Jinhuang powder hydrogel as well as preparation method and application thereof

Abstract

The invention relates to the technical field of medical treatment, in particular to golden yellow powder hydrogel which is prepared from polyvinyl alcohol, cellulose and / or cellulose derivatives, polyphenol compounds, golden yellow powder alcohol extract and water. The mass ratio of the polyvinyl alcohol to the cellulose and / or the cellulose derivative is regulated to be (20-40): 1, the mass of the polyphenol compound accounts for 1-10% of the total mass of the polyvinyl alcohol and the carboxymethyl cellulose, the raw materials further comprise glycerol, and the mass ratio of the glycerol to the polyvinyl alcohol is 1: (0.2-1); the preparation method is further optimized, so that the prepared hydrogel material has excellent mechanical performance, self-repairing performance, drug loading capacity, transdermal performance, air permeability and adhesion; when being used as a dressing, the ointment has good compatibility and affinity with skin, is easy to uncover and paste, and has no skin irritation and residue.

Description

Technical Field

[0001] The present invention relates to the field of medical technology, A61L15 / 22, and particularly relates to a golden powder hydrogel, a preparation method thereof, and an application thereof. Background Art

[0002] Ruyi Jinhuang Powder originated from a classic traditional Chinese medicine compound preparation in "Orthodox Manual of Surgery" by Chen Shigong in the Ming Dynasty. Long-term clinical applications have proven its definite curative effect and safe medication. It has active ingredients for clearing heat and detoxifying, and detumescence and pain relief, and has a good preventive and therapeutic effect on boils with local redness, swelling, heat, and pain caused by bacterial acute suppurative infections. Currently, this prescription is mostly stored or used in the form of powders or ointments. However, the powder is prone to moisture when stored for a long time, inconvenient to use, inaccurate in dosage, low in transdermal absorption rate, and slow in taking effect; the ointment contains sesame oil, petrolatum, etc., making it have a strong greasy feeling and a strong smell, resulting in low patient compliance in taking medicine.

[0003] Chinese Patent CN219148653U discloses a novel golden powder nano-silver antibacterial dressing. The internal structure of the dressing sequentially includes a backing layer, a silver ion fiber textile layer, a plaster layer, and a medicine-sealing layer. The plaster layer includes Ruyi Jinhuang Powder and honey. Although the method uses a medicine-sealing layer to fix the plaster layer and solves the sticky skin feeling caused by the use of honey, the dressing has too high viscosity and strong skin irritation when torn off. Chinese Patent CN102362914B discloses a traditional Chinese medicine gel for preventing and treating phlebitis. This patent encapsulates traditional Chinese medicine components in a hydrophilic gel matrix material, avoiding the problem of airtightness of traditional ointments. However, the use method of this hydrogel is still smearing, and it still has problems of inconvenient use and greasy skin feeling.

[0004] Therefore, it is of great significance to prepare a golden powder dosage form with a large drug loading capacity, good moisturizing property, good skin compatibility and affinity, easy to peel off, no skin irritation and residue, accurate dosage, convenient to use, which can significantly improve patient compliance, and high transdermal rate for use. Summary of the Invention

[0005] To solve the above technical problems, the present invention first provides a golden powder hydrogel. The preparation raw materials of the hydrogel include: polyvinyl alcohol, cellulose and / or cellulose derivatives, polyphenolic compounds, golden powder ethanol extract, and water.

[0006] Further, by mass, the preparation raw materials of the hydrogel include: 1-45 parts of polyvinyl alcohol, 0.05-10 parts of cellulose and / or cellulose derivatives, 0.05-4 parts of polyphenolic compounds, 5-90 parts of golden powder ethanol extract, and 20-300 parts of water.

[0007] Preferably, by mass parts, the raw materials for preparing the hydrogel include: 3-10 parts of polyvinyl alcohol, 0.1-1 part of cellulose and / or cellulose derivative, 0.1-3 parts of polyphenolic compound, 20-60 parts of ethanol extract of Jinhuang Powder, and 50-200 parts of water.

