A multicolor steady-state enhanced 3D printing buccal dissolving film based on gel-solution co-assembly and a preparation method thereof

Abstract

The application discloses a multi-color steady-state enhanced 3D printing oral dissolving film based on gel-solution co-assembly and a preparation method thereof, wherein the preparation method comprises the following steps: mixing an anthocyanin solution and a phycocyanin solution to obtain a phycocyanin-anthocyanin mixed solution; mixing the phycocyanin-anthocyanin mixed solution and a chitosan oligosaccharide solution to obtain a phycocyanin-anthocyanin-chitosan oligosaccharide solution; mixing the phycocyanin-anthocyanin-chitosan oligosaccharide solution, first pregelatinized starch, kappa-carrageenan and a plasticizer to obtain a printing ink; mixing second pregelatinized starch and pullulan to obtain a pregelatinized starch-pullulan mixed solution; printing the printing ink into the pregelatinized starch-pullulan mixed solution through a 3D printing mode, so that the pregelatinized starch-pullulan mixed solution forms an encapsulation film layer on the surface of a printing core film formed by the printing ink through the 3D printing mode, and the multi-color steady-state enhanced 3D printing oral dissolving film is obtained after drying.

Description

TECHNICAL FIELD

[0001] The present application belongs to the field of food dietary supplement film preparation, more particularly, relates to a multi-color stable-state enhanced 3D printed oral dissolving film based on gel-solution co-assembly and a preparation method thereof. BACKGROUND

[0002] The oral dissolving film is a polymer film composed of hydrophilic film-forming polymer, plasticizer, active ingredient and other additives, and its main feature is that it can rapidly disintegrate and adhere to the oral mucosa when in contact with saliva. As a new type of active ingredient and dietary supplement delivery system, the oral dissolving film has many advantages. Among them, since the active ingredient can be rapidly released into the saliva and directly absorbed into the systemic circulation through the oral mucosa, it avoids the destruction of the liver first-pass metabolism to the active ingredient, and increases the bioavailability of the active ingredient. In addition, the oral dissolving film is convenient to carry and does not require water assistance when eaten, greatly improving the convenience. For patients with poor medication compliance, the oral dissolving film is easy to administer and effectively adheres to the tongue or palate, which can prevent spitting or suffocation, so consumers have a high acceptance of the oral dissolving film. In recent years, the oral dissolving film has been proven to have great application potential in the field of functional foods, such as being an excellent delivery platform for many active ingredients such as probiotics, vitamins, melatonin, proteins and functional extracts.

[0003] At present, the traditional preparation technology of the oral dissolving film is based on solution casting, but it lacks flexibility in the design and preparation of the oral dissolving film, and only fixed-size oral dissolving films can be prepared, which has certain limitations. At the same time, the existing oral dissolving film products have the problem of single color, and color is an important part of food perception science, and the rich color of food can stimulate consumers to produce a pleasant mood, so it is difficult to meet the demand of consumers for multi-color oral dissolving films. SUMMARY

[0004] The purpose of the present application is to overcome the above-mentioned defects existing in the prior art, and to provide a multi-color stable-state enhanced 3D printed oral dissolving film based on gel-solution co-assembly and a preparation method thereof. By immobilizing the 3D printed oral dissolving film, not only the color gamut and morphology of the oral dissolving film can be diversified and personalized, but also the stability of the active ingredient can be ensured, and the color and active ingredient of the 3D printed oral dissolving film can be stably enhanced.

[0005] To achieve the above-mentioned purpose, the technical scheme of the present application is as follows:

[0006] A preparation method of a multi-color stable-state enhanced 3D printed oral dissolving film based on gel-solution co-assembly, comprising the following steps:

[0007] Mixing the anthocyanin solution and the phycocyanin solution to obtain a phycocyanin-anthocyanin mixed solution;

[0008] Mixing the phycocyanin-anthocyanin mixed solution with a chitosan oligosaccharide solution to obtain a phycocyanin-anthocyanin-chitosan oligosaccharide solution;

[0009] The phycocyanin-anthocyanin-chitosan oligosaccharide solution is mixed with the first pregelatinized starch and kappa-carrageenan, and a plasticizer is added and mixed to obtain a printing ink;

[0010] mixing the second pregelatinized starch and pullulan to obtain a pregelatinized starch-pululan mixed solution;

[0011] The printing ink is printed into the pregelatinized starch-pullulan mixed solution by 3D printing, so that the pregelatinized starch-pullulan mixed solution forms an encapsulation film layer on the surface of the printing core film, and after drying, the multi-color stable enhanced 3D printed orally dissolving film is obtained; the printing core film is formed by the printing ink by 3D printing.

