A HydroMg negative hydrogen ion sustained-release microcapsule and its preparation method and application

Abstract

The present invention relates to a kind of HydroMg negative hydrogen ion sustained-release microcapsule and its preparation method and application, the sustained-release microcapsule includes a core material and a wall material, the mass ratio of the core material to the wall material is 1: (1.0-2.5); the wall material includes resistant dextrin; in parts by mass, the core material includes the following components: 5-10 parts of magnesium-based hydrogen storage material, 10-20 parts of guanidine, 5-10 parts of sodium hyaluronate, and 5-10 parts of compound lactic acid bacteria; the magnesium-based hydrogen storage material is obtained by reacting magnesium oxide raw material with hydrogen to obtain HydroMg negative hydrogen ion material, and then pre-coating the HydroMg negative hydrogen ion material; the microcapsule is prepared by negative pressure low-temperature spray drying. The sustained-release capsule obtained by the present invention has an excellent sustained-release effect and can effectively avoid the loss of negative hydrogen ions in the magnesium-based hydrogen storage material.

Description

Technical Field

[0001] The present invention belongs to the technical field of magnesium-based hydrogen storage materials, and in particular relates to a HydroMg negative hydrogen ion sustained-release microcapsule and a preparation method and application thereof. Background Art

[0002] Negative hydrogen ions, also known as hydride ions, are hydrogen atoms with an extra electron, resulting in a negative charge. Negative hydrogen ions play a crucial role in all life on Earth, acting as energy carriers in a wide range of organisms. Negative hydrogen ions are tiny and extremely light, making them essential antioxidants for all life on Earth. They activate cells and boost metabolism. Existing research indicates that negative hydrogen ions have numerous benefits, including prolonging life, improving sleep, increasing skin elasticity, and preventing cancer.

[0003] In the existing technology, magnesium-based hydrogen storage materials are generally used to store and provide negative hydrogen ions. The high hydrogen absorption and desorption temperature and slow hydrogen absorption and desorption rate of magnesium-based hydrogen storage materials limit their practical application. Therefore, the use of a core-shell structure similar to a microcapsule to coat nano-magnesium-based hydrogen storage materials helps to improve the hydrogen storage performance of the material, and certain results have been achieved.

[0004] Microencapsulation technology, which encapsulates trace amounts of substances in polymer films, is a micro-packaging technology for storing solids, liquids, and gases. Specifically, it involves completely encapsulating a target substance (the core or inner phase) with a continuous film (the wall or outer phase) of various natural or synthetic polymer compounds, without compromising the target's original chemical properties. The target's functions are then gradually re-emerged through certain external stimuli or sustained-release effects, or the core material is protected by the barrier effect of the capsule wall.

[0005] At present, microcapsule technology has gradually become a key research direction in the field of sustained release. For example, patent application CN115428945A discloses a sustained-release antioxidant composition containing magnesium hydride and its application. The sustained-release antioxidant composition includes the following components, in parts by weight: 80-160 parts of magnesium hydride microcapsules, 180-220 parts of γ-aminobutyric acid, and 1-4 parts of niacinamide. The magnesium hydride microcapsules are prepared by spray drying with magnesium hydride and malic acid as a mixed core material and sodium alginate, ethyl cellulose and sodium hyaluronate as a composite wall material; the mass percentage ratio of the core material to the wall material is 1:(2-3.5); the mass percentage ratio of magnesium hydride to malic acid in the mixed core material is (3-5):(10-20); and the magnesium hydride is prepared by reaction using magnesium oxide as a raw material. While this patent represents a significant breakthrough and contribution in terms of sustained release and improved utilization of magnesium hydrogen compared to existing technologies, it utilizes a composite wall material of sodium alginate, ethylcellulose, and sodium hyaluronate. This wall material is relatively expensive, and the sustained release effect still needs to be improved. Furthermore, the protection of magnesium hydrogen during the coating process is insufficient, which can easily lead to premature reaction and inactivation of some of it. Furthermore, the spray drying method employed uses relatively high temperatures, which is unfriendly to probiotics and can reduce their efficacy to a certain extent.