[0008] Furthermore, the cellulose and / or cellulose derivative includes but is not limited to at least one of cellulose, carboxymethyl cellulose, sodium carboxymethyl cellulose, and sodium hydroxypropyl methyl cellulose.

[0009] Preferably, the cellulose and / or cellulose derivative includes carboxymethyl cellulose and / or sodium carboxymethyl cellulose.

[0010] Furthermore, the mass ratio of the polyvinyl alcohol to the cellulose and / or cellulose derivative is (20-40):1.

[0011] In this application, polyvinyl alcohol has a flexible molecular chain, rich hydrophilic side groups, and good biocompatibility, but the gel mechanical strength is insufficient when used to make hydrogels. Carboxymethyl cellulose is used in combination, and a cyclic rigid structure is doped in the flexible structure of polyvinyl alcohol to enhance the mechanical strength of the hydrogel network. It should be noted that due to intermolecular forces such as hydrogen bonds and electrostatic interactions, some drug components will be adsorbed on the surface of the hydrogel skeleton structure, and another part of the drug will be fixed inside the gel skeleton. Therefore, it is necessary to strictly control the mass ratio of polyvinyl alcohol and carboxymethyl cellulose within a specified range to make the cross-linked structure formed by the two have appropriate rigidity and flexibility and cross-linking degree, and avoid excessive cross-linking degree resulting in difficult migration of drug components inside the gel, thereby reducing the efficacy of the gel patch.

[0012] Further preferably, the mass ratio of the polyvinyl alcohol to the cellulose and / or cellulose derivative is (25-35):1.

[0013] Furthermore, the polyphenolic compound is selected from at least one of gallic acid, propyl gallate, catechin, arbutin, tannic acid, and dopamine.

[0014] Furthermore, the polyphenolic compound is selected from at least one of gallic acid and tannic acid.

[0015] Preferably, the polyphenolic compound is tannic acid.

[0016] The polyphenol group in the molecular structure of tannic acid and the -SH and -NH of polypeptides and proteins on the tissue surface 2There is a strong binding affinity between them. When added to the gel system, it can improve the adhesion of the hydrogel to the skin. In addition, the large number of phenolic groups it contains can participate in the network structure of the hydrogel as the action sites of hydrogen bonds, ionic bonds, and coordination bonds. This reversible physical cross-linking mode endows the hydrogel with good self-healing performance. Finally, tannic acid, as a natural antibacterial small molecule, can also enhance the antioxidant, antibacterial, and antimicrobial effects of the gel patch. However, when the addition amount is too much, the cross-linking effect generated will significantly increase the cohesion of the gel, resulting in problems such as hardening of the gel and a decrease in adhesion performance.

[0017] Furthermore, the mass of the polyphenolic compound accounts for 1-10% of the total amount of polyvinyl alcohol and carboxymethyl cellulose, preferably 3-10%, more preferably 6-10%.

[0018] Furthermore, the preparation method of the ethanol extract of Jinhuang Powder includes the following steps: (1) Take the crushed Magnolia officinalis, Citrus reticulata Blanco, and Atractylodes lancea (Thunb.) DC. and mix them, and steam-distill to extract the volatile oil, which is reserved as phase A; (2) Take the crushed Angelica dahurica (Fisch. ex Hoffm.) Benth. et Hook. f. ex Franch. et Sav., Curcuma longa L., and the medicinal residues left in (1), and perform percolation by the percolation method, collect the percolate, recover the solvent, and concentrate it under reduced pressure to an extract with a relative density of 1.0-1.5 g / mL, which is reserved as phase B; (3) Take the crushed Phellodendron amurense Rupr., Glycyrrhiza uralensis Fisch., Arisaema heterophyllum Blume, and Rheum palmatum L. and decoct them several times, combine the filtrates, and heat-concentrate to an extract density of 1.0-1.5 g / mL, which is reserved as phase C; (4) Add phase A and phase B to phase C and mix evenly to prepare the ethanol extract of Jinhuang Powder.