[0012] The present invention also discloses a multi-color stable enhanced 3D printed orally dissolving film prepared by the above-mentioned preparation method.

[0013] Implementing the embodiments of the present invention will have the following beneficial effects:

[0014] The embodiment of the present invention obtains a phycocyanin-anthocyanin mixed solution with a multi-color gamut by compounding anthocyanin solution and phycocyanin solution, taking advantage of the natural rich color and good water solubility of the two. By adding chitosan oligosaccharide to combine with phycocyanin and anthocyanin, a stable ternary complex is formed, the stability of anthocyanin and phycocyanin is improved, and the steady state of the multi-color gamut is ensured. Pregelatinized starch is inexpensive, biodegradable, and has good film-forming properties. By adding pregelatinized starch, it is combined with kappa-carrageenan and a plasticizer to form a printing ink with good 3D printing performance. The printing ink is printed into the pregelatinized starch-pullulan mixed solution by 3D printing, so that the pregelatinized starch-pullulan mixed solution forms an encapsulation film layer on the surface of the printed core film, which can prevent the degradation of the active ingredients, solve the problem of poor stability of the active ingredients, and make the prepared 3D printed orally dissolving film present a long-lasting and stable multi-color gamut.

[0015] In summary, the embodiment of the present application adopts a 3D printing method based on gel-solution co-assembly, and realizes the diversification and personalization of the color gamut and morphology of the oral dissolving film by fixing and assembling the 3D printing formed oral dissolving film, so as to meet the diversified needs of consumers, solve the problems of single color and morphology in the preparation of traditional oral dissolving films, ensure the stability of active ingredients, and realize the steady-state enhancement of color and active ingredients of the 3D printing oral dissolving film. The prepared 3D printing oral dissolving film has strong antioxidant activity and good stability, and can be used as a new type of dietary supplement and applied in functional food. BRIEF DESCRIPTION OF DRAWINGS

[0016] Figure 1 A and B are respectively the 3D printing oral dissolving film actual photos of Comparative Example 1 and Example 1.

[0017] Figure 2 (A, B) are respectively the tensile strength and elongation at break of the 3D printing oral dissolving film of Comparative Example 1 and Example 1 (different lowercase letters represent significant differences between groups p<0.05).

[0018] Figure 3 is the color difference value of the color stability evaluation of the 3D printing oral dissolving film of Comparative Example 1 and Example 1 after light storage for 8d (different lowercase letters represent significant differences between groups p<0.05).

[0019] Figure 4 is the retention rate of anthocyanins in the 3D printing oral dissolving film of Comparative Example 1 and Example 1 after light storage for 8d (different lowercase letters represent significant differences between groups p<0.05).

[0020] Figure 5 A and B are respectively the DPPH and ABTS antioxidant activity evaluation of the 3D printing oral dissolving film of Comparative Example 1 and Example 1 (different lowercase letters represent significant differences between groups p<0.05).

[0021] Figure 6 is the 3D printing oral dissolving film actual photo prepared by different concentrations of active substances. DETAILED DESCRIPTION

[0022] The present application will be further described below in conjunction with specific embodiments, but in no way limits the present application.

[0023] The present application discloses a preparation method of a multi-color steady-state enhanced 3D printing oral dissolving film based on gel-solution co-assembly, comprising the following steps:

[0024] 1) Mix the anthocyanin solution and the phycocyanin solution to obtain a phycocyanin-anthocyanin mixed solution.

[0025] Specifically, the application introduces natural substances anthocyanin and phycocyanin as raw materials, compounding anthocyanin solution and phycocyanin solution, anthocyanin is a natural water-soluble pigment, and phycocyanin is a natural water-soluble pigment protein with light capturing function, and the natural rich color and good water solubility of the two are used to obtain a phycocyanin-anthocyanin mixed solution with multiple color domains.

[0026] In a specific embodiment, step 1) specifically comprises the following steps:

[0027] 1.1) Dissolve anthocyanin in a sodium phosphate dibasic-citric acid buffer solution to obtain an anthocyanin solution.