[0006] Therefore, how to provide a sustained-release microcapsule that has excellent sustained-release effect, reduces the loss of negative hydrogen ions, and retains the efficacy of active substances to the maximum extent has become a technical problem that needs to be solved urgently in the existing technology. Summary of the Invention

[0007] In response to the above-mentioned deficiencies in the prior art, the present invention aims to provide HydroMg negative hydrogen ion sustained-release microcapsules, as well as their preparation method and application. By using the HydroMg negative hydrogen ion sustained-release microcapsules provided by the present invention and selecting specific types and amounts of core and wall materials to prepare the sustained-release microcapsules, the active substance content and sustained-release effect of the microcapsules can be significantly optimized.

[0008] In order to solve the above technical problems, the first aspect of the present invention provides a HydroMg negative hydrogen ion sustained-release microcapsule, comprising a core material and a wall material, wherein the mass ratio of the core material to the wall material is 1:(1.0-2.5);

[0009] The wall material includes resistant dextrin;

[0010] The core material comprises the following components in parts by mass:

[0011]

[0012] The magnesium-based hydrogen storage material is prepared by reacting a magnesium oxide raw material with hydrogen to obtain a HydroMg negative hydrogen ion material, and then pre-coating the HydroMg negative hydrogen ion material;

[0013] The microcapsules are prepared by a negative pressure low-temperature spray drying method.

[0014] Furthermore, the composite lactic acid bacteria includes Streptococcus thermophilus and Lactobacillus bulgaricus in a mass ratio of 1:(1-2).

[0015] Furthermore, the wall material further includes a wall material ingredient selected from at least one of gelatin, chitosan, sodium alginate, and lauric acid monoglyceride, and the total mass ratio of the wall material ingredients to the resistant dextrin is (5-15):10. Specifically, the resistant dextrin, gelatin, and sodium alginate are mixed in a mass ratio of 10:(2-6):(2-6), or the resistant dextrin, gelatin, chitosan, and lauric acid monoglyceride are mixed in a mass ratio of 10:(2-6):(1-2):(2-5) to provide the wall material.

[0016] Furthermore, the negative pressure low temperature spray drying method comprises the following steps:

[0017] (1): Add the wall material raw materials into 60-80℃ deionized water and stir to obtain a wall material solution;

[0018] (2): Add bird's nest acid and sodium hyaluronate to the wall material solution, homogenize at high speed, and cool to room temperature;

[0019] (3): Adding the composite lactic acid bacteria and the magnesium-based hydrogen storage material to the solution of step (2) in sequence, and pressurizing and homogenizing;

[0020] (4): The material homogenized in step (3) is atomized in a negative pressure drying chamber, and a 20-40°C drying gas is introduced for spray drying.

[0021] Furthermore, 1-5% of the weight of the wall material raw material sodium dihydrogen phosphate is added to the wall material solution; when the temperature in step (2) drops to 35-45° C., 1-5% of the weight of the sodium hyaluronate collagen peptide is added with stirring.

[0022] Furthermore, the magnesium-based hydrogen storage material further includes a hydrogen storage auxiliary material, which is selected from at least one of magnesium gluconate, yeast beta glucose, and oyster powder. Preferably, the HydroMg negative hydrogen ion material and the hydrogen storage auxiliary material are mixed in a mass ratio of (10-17):1, and in the hydrogen storage auxiliary material, magnesium gluconate, yeast beta glucose and oyster powder are compounded in a mass ratio of 1:(1-3):(1-3); the pre-coating process comprises the following steps:

[0023] (1) Grinding HydroMg negative hydrogen ion material;

[0024] (2) Dispersing the HydroMg negative hydrogen ion material and hydrogen storage auxiliary materials in liquid polyethylene glycol and vacuum drying.

[0025] Furthermore, the microcapsules have an average particle size of 5-50 μm, preferably 5-30 μm, and more preferably 10-20 μm; a moisture content of less than 3.5 wt%, preferably less than 3 wt%, a water activity of less than 0.38 aw, preferably less than 0.3 aw, and a microcapsule encapsulation efficiency greater than 90%. Moisture content and water activity significantly affect the viscosity, microbial stability, oxidation degree, and storage stability of the microcapsules. The present invention has low moisture content and water activity, ensuring storage stability and safety in use.