[0019] Furthermore, in the step (2), the solvent is 50-75 wt% ethanol.

[0020] Furthermore, the raw materials for preparing the Jinhuang Powder hydrogel also include glycerol, and the mass ratio of glycerol to polyvinyl alcohol is 1:(0.2-1).

[0021] Relatively speaking, the addition of glycerol can enhance the uniform dispersion of the medicinal components in the system, and this small molecule substance has higher molecular activity in the gel structure. During the use of the gel, it will carry the drugs inside the gel pores to the gel surface to take effect, enhancing the therapeutic effect of the gel patch and avoiding the waste of drug components. However, when the addition amount is too much, the gel surface will show stickiness.

[0022] Furthermore, the raw materials for preparing the Jinhuang Powder hydrogel also include a penetrant.

[0023] Furthermore, the penetrant includes but is not limited to at least one of azone, borneol, and peppermint oil.

[0024] Preferably, the penetrant includes azone.

[0025] Secondly, the present application also provides a method for preparing a Jinhuang powder hydrogel, which comprises the following steps:

[0026] S1. Dilute polyvinyl alcohol and cellulose and / or cellulose derivatives into solutions with water respectively, and then mix the two evenly;

[0027] S2. Dilute polyphenolic compounds into an aqueous solution with a concentration of 2-10 wt%, and drop it into the solution of S1 and stir;

[0028] S3. Add the ethanol extract of Jinhuang powder to the solution of S2, mix well, remove bubbles by ultrasonic treatment, and pour it into a mold for freeze-thaw cycling.

[0029] Further, the preparation method comprises the following steps:

[0030] S1. Dilute polyvinyl alcohol and cellulose and / or cellulose derivatives into solutions with water respectively, and mix the two evenly;

[0031] S2. Drop an aqueous solution of polyphenolic compounds with a concentration of 2-10 wt% into the solution of S1 and stir;

[0032] S3. Add glycerol, a penetrant, and the ethanol extract of Jinhuang powder to the solution of S2 in sequence, mix well, remove bubbles by ultrasonic treatment, and pour it into a mold for freeze-thaw cycling.

[0033] Further, the freeze-thaw cycling specifically is: freeze at -30 to -10 °C for 12-20 h, thaw at 10 to 40 °C for 2-12 h, and perform freeze-thaw cycling 2-6 times.

[0034] The physical gelation of the system of the present application occurs during the freezing process. At the specified freezing temperature, this freezing rate can not only cause appropriate cross-linking of the specified gel substances, but also make the crystals of the solvent serve as pore-forming agents, enabling the gel to have appropriate pores and pore size distribution. The interconnectivity between pores is improved through multiple freeze-thaw cycles. This three-dimensional interconnected pore structure generated by the combined action of the above factors will endow the gel system with good water-vapor permeability, which is beneficial to wound recovery.

[0035] Further, the freeze-thaw cycling specifically is: freeze at -25 to -12 °C for 14-20 h, thaw at 20 to 30 °C for 4-10 h, and perform freeze-thaw cycling 2-5 times.

[0036] Preferably, the freeze-thaw cycling specifically is: freeze at -20 to -16 °C for 17-20 h, thaw at 20 to 30 °C for 5-8 h, and perform freeze-thaw cycling 3-4 times.

[0037] Finally, the present application also provides the application of the Jinhuang powder hydrogel as a hydrogel dressing.

[0038] Beneficial effects:

[0039] 1. The Jinhuang powder hydrogel of the present application has the advantages of large drug loading capacity, simple preparation process, convenient use, and no clothing pollution, and can become an optimal dosage form for external use of traditional Chinese medicine compound preparations.

[0040] 2. The present application utilizes the elastic molecular chain of polyvinyl alcohol, the rigid supporting framework of carboxymethyl cellulose, and the multiple synergistic effects of tannic acid to enhance the network. By controlling the addition amounts of the above three components, the hydrogel has excellent mechanical properties, self-healing properties, drug loading capacity, and adhesiveness. When used as a poultice, the hydrogel has an excellent adhesion effect on the skin.