[0028] In a specific embodiment, the pH of the sodium phosphate dibasic-citric acid buffer solution is 3.

[0029] In a specific embodiment, step 1.1) specifically comprises:

[0030] 1.1.1) Take 28.392 g of sodium phosphate dibasic, dissolve and dilute to 1000 mL with distilled water, shake well, and obtain a 0.2 mol / L sodium phosphate dibasic solution.

[0031] 1.1.2) Take 19.212 g of citric acid, dissolve and dilute to 1000 mL with distilled water, shake well, and obtain a 0.1 mol / L citric acid solution.

[0032] 1.1.3) Mix the 0.2 mol / L sodium phosphate dibasic solution and the 0.1 mol / L citric acid solution at a volume ratio of 4.11:15.89 to obtain a sodium phosphate dibasic-citric acid buffer solution with a pH of 3.

[0033] 1.1.4) Under room temperature and light shielding conditions, magnetically stir the anthocyanin and the sodium phosphate dibasic-citric acid buffer solution at a speed of 500 r / min-800 r / min for 20 min-40 min, then perform ultrasonic treatment at an ultrasonic power of 40 kHz for 3 min-10 min, and then filter with a 0.45 μm filter membrane to obtain the anthocyanin solution.

[0034] In a specific embodiment, the concentration of anthocyanin in the anthocyanin solution is 5 mg / mL-10 mg / mL.

[0035] In a specific embodiment, the anthocyanin is blueberry anthocyanin.

[0036] 1.2) Dissolve phycocyanin in distilled water to obtain a phycocyanin solution.

[0037] In a specific embodiment, the concentration of phycocyanin in the phycocyanin solution is 5 mg / mL-10 mg / mL.

[0038] 1.3) The anthocyanin solution and the phycocyanin solution are dissolved in distilled water and magnetically stirred for 10-30 min to obtain a phycocyanin-anthocyanin mixed solution.

[0039] In a specific embodiment, the concentration of anthocyanin in the phycocyanin-anthocyanin mixed solution is 0.1-0.5 mg / mL.

[0040] In a specific embodiment, the concentration of phycocyanin in the phycocyanin-anthocyanin mixed solution is 0.05-2.5 mg / mL.

[0041] In a specific embodiment, the concentration ratio of anthocyanin to phycocyanin in the phycocyanin-anthocyanin mixed solution is 1:(0.5-5).

[0042] 2) The phycocyanin-anthocyanin mixed solution is mixed with a chitosan oligosaccharide solution to obtain a phycocyanin-anthocyanin-chitosan oligosaccharide solution.

[0043] Specifically, by combining chitosan oligosaccharide with the phycocyanin-anthocyanin mixed solution, a stable ternary complex of anthocyanin and phycocyanin is formed, thereby improving the stability of anthocyanin and phycocyanin and ensuring the stability of the multi-color gamut.

[0044] In a specific embodiment, step 2) specifically comprises the following steps: the chitosan oligosaccharide solution is mixed with the phycocyanin-anthocyanin mixed solution at a ratio of 1:1 (v / v) and magnetically stirred for 10-30 min to obtain a phycocyanin-anthocyanin-chitosan oligosaccharide solution.

[0045] In a specific embodiment, the concentration of chitosan oligosaccharide in the chitosan oligosaccharide solution is 2.5-10 mg / mL.

[0046] 3) The phycocyanin-anthocyanin-chitosan oligosaccharide solution is mixed with first pre-gelatinized starch and κ-carrageenan, and a plasticizer is added and mixed to obtain a printing ink.

[0047] In a specific embodiment, the first pre-gelatinized starch is pre-gelatinized tapioca starch. Specifically, by adding first pre-gelatinized starch as pre-gelatinized tapioca starch, not only is the price low, but also biodegradable, and it has good film-forming property, and after being combined with κ-carrageenan and a plasticizer, a printing ink with good 3D printing performance is formed.

[0048] In a specific embodiment, step 3) specifically comprises the following steps:

[0049] 3.1) The first pre-gelatinized starch and the κ-carrageenan are slowly added to the phycocyanin-anthocyanin-chitosan oligosaccharide solution, and then the plasticizer is added and magnetically stirred at 50-80°C for 20-40 min to obtain a printing ink.