[0026] A second aspect of the present invention provides a method for preparing the aforementioned HydroMg negative hydrogen ion sustained-release microcapsules of the present invention, the method comprising the following steps:

[0027] S1. Preparation of magnesium-based hydrogen storage materials:

[0028] S1.1 Heat magnesium oxide powder, introduce hydrogen, cool the product to room temperature, and grind it to obtain HydroMg negative hydrogen ion material;

[0029] S1.2 The HydroMg negative hydrogen ion material and the optional hydrogen storage auxiliary material are dispersed in liquid polyethylene glycol with a molecular weight of 400-600 for pre-coating, and vacuum dried;

[0030] S2. Preparation of sustained-release microcapsules by negative pressure low-temperature spray drying:

[0031] S2.1 Add the wall material raw materials into 60-80℃ deionized water and stir to obtain a wall material solution;

[0032] S2.2 Add sialic acid and sodium hyaluronate to the wall material solution, homogenize at high speed, and cool to room temperature;

[0033] S2.3 Add the composite lactic acid bacteria and magnesium-based hydrogen storage material to the solution of step S2.2 in sequence and homogenize under pressure;

[0034] S2.4 Atomize the material homogenized in step S2.3 in a negative pressure drying chamber while introducing dry gas. The vacuum degree in the drying chamber is -0.1 to -0.01 MPa, the air inlet temperature in the drying chamber is 20-40°C, and the air outlet temperature is 10-25°C.

[0035] Furthermore, the speed of the high-speed homogenizer is 15000-25000 rpm, and the time of high-speed homogenization is 0.5-5 minutes; the speed of the pressurized homogenizer is 10000-15000 r / min, and the homogenization is performed at 30-50 MPa for 1-3 times.

[0036] The third aspect of the present invention is the use of the aforementioned sustained-release microcapsules in food, medicine or skin care products.

[0037] The present invention has the advantages that:

[0038] (1) According to the requirements of the use environment and the properties of the materials, specific types and amounts of core materials and wall materials are used to prepare sustained-release microcapsules: resistant dextrin is used as the wall material. Resistant dextrin is not easily decomposed by various starch alcohols. When taken orally, it is firstly not easily utilized by amylase and caries bacteria in the oral cavity. Secondly, gastric acid, pancreatic amylase, small intestinal mucosal enzymes, etc. cannot decompose it, so no heat is generated, which does not affect the stability of the HydroMg negative hydrogen ion material. The gelling property of water-soluble dietary fiber is used to delay the retention time of the HydroMg negative hydrogen ion material in the digestive tract to achieve the slow release of hydrogen. In addition, after entering the intestine, the resistant dextrin is fermented by bacteria in the intestine to convert it into short-chain fatty acids such as acetic acid, propionic acid, and butyric acid, which increases local acidity and promotes the release of Mg.

[0039] The HydroMg negative hydrogen ion material used in the core material is at the micro-nano size level, which can prevent / alleviate various adverse symptoms caused by magnesium deficiency in the body. At the same time, the introduction of hydrogen's antioxidant effect is also beneficial for anti-inflammation, strengthening the body, delaying aging, and preventing diseases. The endogenous driving force of released hydrogen can be used to assist in the directional transport and local treatment of other active substances. At the same time, the sustained-release and controlled-release hydrogen function of the HydroMg negative hydrogen ion material of the present invention is also triple-guaranteed. On the one hand, the surface of the HydroMg negative hydrogen ion material is covered with a small amount of oxide, and its state is relatively stable. It slowly releases hydrogen when it comes into contact with water. The oxide on its surface gradually decomposes in an acidic environment, and the HydroMg negative hydrogen ion material gradually releases hydrogen; on the other hand, the HydroMg negative hydrogen ion material is pre-coated with polyethylene glycol, which can be highly compatible and highly uniformly dispersed in the wall material solution, and can slow down the impact of the aqueous solution and spray drying process on the HydroMg negative hydrogen ion material, avoiding premature consumption and loss of effective ingredients; in addition, the present invention uses a microcapsule structure as a whole, based on the characteristics of the resistant dextrin wall material, which can effectively target sustained and controlled release, and maximize the effectiveness of the core material.

[0040] After sustained-release microcapsules enter the human body, some body fluids carry a negative charge (such as saliva). Adding bird's nest acid to the core material can enhance the adsorption capacity of positively charged minerals, vitamins, and hydrogen. Sodium hyaluronate can further enhance the stability of sustained-release microcapsules.