[0041] 3. The extract of traditional Chinese medicine compound itself belongs to a complex system with multiple components and a wide range of component polarities. When preparing the alcohol extract of Jinhuang powder in the present application, a water-alcohol double extraction strategy is adopted, which can achieve the full extraction of the effective components of traditional Chinese medicine raw materials.

[0042] 4. On the basis of controlling the raw material components, the present application further optimizes the preparation method of the hydrogel, so that the hydrogel has a good three-dimensional interconnected network structure, enhances the air permeability of the hydrogel, and is beneficial to the recovery of the user's injury;

[0043] 5. The materials of the hydrogel of the present application are all biocompatible and biodegradable materials, with good biocompatibility, biodegradability, relatively high gel strength, and good shape recovery ability. They do not contain any toxic chemical agents and have high potential application value in the fields of medical dressings, etc. The preparation of green and environmentally friendly medical dressings is realized. BRIEF DESCRIPTION OF THE DRAWINGS

[0044] Figure 1 : Scanning electron micrograph of the hydrogel of Example 1;

[0045] Figure 2 : Test pictures of the adhesiveness of the hydrogel patch of Example 1. DETAILED DESCRIPTION OF THE EMBODIMENTS

[0046] EXAMPLES

[0047] Example 1

[0048] This example provides a Jinhuang powder hydrogel; calculated by mass, the raw materials for preparing the hydrogel include: 6 parts of polyvinyl alcohol, 0.2 part of carboxymethyl cellulose, 0.5 part of tannic acid, 30 parts of the alcohol extract of Jinhuang powder, 10 parts of glycerol, 3 parts of azone, and 90 parts of water.

[0049] Further, the preparation method of the ethanol extract of Jinhuang Powder comprises the following steps: (1) Weigh 25 g of Magnolia officinalis, 25 g of Citrus reticulata Blanco, and 25 g of Atractylodes lancea according to the formula amount, mix them after crushing, and extract the volatile oil by steam distillation. The volatile oil is reserved as Phase A; (2) Weigh 62.5 g of Angelica dahurica, 62.5 g of Curcuma longa, and the medicinal residues left in (1), use 70 wt% ethanol as the solvent, perform percolation by the percolation method, collect the percolate, recover the solvent, and concentrate it under reduced pressure to an extract with a relative density of 1.25 as Phase B for standby; (3) Weigh 62.5 g of Phellodendron amurense, 25 g of Glycyrrhiza uralensis Fisch, 25 g of Arisaema heterophyllum Blume, and 62.5 g of Rheum palmatum, decoct twice, combine the filtrates, and heat and concentrate to an extract density of 1.25 g / mL as Phase C for standby; (4) Add Phase A and Phase B to Phase C and mix them evenly to prepare the ethanol extract of Jinhuang Powder.

[0050] This embodiment also provides a preparation method of the Jinhuang Powder hydrogel, which comprises the following steps:

[0051] S1. Put polyvinyl alcohol into 60 parts of water, heat and stir at 90 °C to dilute it into an aqueous polyvinyl alcohol solution; then dilute carboxymethyl cellulose with 20 parts of water into an aqueous carboxymethyl cellulose solution, and mix the two evenly;

[0052] S2. Take tannic acid and add it to 10 parts of water to make a 5 wt% tannic acid aqueous solution, and drop all of it into the solution in S1 and stir for 15 min;

[0053] S3. Add glycerol, azone, and the ethanol extract of Jinhuang Powder to the solution in S2 in sequence, mix well, remove bubbles by ultrasonic treatment, pour it into a mold, freeze at -18 °C for 18 h, thaw at 25 °C for 6 h, and perform freeze-thaw cycling 3 times.