[0050] In an embodiment, the mass concentration of the first pregelatinized starch in the printing ink is 8% to 12%.

[0051] In an embodiment, the mass concentration of the kappa-carrageenan in the printing ink is 0.5% to 3.0%.

[0052] In an embodiment, the plasticizer is glycerol.

[0053] In an embodiment, the volume fraction of the plasticizer is 3% to 10% based on 100% of the volume of the printing ink.

[0054] 4) mixing the second pregelatinized starch and the pullulan to obtain a pregelatinized starch-pullulan mixed solution.

[0055] In an embodiment, step 4) specifically comprises the following steps: magnetically stirring the second pregelatinized starch and the pullulan at 50°C to 80°C for 20 min to 40 min to obtain the pregelatinized starch-pullulan mixed solution.

[0056] In an embodiment, the mass concentration of the second pregelatinized starch in the pregelatinized starch-pullulan mixed solution is 2% to 6%.

[0057] In an embodiment, the mass concentration of the pullulan in the pregelatinized starch-pullulan mixed solution is 6% to 8%.

[0058] In an embodiment, the second pregelatinized starch is pregelatinized tapioca starch.

[0059] 5) printing the printing ink into the pregelatinized starch-pullulan mixed solution by 3D printing to form an encapsulation film layer on the surface of the printing core film, and drying to obtain a multi-color steady-state enhanced 3D printed oromucosal film; the printing core film is formed by 3D printing of the printing ink.

[0060] Specifically, the printing ink is printed into the pregelatinized starch-pullulan mixed solution by 3D printing to form an encapsulation film layer on the surface of the printing core film in the form of macromolecular encapsulation, which can prevent degradation of the active ingredients and solve the problem of poor stability of the active ingredients, so that the prepared 3D printed oromucosal film presents a long-acting steady-state multi-color gamut. The formed encapsulation film layer is colorless and transparent, avoiding the influence of the existence of the outer encapsulation film layer on the color display of the inner printing core film.

[0061] In an embodiment, the thickness ratio of the printing core film to the encapsulation film layer is 1:(0.5 to 1).

[0062] In a specific embodiment, step 5) specifically comprises the following steps:

[0063] 5.1) Put the printing ink into the printing cartridge matched with the 3D printer, and centrifuge at 3000 r / min to 5000 r / min for 10 min to 30 min to sufficiently remove the bubbles.

[0064] 5.2) Start the 3D printer, install the printing cartridge, and test whether the printing ink can be extruded according to the extrusion, to ensure that the printing ink can be smoothly extruded.

[0065] 5.3) Select the desired model pattern from the model library, set the corresponding parameters, and then print the printing ink after centrifugation into the pregelatinized starch-pullulan mixed solution by 3D printing, so that the pregelatinized starch-pullulan mixed solution forms an encapsulation film layer on the surface of the printing core film, and after drying at 35℃ to 40℃ for 6 h to 12 h, a steady-state 3D printing oral film is obtained.

[0066] In a specific embodiment, the diameter of the 3D printing nozzle is 0.2 mm to 1.0 mm, and the 3D printing speed is 9 mm / s to 36 mm / s.

[0067] The application also discloses a multi-color steady-state enhanced 3D printing oral film prepared by the preparation method provided in any of the embodiments of the application. The 3D printing oral film prepared by the 3D printing method based on gel-solution co-assembly can be fixedly assembled, and not only can realize the diversification and individualization of the color gamut and morphology of the oral film, meet the diversified needs of consumers, solve the problem of single color and morphology of the oral film in the traditional preparation, but also can guarantee the stability of the active ingredients, realize the steady-state enhancement of the color and active ingredients of the 3D printing oral film, and can be used as a new type of dietary supplement film and applied in functional foods.

