination method of paeonol is the same as that in Example 1.

[0202] (2) Application of large-particle, high-purity paeonol in the preparation of toothpaste

[0203] The application of the paeonol prepared in this embodiment in preparing toothpaste comprises the following steps:

[0204] (1) Mix 13 g of glycerol, 1 g of menthol, and 2.5 g of sodium carboxymethyl cellulose (CMC) to obtain glue A.

[0205] (2) 0.5 g of methylparaben was added to 25 g of water, heated to 85 ° C for full dissolution for 5 min, cooled to 55 ° C, and 0.45 g of xylitol, 0.15 g of saccharin, 12 g of sorbitol, 2.0 g of sodium lauryl sulfate, 0.5 g of sodium N-lauroyl sarcosinate, 0.8 g of Xanthoceras sorbifolia oil and 0.5 g of paeonol were added to obtain aqueous solution B.

[0206] (3) Mix glue solution A with aqueous solution B, stir at 55°C for 10 min, and obtain solution C;

[0207] (4) 40 g of powdered calcium hydrogen phosphate dihydrate and 5 g of hydrated silica were added to liquid C to prepare a toothpaste mixture. The mixture was stirred at a low speed (200 rpm) for 15 min using a toothpaste vacuum mixer. The vacuum was then turned on and the vacuum degree was controlled to 0.06 MPa. The mixture was stirred and homogenized for 10 min to obtain a toothpaste paste.

[0208] (5) The toothpaste paste was centrifuged and degassed at 3000 rpm for 10 min and then transferred to an aging tank. The toothpaste paste was aged for 120 min to cool to room temperature before packaging.

[0209] (6) The toothpaste efficacy determination method was the same as in Example 1, and the determination results were not significantly different from those in Example 1.

[0210] The above specific embodiments do not limit the scope of protection of the present invention. Those skilled in the art will appreciate that various modifications, combinations, sub-combinations, and substitutions may occur depending on design requirements and other factors. Any modifications, equivalent substitutions, and improvements made within the spirit and principles of the present invention are intended to be included within the scope of protection of the present invention.

Claims

1. A method for preparing paeonol crystals from peony bark, comprising the following steps: (1) mixing the crushed peony bark and a sodium chloride aqueous solution in a distillation flask of a distillation apparatus to uniformly soak the peony bark; (2) Connect the distillation apparatus, turn on the heater, and simultaneously open the water inlet and outlet of the condenser and the interlayer U-shaped tube. Set the distillation temperature, the condensed water temperature of the condenser, and the condensed water temperature of the interlayer U-shaped tube. Heat and distill. After the distillation is completed, collect the distillate. (3) subjecting the distillate to cooling crystallization; (4) filtering the distillate after the crystallization by cooling to obtain white needle-shaped crystals, and drying the crystals to obtain paeonol crystals; The distillation device comprises a heater (1), a distillation flask (2), a thermometer (3), a first curved pipe (6), a condenser (9), a second curved pipe (12), a sandwich U-shaped pipe (19), and a third curved pipe (23); wherein, The top opening of the distillation flask (2) is sealedly connected to the first end (5) of the first curved pipe; the second end (8) of the first curved pipe is sealedly connected to the first end (16) of the condenser pipe; the second end (17) of the condenser pipe is sealedly connected to the first end (11) of the second curved pipe; the second end (13) of the second curved pipe is sealedly connected to the first end of the interlayer U-shaped pipe (19); and the second end of the interlayer U-shaped pipe (19) is sealedly connected to the first end (22) of the third curved pipe.

2. The method for preparing paeonol crystals from Paeonia suffruticosa moutan according to claim 1, wherein: In the step (1), the crushed peony bark is peony bark powder that has passed through an 80-100 mesh sieve; the mass percentage concentration of the sodium chloride aqueous solution is 4%-6%; the material-liquid ratio of the peony bark to the sodium chloride aqueous solution is 1g / 10mL-1g / 20mL; and the soaking time is 18h-24h.