[0054] Example 2

[0055] This embodiment provides a Jinhuang Powder hydrogel; calculated by mass, the raw materials for preparing the hydrogel include: 3 parts of polyvinyl alcohol, 0.12 part of carboxymethyl cellulose, 0.19 part of tannic acid, 20 parts of the ethanol extract of Jinhuang Powder, 15 parts of glycerol, 1.8 parts of azone, and 133.5 parts of water.

[0056] Furthermore, the preparation method of the ethanol extract of Jinhuang Powder comprises the following steps: (1) Weigh 25 g of Magnolia officinalis, 25 g of Citrus reticulata Blanco, and 25 g of Atractylodes lancea according to the formula, mix them after pulverization, and extract the volatile oil by steam distillation. This volatile oil is reserved as Phase A; (2) Weigh 62.5 g of Angelica dahurica, 62.5 g of Curcuma longa, and the medicinal residues left in step (1), perform percolation by the percolation method, collect the percolate, recover the solvent, and concentrate it under reduced pressure to an extract with a relative density of 1.5, which is reserved as Phase B; (3) Weigh 62.5 g of Phellodendron amurense, 25 g of Glycyrrhiza uralensis Fisch., 25 g of Arisaema heterophyllum Blume, and 62.5 g of Rheum palmatum L., decoct twice, combine the filtrates, and concentrate by heating to an extract density of 1.5 g / mL, which is reserved as Phase C; (4) Add Phase A and Phase B to Phase C and mix them evenly to obtain the ethanol extract of Jinhuang Powder.

[0057] This embodiment also provides a preparation method of the Jinhuang Powder hydrogel, which comprises the following steps:

[0058] S1. Put polyvinyl alcohol into 100 parts of water, heat and stir at 90 °C to dilute it into an aqueous polyvinyl alcohol solution; then dilute carboxymethyl cellulose with 24 parts of water into an aqueous carboxymethyl cellulose solution, and mix the two evenly;

[0059] S2. Take tannic acid, add it to 9.5 parts of water to make a 2 wt% tannic acid aqueous solution, and drop all of it into the solution in S1 and stir;

[0060] S3. Add glycerol, azone, and the ethanol extract of Jinhuang Powder to the solution in S2 in sequence, mix well, remove bubbles by ultrasonic treatment, pour it into a mold, freeze at -20 °C for 17 h, thaw at 23 °C for 7 h, and perform freeze-thaw cycling 4 times.

[0061] Example 3

[0062] This embodiment provides a Jinhuang Powder hydrogel; calculated by mass parts, the raw materials for preparing the hydrogel include: 10 parts of polyvinyl alcohol, 0.29 parts of carboxymethyl cellulose, 1.03 parts of tannic acid, 60 parts of the ethanol extract of Jinhuang Powder, 10 parts of glycerol, 4.6 parts of azone, and 69.9 parts of water.

[0063] Further, the preparation method of the ethanol extract of Jinhuang Powder comprises the following steps: (1) Weigh 25 g of Magnolia officinalis, 25 g of Citrus reticulata Blanco, and 25 g of Atractylodes lancea, all in powdered form, mix them, and extract the volatile oil by steam distillation. This volatile oil is reserved as Phase A. (2) Weigh 62.5 g of Angelica dahurica, 62.5 g of Curcuma longa, and the medicinal residues left in (1), and perform percolation by the percolation method. Collect the percolate, recover the solvent, and concentrate it under reduced pressure to an extract with a relative density of 1.0, which is reserved as Phase B. (3) Weigh 62.5 g of Phellodendron amurense, 25 g of Glycyrrhiza uralensis Fisch., 25 g of Arisaema heterophyllum Blume, and 62.5 g of Rheum palmatum L., decoct them twice, combine the filtrates, and heat and concentrate to an extract density of 1.0 g / mL, which is reserved as Phase C. (4) Add Phase A and Phase B to Phase C and mix them evenly to obtain the ethanol extract of Jinhuang Powder.