[0068] The following are specific embodiments

[0069] Embodiment 1

[0070] The preparation method of the 3D printed orodispersible film of the present embodiment comprises the following steps: under room temperature and light shielding condition, blueberry anthocyanin and sodium phosphate dibasic-citric acid buffer solution with pH of 3 are subjected to magnetic stirring at a rotating speed of 500 r / min for 30 min, then ultrasonic treatment is performed under 40 kHz ultrasonic power for 5 min, and then filtration is performed by using a 0.45 μm filter to obtain an anthocyanin solution with a blueberry anthocyanin concentration of 10 mg / mL. Phycocyanin is dissolved in distilled water to obtain a phycocyanin solution with a concentration of 10 mg / mL. 1 mL of the anthocyanin solution is added into 47.5 mL of distilled water to make the final concentration of the anthocyanin solution 0.2 mg / mL, and then 1.5 mL of the phycocyanin solution is added after magnetic stirring to make the final concentration of the phycocyanin solution 0.3 mg / mL, and the mixture is subjected to magnetic stirring at a rotating speed of 500 r / min for 15 min to obtain 50 mL of a phycocyanin-anthocyanin mixed solution. 500 mg of chitosan oligosaccharide is dissolved in 50 mL of distilled water to obtain a chitosan oligosaccharide solution with a concentration of 10 mg / mL. The chitosan oligosaccharide solution and the phycocyanin-anthocyanin mixed solution are mixed in a ratio of 1:1 (v / v) (the final concentration of chitosan oligosaccharide is 5 mg / mL), and the mixture is subjected to magnetic stirring at a rotating speed of 500 r / min for 20 min to obtain 100 mL of a phycocyanin-anthocyanin-chitosan oligosaccharide solution. Pre-gelatinized tapioca starch and K-carrageenan are slowly added into the above-mentioned phycocyanin-anthocyanin-chitosan oligosaccharide solution preheated to 50°C under magnetic stirring, and then glycerol is added into the system, and the mixture is subjected to continuous magnetic stirring at a rotating speed of 800 r / min for 30 min to obtain a printing ink. In the printing ink, the mass concentration of pre-gelatinized tapioca starch is 10%, the mass concentration of K-carrageenan is 1.5%, and the volume fraction of glycerol is 5% based on 100% of the volume of the printing ink. Pre-gelatinized tapioca starch and pullulan are subjected to magnetic stirring at 50°C for 30 min to obtain a pre-gelatinized starch-pullulan mixed solution, and in the pre-gelatinized starch-pullulan mixed solution, the mass concentration of pre-gelatinized tapioca starch is 4% and the mass concentration of pullulan is 7%. The pre-gelatinized starch-pullulan mixed solution is poured into a small dish. The printing ink is placed in a printing cartridge matched with a 3D printer, and the mixture is subjected to centrifugation at a rotating speed of 3500 r / min for 20 min to sufficiently remove air bubbles. After the 3D printer is started and the printing cartridge is installed to ensure that the printing ink can be smoothly extruded, a desired model pattern is selected from a model library, and the centrifuged printing ink is printed into the small dish containing the pre-gelatinized starch-pullulan mixed solution by a 3D printing method. The diameter of a 3D printing nozzle is 0.4 mm, and the 3D printing speed is 24 mm / s. After printing, the mixture is dried at 35°C for 10 h to obtain a 3D printed orodispersible film as shown in Figure 1 B. The pre-gelatinized starch-pullulan mixed solution forms an encapsulating film layer on the surface of the printed core film, and the thickness ratio of the printed core film to the encapsulating film layer is 1:0.8.

[0071] Comparative Example 1

[0072] The present comparative example is compared with Example 1, the only difference being that the preparation method of the present comparative example does not contain a pre-gelatinized starch-pullulan mixed solution to form an encapsulation film layer on the surface of the printing ink. The 3D-printed orally dissolving film of the present comparative example is as shown in Figure 1 A.

[0073] Test Example

[0074] I. Evaluation of the physical properties of the 3D-printed orally dissolving films of Example 1 and Comparative Example 1

[0075] The mechanical properties of the orally dissolving film were evaluated to determine the product's molding ability and application stability. The mechanical properties of the orally dissolving film were determined according to the method of GB / T 1040.3-2006 "Determination of tensile properties of plastics". The film was cut into a long strip of 100 mm x 15 mm and fixed on an electronic tensile testing machine to measure the tensile strength and elongation at break of the film. The test results are shown in Figure 2 A and B. Figure 2 (A, B) are the tensile strength and elongation at break of the orally dissolving films of Comparative Example 1 and Example 1, respectively (different lowercase letters represent significant differences between groups p < 0.05). As can be seen from Figure 2 A, B, the tensile strength and elongation at break of the 3D-printed orally dissolving film of Example 1 prepared based on gel-solution co-assembly are significantly improved compared to Comparative Example 1. Therefore, the encapsulation film layer formed by immobilizing the 3D-printed orally dissolving film can improve the mechanical properties of the 3D-printed orally dissolving film.