3. The method for preparing paeonol crystals from Paeonia suffruticosa moutan according to claim 1, wherein: The distillation temperature is 100°C-102°C; the condensed water temperature of the condenser is 60°C-62°C; the condensed water temperature of the interlayer U-shaped tube is 55°C-58°C, and the heating distillation time is 2.5h-2.8h.

4. The method for preparing paeonol crystals from Paeonia suffruticosa moutan according to claim 1, wherein: The distillate in step (3) is a distillate at 35°C-40°C; the cooling crystallization is performed by cooling the temperature to 2°C-4°C for 20h-24h according to the cooling rate curve.

5. The method for preparing paeonol crystals from Paeonia suffruticosa moutan according to claim 1, wherein: The conditions for the filtration in step (4) are a temperature of 20-25°C and a pressure of 0.04-0.06 MPa; the drying temperature is 20-25°C.

6. Paeonol crystals from the cortex moutan prepared by the method according to any one of claims 1 to 5.

7. A toothpaste comprising the following ingredients in parts by weight: 0.3-0.5 parts of the paeonol crystals of claim 6, 45-50 parts of an abrasive, 1.5-2.5 parts of a foaming agent, 1.5-2.5 parts of a thickener, 20-25 parts of a moisturizing agent, 0.5-1.0 parts of a flavoring agent, 0.2-0.5 parts of xylitol, 0.3-0.5 parts of methylparaben, 0.4-0.8 parts of Xanthoceras sorbifolia oil, and the remainder being water; The paeonol crystals are effective anti-inflammatory factors; the abrasive is composed of calcium hydrogen phosphate dihydrate and hydrated silica, the foaming agent is composed of sodium lauryl sulfate and sodium N-lauroyl sarcosine, the thickener is composed of sodium carboxymethyl cellulose and sodium hydroxyethyl cellulose, the moisturizer is composed of sorbitol and glycerin, the flavoring agent is menthol, the sweetener is xylitol and edible saccharin, and the preservative is methylparaben.

8. The toothpaste according to claim 7, characterized in that: The mass ratio of the friction agent hydrated silica to dihydrated calcium phosphate is (0-1):(8-9); the mass ratio of the foaming agent sodium N-lauroyl sarcosinate to sodium lauryl sulfate is (0-1):(4-6); the mass ratio of the thickener sodium hydroxyethyl cellulose to sodium carboxymethyl cellulose is (0-1):(3-5); and the mass ratio of the moisturizing agent sorbitol to glycerin is 1:(1.0-1.2).

9. The toothpaste according to claim 8, characterized in that: The toothpaste is made from the following ingredients by weight: 0.3-0.5 parts of the paeonol crystals according to claim 6, 40-42 parts of calcium hydrogen phosphate dihydrate, 3-5 parts of hydrated silica, 1.5-2.0 parts of sodium lauryl sulfate, 0.5-1.0 parts of sodium N-lauroyl sarcosinate, 1.5-2.0 parts of sodium carboxymethyl cellulose, 0.4-0.8 parts of sodium hydroxyethyl cellulose, 10-12 parts of sorbitol, 10-13 parts of glycerol, 0.2-0.5 parts of xylitol, 0.5-1.0 parts of menthol, 0.3-0.5 parts of methylparaben, 0.4-0.8 parts of Xanthoceras sorbifolia oil and 20-25 parts of water.

10. The method for preparing the toothpaste according to any one of claims 7 to 9, comprising the steps of: (1) Glycerin, Xanthoceras sorbifolia oil, menthol and sodium carboxymethyl cellulose are mixed to obtain glue A; (2) adding methylparaben to water, heating to 80-85°C to fully dissolve for 3-5 minutes, cooling to 50-55°C, adding xylitol, sorbitol, sodium lauryl sulfate, sodium N-lauroyl sarcosinate and paeonol crystals to obtain aqueous solution B; (3) mixing the glue solution A with the aqueous solution B, stirring at 50-55° C. for 5-10 minutes to obtain solution C; (4) Adding powdered calcium hydrogen phosphate dihydrate and hydrated silica to the liquid C to prepare toothpaste.

Images