[0064] This embodiment also provides a preparation method of the Jinhuang Powder hydrogel, which comprises the following steps:

[0065] S1. Put polyvinyl alcohol into 50 parts of water, heat and stir at 90 °C to dilute it into an aqueous polyvinyl alcohol solution; then dilute carboxymethyl cellulose with 9.6 parts of water into an aqueous carboxymethyl cellulose solution, and mix the two evenly.

[0066] S2. Take tannic acid, add it to 10.3 parts of water to make a 10 wt% tannic acid aqueous solution, and drop all of it into the solution in S1 and stir.

[0067] S3. Add glycerol, azone, and the ethanol extract of Jinhuang Powder to the solution in S2 in sequence, mix evenly, remove bubbles by ultrasonic treatment, pour it into a mold, freeze at -16 °C for 20 h, thaw at 26 °C for 5 h, and perform freeze-thaw cycling 4 times.

[0068] Example 4

[0069] It is basically the same as Example 1, except that the amount of tannic acid is 0.74 part.

[0070] Example 5

[0071] It is basically the same as Example 1, except that the amount of tannic acid is 0.06 part.

[0072] Example 6

[0073] It is basically the same as Example 1, except that Step S3 is: Add glycerol, azone, and the ethanol extract of Jinhuang Powder to the solution in S2 in sequence, mix evenly, remove bubbles by ultrasonic treatment, pour it into a mold, freeze at -25 °C for 18 h, thaw at 25 °C for 6 h, and perform freeze-thaw cycling 2 times.

[0074] Example 7

[0075] It is basically the same as Example 1, with the difference that: S3. Glycerol, azone, and ethanol extract of Flos Chrysanthemi Indici were successively added to the solution of S2. After mixing evenly, the bubbles were removed by ultrasonic treatment, and then it was poured into a mold, frozen at -12°C for 20 h, thawed at 25°C for 4 h, and the freeze-thaw cycle was repeated 3 times.

[0076] Comparative Example 1

[0077] It is basically the same as Example 1, with the difference that: 5.8 parts of polyvinyl alcohol and 0.4 parts of carboxymethyl cellulose are used.

[0078] Comparative Example 2

[0079] It is basically the same as Example 1, with the difference that: 0.018 parts of tannic acid are used.

[0080] Comparative Example 3

[0081] It is basically the same as Example 1, with the difference that: 4 parts of glycerol are used.

[0082] Comparative Example 4

[0083] It is basically the same as Example 1, with the difference that: Step S3 is: Glycerol, azone, and ethanol extract of Flos Chrysanthemi Indici were successively added to the solution of S2. After mixing evenly, the bubbles were removed by ultrasonic treatment, and then it was poured into a mold, frozen at -10°C for 18 h, thawed at 25°C for 6 h, and the freeze-thaw cycle was repeated 5 times.

[0084] Performance test method:

[0085] 1. Scanning electron micrograph: Attached Figure 1 is the FE-SEM image of the hydrogel of Example 1, with a magnification of 200 times.

[0086] As can be seen from the figure: The hydrogel presents a porous network structure, with a high porosity, uniform pore distribution and interconnection, forming a unique interpenetrating network structure, which will be beneficial to the exchange of water, gas and some small molecule substances; in addition, there is no obvious phase separation between polyvinyl alcohol and carboxymethyl cellulose in the hydrogel, indicating good compatibility between the two components.

[0087] 2. Adhesion: (1) Method 1: The hydrogel of the example was made into a compound gel plaster with a diameter of 5 cm and placed on the back of the experimenter's hand. The gel formed a seamless adhesion with the plane of the rubber glove. It was continuously flipped 180° 10 times to observe whether it could not fall off under its own weight, and the adhesion performance was judged; The adhesion test pictures of Example 1 are shown in the attachment Figure 2; (2) Method 2: The hydrogel sample film was made into a size of 15 mm (length) × 10 mm (width) × 1 mm (thickness), placed between two pieces of porcine skin tissue, and then subjected to a gentle pressure of 10 s (200 g weight) to achieve adhesion. Under a loading speed of 10 mm / min, a lap shear test was carried out using a 500 N load cell. The adhesion strength (kPa) was calculated as the maximum load (kN) divided by the area (m 2 ). The statistical results of the examples and comparative examples are shown in Table 1.