[0076] II. Evaluation of the color stability of the 3D-printed orally dissolving films of Example 1 and Comparative Example 1

[0077] The 3D-printed orally dissolving films of Comparative Example 1 and Example 1 were subjected to simulated light accelerated testing to evaluate their color stability under light stress. The color difference value (ΔE) of the color change was calculated according to the following formula:

[0078]

[0079] The results are shown in Figure 3 A and B. Figure 3 The color difference value (ΔE) of the 3D-printed orally dissolving films of Comparative Example 1 and Example 1 after 8 days of light storage is shown in

[0080] III. Evaluation of the anthocyanin content stability of the 3D-printed orally dissolving films of Example 1 and Comparative Example 1

[0081] The 3D-printed oral dissolving films of Comparative Example 1 and Example 1 were evaluated for the retention rate of anthocyanins under simulated light accelerated conditions to evaluate the steady-state effect of anthocyanins in Comparative Example 1 and Example 1. The content of anthocyanins was determined according to the pH differential method, and the retention rate was calculated according to the following formula:

[0082] Retention rate of anthocyanins (%) = C t / C0 x 100

[0083] Wherein, C t and C0 are the concentrations of anthocyanins at time t and the initial time, respectively, mg / mL.

[0084] The results are shown in Table 1. Figure 4 Figure 4 After 8 days of light storage, the retention rate of anthocyanins in the oral dissolving films of Comparative Example 1 and Example 1 in the present application (different lowercase letters represent significant differences within the group, p < 0.05), the retention rate of anthocyanins decreased with increasing storage time. After 8 days of light treatment, the retention rate of anthocyanins in the 3D-printed oral dissolving films of Comparative Example 1 was 61.42%, while the retention rate of anthocyanins in Example 1 was 70.33%. Compared with Comparative Example 1, the oral dissolving films formed by 3D printing in Example 1 significantly improved the retention rate of anthocyanins during storage, achieving the effect of steady-state enhancement of anthocyanin content.

[0085] IV. Evaluation of the antioxidant activity of the 3D-printed oral dissolving films of Example 1 and Comparative Example 1

[0086] To prove that the prepared 3D-printed oral dissolving films have good biological activity, the antioxidant activity of the 3D-printed oral dissolving films of Example 1 and Comparative Example 1 was evaluated by DPPH and ABTS radical scavenging capacity after 4 days of light accelerated storage, to further analyze the steady-state enhancement effect of the antioxidant activity of the 3D-printed oral dissolving films.

[0087] Determination of antioxidant capacity by DPPH method: 100 μL of 0.2 mM DPPH ethanol solution was placed in a 96-well plate, 100 μL of sample ethanol solution was added, mixed thoroughly, and then incubated at room temperature for 30 min in the dark. The absorbance value of each well was measured at 517 nm using a microplate reader. The activity formula for scavenging DPPH radicals is as follows:

[0088] DPPH scavenging activity (%) = [1 - (S - SB) / (C - CB)] x 100%

[0089] Wherein: S sample: 100 μL sample solution + 100 μL DPPH solution; SB sample blank: 100 μL sample solution + 100 μL anhydrous ethanol; C control: 100 μL anhydrous ethanol + 100 μL DPPH solution; CB blank control: 200 μL anhydrous ethanol.​

[0090] ABTS method was used to determine the antioxidant capacity: ABTS was dissolved in PBS (0.01 M, pH 7.4) to prepare a 7 mM ABTS solution, which was then reacted with potassium persulfate (final concentration 2.45 mM) to generate ABTS. + Place the ABTS in a dark place at room temperature for 16 hours. + The solution was diluted with PBS (0.01M, pH 7.4) until the absorbance at 734 nm reached 0.70 ± 0.02. After equilibration at 30°C for 30 min, it was ready for measurement. 150 μL of ABTS solution was added to a 96-well plate, followed by 100 μL of the sample ethanol solution to be tested. After thorough mixing, the plate was allowed to stand for 20 min, and the absorbance at 734 nm was measured using a microplate reader. + The scavenging activity was calculated as follows:

[0091] ABTS + Scavenging activity (%) = [1-(S-SB) / (C-CB)] × 100%

[0092] Where: S sample: 100 μL sample solution + 150 μL ABTS + Solution; SB sample blank: 100 μL sample solution + 150 μL PBS; C control: 100 μL anhydrous ethanol + 150 μL ABTS + Solution; CB blank control: 100 μL anhydrous ethanol + 150 μL PBS.