[0041] (2) The sustained-release microcapsules contain a variety of active substances, such as compound lactic acid bacteria, which are sensitive to temperature, acid-base environment, etc. and are easily inactivated prematurely during production, transportation, and use. The present invention uses a negative pressure low-temperature spray drying method to quickly form and solidify the microcapsule wall material structure and ensure the stability of the sustained-release microcapsules, while effectively preventing the active substances such as compound lactic acid bacteria in the core material from being decomposed or inactivated due to heat. DETAILED DESCRIPTION

[0042] In order to make the purpose, technical solutions and advantages of the present invention clearer, the present invention will be described in further detail below. Unless otherwise specified, the reagents used in the specific embodiments and examples are all commercially available products.

[0043] A HydroMg negative hydrogen ion sustained-release microcapsule comprising a core material and a wall material, wherein the mass ratio of the core material to the wall material is 1:(1.0-2.5);

[0044] (1) Wall material, including resistant dextrin. Preferably, the wall material also includes a wall material ingredient selected from at least one of gelatin, chitosan, sodium alginate, and lauric acid monoglyceride, and the total mass of the wall material ingredients and the mass ratio of the resistant dextrin are (5-15):10. More preferably, the resistant dextrin, gelatin and sodium alginate are in a mass ratio of 10:(2-6):(2-6), or the resistant dextrin, gelatin, chitosan and lauric acid monoglyceride are compounded in a mass ratio of 10:(2-6):(1-2):(2-5) to provide the wall material. In the present invention, by further adding wall material ingredients to the wall material and regulating the mass ratio of the total mass of the wall material ingredients to the resistant dextrin, the physical and chemical properties of the microcapsules, such as water activity, fluidity, hygroscopicity, and particle size distribution, are improved, and the microcapsules have relatively excellent encapsulation rate and yield;

[0045] (2) The core material, in parts by mass, comprises the following components:

[0046] (2.1) 5-10 parts of magnesium-based hydrogen storage material, wherein the magnesium-based hydrogen storage material is made of magnesium oxide, preferably food-grade magnesium oxide, and undergoes chemical reaction and / or physical adsorption with hydrogen to obtain HydroMg negative hydrogen ion material, which is then prepared by pre-coating treatment, preferably using polyethylene glycol for pre-coating; more preferably, in order to further optimize the hydrogen storage performance of the sustained-release microcapsules, a hydrogen storage auxiliary material can be added to the magnesium-based hydrogen storage material, for example, the hydrogen storage auxiliary material is selected from at least one of magnesium gluconate, yeast beta glucose, and oyster powder, preferably the HydroMg negative hydrogen ion material and the hydrogen storage auxiliary material are mixed in a mass ratio of (10-17):1, and in the hydrogen storage auxiliary material, magnesium gluconate, yeast beta glucose and oyster powder are compounded in a mass ratio of 1:(1-3):(1-3). The pre-coating treatment further comprises the following steps: S1, grinding the hydrogenation reaction product to obtain HydroMg negative hydrogen ion material; S2, dispersing the HydroMg negative hydrogen ion material and optional hydrogen storage auxiliary materials in liquid polyethylene glycol, and vacuum drying;

[0047] (2.2) 10-20 parts of bird's nest acid,

[0048] (2.3) 5-10 parts of sodium hyaluronate,

[0049] (2.4) 5-10 parts of composite lactic acid bacteria, preferably comprising Streptococcus thermophilus and Lactobacillus bulgaricus in a mass ratio of 1:(1-2).

[0050] With respect to the aforementioned HydroMg negative hydrogen ion sustained-release microcapsules, the present invention also provides a preparation method thereof, comprising the following steps:

[0051] S1. Preparation of magnesium-based hydrogen storage materials:

[0052] S1.1 The magnesium oxide powder is heated, hydrogen is introduced, the product is cooled to room temperature, and ground to obtain HydroMg negative hydrogen ion material; the magnesium oxide is preferably made of food-grade magnesium oxide raw material, and the heating temperature can be selected from 400-800°C. At this temperature, the magnesium oxide and hydrogen will undergo chemical reaction and / or physical adsorption, etc., to achieve the hydrogen storage effect; alternatively, the reaction of magnesium oxide and hydrogen can also refer to the process disclosed in CN115428945A;

[0053] S1.2 The HydroMg negative hydrogen ion material and the optional hydrogen storage auxiliary material are dispersed in liquid polyethylene glycol with a molecular weight of 400-600 for pre-coating treatment and vacuum drying; the hydrogen storage auxiliary material is selected from at least one of magnesium gluconate, yeast beta glucose, and oyster powder.