[0088] 3. Compression modulus: The Huangjin San hydrogels of the examples and comparative examples were made into cylinders with a height of 10 mm and a diameter of 15 mm for compression tests (during non-test time, the specimens were stored in a sealed container to avoid long-term contact with air; before testing, the specimens were taken out and placed in the test fixture). The prepared hydrogel was subjected to a compression test on a universal testing machine equipped with a 1 kN loading box. The preloading force was set to 0.005 N (the initial load before starting compression), and the test was started at a loading rate of 5 mm / min. The specimen was compressed to 60% strain, that is, a stroke of 6 mm. During the test, a load sensor and a displacement sensor were used to obtain load and displacement data to ensure the accuracy and consistency of the data. All experiments were carried out at 25 °C, and the samples were kept moist during the test. The compression modulus (E) of the specimen was calculated according to the results; the calculation formula is as follows: E = σ / ε. Where, σ is the stress (N) and ε is the stress area (m 2 ). The statistical results of the examples and comparative examples are shown in Table 1.

[0089] 4. In vitro transdermal experiment: The prepared mouse skin was fixed between the supply chamber and the receiving chamber of a double-chamber diffusion cell (the cross-sectional area of the skin is 3.14 cm 2 ), so that the dermal layer of the mouse skin was in contact with the receiving solution, that is, the dermal layer was facing down; the stratum corneum was in contact with the supply solution, and the stratum corneum was facing up. PBS buffer solution with pH = 7.0 was added to the receiving chamber (19.0 mL as the receiving solution, and then placed on a magnetic stirrer that rotates at a constant temperature and speed (maintaining a constant temperature of 32 °C and a constant speed of 300 r / min for stirring). The golden composite hydrogels of each group were closely attached to the mouse skin.

[0090] Samples of 1 mL were taken at the time points of 4 h, 8 h, 12 h, 24 h, and 36 h respectively, and an equal volume of fresh PBS receiving solution was added in time. After filtering the samples with a 0.22 μm microporous membrane, they were injected into an HPLC chromatograph to measure their peak areas and calculate the drug concentration, and the cumulative permeability per unit area was calculated: K = [Q / m] × 100%. Where, Q is the cumulative permeation amount per unit area, m is the amount of the active ingredient berberine hydrochloride in 1 g of the gel. The drug concentrations (μg / mL) measured at the nth and ith sampling points are represented by Cn and Ci respectively. The volume of the receiving cell and the sampling volume (mL) are represented by V and V0 respectively. The effective permeation area (cm 2 ) is represented by A. The statistical results of the examples and comparative examples are shown in Table 2.

[0091] Performance test results:

[0092] Table 1

[0093]

[0094] Table 2

[0095]

[0096]

[0097] Result: The golden powder hydrogel prepared by the technical solutions of Examples 1 - 3 has excellent three-dimensional network pore structure, adhesiveness and transdermal permeability.

[0098] Comparing Comparative Example 1 with Comparative Example 1, it can be seen that when the content of carboxymethyl cellulose increases, the mechanical properties of the hydrogel can be improved by increasing the crosslinking strength of the hydrogel. However, when the content is too high, it will lead to a decrease in the transdermal permeability of the hydrogel, which is not conducive to the release of the internal drug and will also reduce the adhesiveness.

[0099] Comparing Comparative Example 1 with Examples 4 - 5 and Comparative Example 2, it can be seen that the use of tannic acid will increase the adhesion performance of the hydrogel. However, when the dosage exceeds the specified value, it will lead to too high crosslinking strength inside the hydrogel, which will instead reduce both the adhesiveness and transdermal permeability of the hydrogel.