[0093] The test results are as follows Figure 5 As shown in A and B, Figure 5 A and B represent the antioxidant activity evaluations of the orally disintegrating films of Comparative Example 1 and Example 1 of the present invention against DPPH and ABTS, respectively (different lowercase letters represent significant differences between groups, p < 0.05). Compared with Comparative Example 1, the antioxidant activity of the 3D-printed orally disintegrating film of Example 1 was significantly enhanced, indicating that the gel-solution co-assembly can alleviate the loss of antioxidant activity of anthocyanins caused by environmental stress. Therefore, the steady-state effect of the antioxidant activity of the 3D-printed orally disintegrating film of Example 1 is enhanced.

[0094] Example 2

[0095] In order to analyze the influence of different concentrations of active substances on the color gamut of the prepared 3D printed oral film, in the phycocyanin-anthocyanin mixed solution, sample A without blueberry anthocyanin and phycocyanin, sample B containing 0.2 mg / mL of blueberry anthocyanin and without phycocyanin, sample C containing 0.2 mg / mL of blueberry anthocyanin and containing 0.1 mg / mL of phycocyanin, sample D containing 0.2 mg / mL of blueberry anthocyanin and containing 0.2 mg / mL of phycocyanin, sample E containing 0.2 mg / mL of blueberry anthocyanin and containing 0.3 mg / mL of phycocyanin, sample F containing 0.2 mg / mL of blueberry anthocyanin and containing 0.4 mg / mL of phycocyanin, sample G containing 0.2 mg / mL of blueberry anthocyanin and containing 0.5 mg / mL of phycocyanin, and sample H containing 0.3 mg / mL of phycocyanin without blueberry anthocyanin were set.

[0096] According to the preparation method of Example 1, the above samples were prepared into 3D printed oral films, and the results are shown in Table 1. Figure 6 As shown in Table 1, sample A without blueberry anthocyanin and phycocyanin is colorless and translucent, sample H without blueberry anthocyanin and containing 0.3 mg / mL of phycocyanin is light blue, sample B containing 0.2 mg / mL of blueberry anthocyanin and without phycocyanin is light purple, and as the concentration of phycocyanin increases, the sample presents a multi-color gamut from light purple, dark purple to blue-purple, so that the prepared 3D printed oral film has a multi-rich color, and the printed oral film has a good appearance and uniform structure.

[0097] In summary, the gel-solution co-assembled 3D printed oral film obtained by the embodiment of the present application has appropriate viscoelasticity, smooth lines during printing, and is not easy to break, has good 3D printing characteristics, and the 3D printed oral film formed after printing has appropriate thickness, uniform color and texture. The prepared 3D printed oral film can present a multi-color gamut, meet the requirements of food perception science, have rich colors, stimulate the appetite of consumers and produce a pleasant mood. At the same time, it is rich in active ingredients anthocyanin and phycocyanin, has strong antioxidant activity, good stability, and can be used as a new type of antioxidant dietary supplement and applied in functional food.

[0098] In addition, the 3D printing method based on gel-solution co-assembly can improve the mechanical properties of the 3D printing oral dissolving film, increase the retention rate of anthocyanins during storage, realize the effect of steady-state enhancement of anthocyanin content, ensure the color stability of the multi-color gamut, realize the effect of steady-state enhancement of color and luster of the 3D printing oral dissolving film, realize the diversification, individualization and automation of product production, enrich the types of 3D printing food materials and the types of oral dissolving film terminal products, the preparation method is simple and practical, the products have various forms, novel and unique, light and portable, easy to use, and can meet the diversified needs of consumers.

[0099] The above-described embodiments only express several embodiments of the present application, and the description is more specific and detailed, but it should not be understood as limiting the scope of the application. It should be noted that for ordinary skilled in the art, without departing from the concept of the present application, a number of modifications and improvements can be made, which are within the scope of the present application. Therefore, the protection scope of the present application patent should be subject to the appended claims.