[0054] S2. Preparation of sustained-release microcapsules by negative pressure low-temperature spray drying:

[0055] S2.1 Add the wall material raw materials to deionized water at 60-80°C and stir to obtain a wall material solution. To further enhance the sustained-release performance of the sustained-release microcapsules, an acidity regulator is preferably added to the wall material solution. For example, sodium dihydrogen phosphate is used as the acidity regulator, preferably in an amount of 1-5% by weight of the wall material raw materials.

[0056] S2.2 Adding bird's nest acid and sodium hyaluronate to the wall material solution, homogenizing at high speed, and cooling to room temperature; preferably, the speed of the high-speed homogenizer is 15,000-25,000 rpm, and the high-speed homogenization time is 0.5-5 minutes; preferably, when the temperature drops to 35-45°C, adding collagen peptides at a concentration of 1-5% by weight of sodium hyaluronate with stirring;

[0057] S2.3 Add the composite lactic acid bacteria and the magnesium-based hydrogen storage material to the solution of step S3 in sequence, and homogenize under pressure; preferably, the speed of the pressurized homogenization is 10000-15000 r / min, and the homogenization is performed at 30-50 MPa for 1-3 times;

[0058] S2.4 The material homogenized in step S4 is atomized in a negative pressure drying chamber while introducing dry gas. The vacuum degree in the drying chamber is -0.1 to -0.01 MPa, the air inlet temperature of the drying chamber is 20-40°C, and the air outlet temperature is 10-25°C.

[0059] Through the above-mentioned component configuration and preparation method, the HydroMg negative hydrogen ion sustained-release microcapsules provided by the present invention have excellent properties, including but not limited to: an average particle size of the microcapsules is 5-50 μm, a moisture content is below 3.5 wt%, a water activity is below 0.38 aw, and a microcapsule embedding rate is greater than 90%.

[0060] The sustained-release microcapsules of the present invention can be used in various fields such as food, medicine or skin care products.

[0061] Example 1

[0062] The HydroMg negative hydrogen ion sustained-release microcapsules of this embodiment include a core material and a wall material, and the mass ratio of the core material to the wall material is 1:1.5;

[0063] (1) The wall material is made of resistant dextrin;

[0064] (2) The core material, in parts by mass, comprises the following components:

[0065] (2.1) 8 parts of magnesium-based hydrogen storage material, which is HydroMg negative hydrogen ion material coated with polyethylene glycol;

[0066] (2.2) 16 parts of swan nest acid,

[0067] (2.3) 6 parts of sodium hyaluronate,

[0068] (2.4) 10 parts of compound lactic acid bacteria, including Streptococcus thermophilus and Lactobacillus bulgaricus in a mass ratio of 1:1.

[0069] The method for preparing the sustained-release microcapsules of this embodiment comprises the following steps:

[0070] S1. Preparation of magnesium-based hydrogen storage materials:

[0071] S1.1 Place magnesium oxide powder in a reactor and continue heating to 400°C. Add hydrogen for 12 hours, cool the product to room temperature, and grind it to obtain HydroMg negative hydrogen ion material.

[0072] S1.2 The HydroMg negative hydrogen ion material is dispersed in liquid polyethylene glycol with a molecular weight of 400-450 for pre-coating, and then vacuum dried;

[0073] S2. Preparation of sustained-release microcapsules by negative pressure low-temperature spray drying:

[0074] S2.1 Dissolve the resistant dextrin in 70°C deionized water to obtain a wall material solution;

[0075] S2.2 Add sialic acid and sodium hyaluronate to the wall material solution, homogenize at high speed (20,000 rpm, 3 minutes), and cool to room temperature;

[0076] S2.3 Add the composite lactic acid bacteria and magnesium-based hydrogen storage material to the solution of step S3 in sequence, and homogenize under pressure (speed 15000 r / min, 40 MPa, homogenize twice);

[0077] S2.4 Atomize the material homogenized in step S2.3 in a negative pressure drying chamber while introducing dry gas. The vacuum degree in the drying chamber is -0.1 MPa, the air inlet temperature in the drying chamber is 40°C, and the air outlet temperature is 22±1°C.