[0100] Comparing Comparative Example 1 with Examples 6 - 7 and Comparative Example 4, it can be seen that the adhesion effect of Examples 6 - 7 is poor, and the release amount of Comparative Example 4 is too high in a short time, and the long-term sustained release effect cannot be achieved. It shows that only appropriate freeze-thaw temperature can make the gel system have appropriate crosslinking speed and degree, and have excellent pore structure and pore distribution inside, so as to improve the transdermal permeability, air permeability and sustained release effect.

[0101] Comparing Examples 1 - 3 with Comparative Example 3, it can be seen that when the addition amount of glycerol is too small, it is not conducive to the migration of the drug in the network structure to the gel surface, resulting in a decrease in transdermal permeability.

Claims

1. A golden powder hydrogel, characterized in that the raw materials for preparing the hydrogel include: polyvinyl alcohol, cellulose and / or cellulose derivatives, polyphenolic compounds, ethanol extract of golden powder, and water; the mass ratio of polyvinyl alcohol to cellulose and / or cellulose derivatives is (20 - 40):

1.

2. The hydrogel according to claim 1, characterized in that the mass ratio of polyvinyl alcohol to cellulose and / or cellulose derivatives is (25 - 35):

1.

3. The hydrogel according to claim 1, characterized in that the polyphenolic compounds are selected from at least one of gallic acid, propyl gallate, catechin, arbutin, tannic acid, and dopamine.

4. The hydrogel according to claim 1, characterized in that the mass of the polyphenolic compounds accounts for 1 - 10% of the total amount of polyvinyl alcohol and carboxymethyl cellulose, preferably 3 - 10%.

5. The hydrogel according to claim 1, characterized in that the preparation method of the ethanol extract of golden powder includes the following steps: (1) Take the crushed magnolia officinalis, citrus reticulata peel, and atractylodes lancea, mix them, and extract the volatile oil by steam distillation. This volatile oil is reserved as phase A; (2) Take the crushed angelica dahurica, curcuma longa, and the medicinal residues left in (1), and perform percolation by the percolation method. Collect the percolate, recover the solvent, and concentrate it under reduced pressure to an extract with a relative density of 1.0 - 1.5 g / mL, which is reserved as phase B; (3) Take the crushed phellodendron amurense, glycyrrhiza uralensis, arisaema heterophyllum, and rheum palmatum, decoct them several times, combine the filtrates, and heat and concentrate them to an extract density of 1.0 - 1.5 g / mL, which is reserved as phase C; (4) Add phase A and phase B to phase C and mix them evenly to obtain the ethanol extract of golden powder.

6. The hydrogel according to claim 1, characterized in that the raw materials for preparing the golden powder hydrogel further include glycerol, and the mass ratio of glycerol to polyvinyl alcohol is 1:(0.2 - 1).

7. The hydrogel according to claim 1, characterized in that the raw materials for preparing the golden powder hydrogel further include a penetrant; the penetrant includes at least one of azone, borneol, and peppermint oil.

8. A method for preparing a hydrogel according to any one of claims 6 - 7, characterized in that the preparation method includes the following steps: S1. Dilute polyvinyl alcohol and cellulose and / or cellulose derivatives into solutions with water respectively, and mix them evenly; S2. Drop a 2 - 10 wt% aqueous solution of polyphenolic compounds into the solution of S1 and stir; S3. Add glycerol, penetrant, and ethanol extract of golden powder to the solution of S2 in sequence, mix them evenly, remove bubbles by ultrasonic treatment, and pour them into a mold for freeze - thaw cycling; The freeze - thaw cycling is specifically: freeze at - 30~ - 10 °C for 12 - 20 h, thaw at 10~40 °C for 2 - 12 h, and perform freeze - thaw cycling 2 - 6 times.

9. The method for preparing a hydrogel according to claim 8, characterized in that the freeze - thaw cycling is specifically: freeze at - 25~ - 12 °C for 14 - 20 h, thaw at 20~30 °C for 4 - 10 h, and perform freeze - thaw cycling 2 - 5 times.

10. An application of the hydrogel according to any one of claims 1 - 7 as a hydrogel dressing.

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