Claims

1. A method for the preparation of a multichromatic steady-state enhanced 3D printed buccal dissolving film based on gel-solution co-assembly, characterized in that, The method comprises the following steps: mixing the anthocyanin solution with the phycocyanin solution to obtain a phycocyanin-anthocyanin mixed solution; mixing the phycocyanin-anthocyanin mixed solution with a chitosan oligosaccharide solution to obtain a phycocyanin-anthocyanin-chitosan oligosaccharide solution; mixing the phycocyanin-anthocyanin-chitosan oligosaccharide solution with first pregelatinized starch and kappa-carrageenan, and then adding a plasticizer to obtain a printing ink; mixing second pregelatinized starch and pullulan to obtain a pregelatinized starch-pullulan mixed solution; printing the printing ink into the pregelatinized starch-pullulan mixed solution by a 3D printing method, so that the pregelatinized starch-pullulan mixed solution forms an encapsulation film layer on the surface of a printing core film, and the multiple color stable state enhanced 3D printing oromucosal film is obtained after drying; the printing core film is formed by the printing ink through the 3D printing method; the thickness ratio of the printing core film to the encapsulation film layer is 1: (0.5-1); the mixing ratio of the chitosan oligosaccharide solution to the phycocyanin-anthocyanin mixed solution is 1:1 (v / v); the concentration of chitosan oligosaccharide in the chitosan oligosaccharide solution is 2.5 mg / mL-10 mg / mL; the mass concentration of the first pregelatinized starch in the printing ink is 8%-12%; the mass concentration of kappa-carrageenan in the printing ink is 0.5%-3.0%; the first pregelatinized starch is pregelatinized cassava starch; the temperature for mixing the phycocyanin-anthocyanin-chitosan oligosaccharide solution, the first pregelatinized starch and the kappa-carrageenan is 50-80 ℃; the mixing time of the phycocyanin-anthocyanin-chitosan oligosaccharide solution, the first pregelatinized starch and the kappa-carrageenan is 20-40 min; the plasticizer is glycerol; the volume fraction of the plasticizer is 3%-10% based on 100% of the volume of the printing ink; the mass concentration of the second pregelatinized starch in the pregelatinized starch-pullulan mixed solution is 2%-6%; the mass concentration of pullulan in the pregelatinized starch-pullulan mixed solution is 6%-8%; the temperature for mixing the second pregelatinized starch and the pullulan is 50-80 ℃; the mixing time of the second pregelatinized starch and the pullulan is 20-40 min; the second pregelatinized starch is pregelatinized cassava starch.

2. A process for the preparation of gel-solution co-assembled multichromic steady state enhanced 3D printed buccal dissolving films according to claim 1, characterized in that, The preparation method of the anthocyanin solution comprises the following steps: dissolving anthocyanin in a sodium phosphate-citric acid buffer solution to obtain the anthocyanin solution; wherein, the concentration of anthocyanin in the anthocyanin solution is 5 mg / mL-10 mg / mL; the pH of the sodium phosphate-citric acid buffer solution is 3; the anthocyanin is blueberry anthocyanin; The preparation method of the phycocyanin solution comprises the following steps: dissolving phycocyanin in distilled water to obtain the phycocyanin solution; wherein, the concentration of phycocyanin in the phycocyanin solution is 5 mg / mL-10 mg / mL.

3. A process for the preparation of gel-solution co-assembled multichromic steady state enhanced 3D printed buccal dissolving films according to claim 1, characterized in that, The concentration of anthocyanins in the phycocyanin-anthocyanin mixed solution is 0.1 mg / mL to 0.5 mg / mL; The concentration of phycocyanin in the phycocyanin-anthocyanin mixed solution is 0.05 mg / mL to 2.5 mg / mL; In the phycocyanin-anthocyanin mixed solution, the concentration ratio of anthocyanins to phycocyanin is 1: (0.5 to 5).

4. A process for the preparation of gel-solution co-assembled multichromic steady state enhanced 3D printed buccal dissolving films according to claim 1, characterized in that, Before 3D printing, the printing ink is further subjected to centrifugation to remove air bubbles; The rotation speed of the centrifugation is 3000 r / min to 5000 r / min; The centrifugation time is 10 min to 30 min; The 3D printing speed is 9 mm / s to 36 mm / s; The drying temperature is 35 ℃ to 40 ℃; The drying time is 6 h to 12 h.

5. A multi-color steady-state enhanced 3D printing buccal film prepared by the preparation method of any one of claims 1 to 4.

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