[0078] Example 2

[0079] The HydroMg negative hydrogen ion sustained-release microcapsules of this embodiment include a core material and a wall material, and the mass ratio of the core material to the wall material is 1:1.5;

[0080] (1) The wall material is made of resistant dextrin;

[0081] (2) The core material, in parts by mass, comprises the following components:

[0082] (2.1) 8 parts of magnesium-based hydrogen storage material, wherein the HydroMg negative hydrogen ion material and the hydrogen storage auxiliary material are mixed in a mass ratio of 15:1, and the hydrogen storage auxiliary material comprises magnesium gluconate, yeast beta-glucose, and oyster powder in a mass ratio of 1:1:1;

[0083] (2.2) 16 parts of swan nest acid,

[0084] (2.3) 6 parts of sodium hyaluronate,

[0085] (2.4) 10 parts of compound lactic acid bacteria, including Streptococcus thermophilus and Lactobacillus bulgaricus in a mass ratio of 1:1.

[0086] The method for preparing the sustained-release microcapsules of this embodiment comprises the following steps:

[0087] S1. Preparation of magnesium-based hydrogen storage materials

[0088] S1.1 Place magnesium oxide powder in a reactor and continue heating to 400°C. Add hydrogen for 12 hours, cool the product to room temperature, and grind it to obtain HydroMg negative hydrogen ion material.

[0089] S1.2 The HydroMg negative hydrogen ion material and the hydrogen storage auxiliary material are mixed and dispersed in liquid polyethylene glycol with a molecular weight of 400-450 for pre-coating treatment, and vacuum dried;

[0090] S2. Preparation of sustained-release microcapsules by negative pressure low-temperature spray drying:

[0091] S2.1 Dissolve resistant dextrin in 70°C deionized water to obtain a wall material solution; add sodium dihydrogen phosphate (about 2% by weight of the wall material raw material) as an acidity regulator to the wall material solution;

[0092] S2.2 Add sialic acid and sodium hyaluronate to the wall material solution, homogenize at high speed (20,000 rpm, 3 minutes), cool to 40°C, add collagen peptide (approximately 3% by weight of sodium hyaluronate) with stirring, and cool to room temperature;

[0093] S2.3 Add the composite lactic acid bacteria and magnesium-based hydrogen storage material to the solution of step S3 in sequence, and homogenize under pressure (speed 15000 r / min, 40 MPa, homogenize twice);

[0094] S2.4 Atomize the material homogenized in step S2.3 in a negative pressure drying chamber while introducing dry gas. The vacuum degree in the drying chamber is -0.1 MPa, the air inlet temperature in the drying chamber is 40°C, and the air outlet temperature is 22±1°C.

[0095] Example 3

[0096] This embodiment is basically the same as embodiment 2, except that the wall material includes the following components:

[0097] (1.1) 10 parts of resistant dextrin

[0098] (1.2) 5 parts gelatin

[0099] (1.3) 5 parts of sodium alginate.

[0100] In the preparation of sustained-release microcapsules by the negative pressure low-temperature spray drying method, the above wall material raw materials are added into deionized water at 70° C. and stirred to obtain a wall material solution.

[0101] Example 4

[0102] The preparation method of this embodiment is basically the same as that of embodiment 2, except that the wall material includes the following components:

[0103]

[0104] In the preparation of sustained-release microcapsules by the negative pressure low-temperature spray drying method, the above wall material raw materials are added into deionized water at 70° C. and stirred to obtain a wall material solution.

[0105] Example 5

[0106] The preparation method of this embodiment is basically the same as that of embodiment 4, except that the mass ratio of the core material to the wall material is 1:2.

[0107] Comparative Example 1

[0108] The sustained-release microcapsules were prepared according to the steps similar to those in Example 4, except that the pre-coating treatment of the HydroMg negative hydrogen ion material and the hydrogen storage auxiliary material was omitted. In the preparation of the sustained-release microcapsules by the negative pressure low-temperature spray drying method, the HydroMg negative hydrogen ion material and the hydrogen storage auxiliary material were directly added to the corresponding wall material solution.

[0109] Comparative Example 2

[0110] The sustained-release microcapsules were prepared according to the steps similar to those in Example 4, except that a conventional spray drying method was used with the following parameters: inlet air temperature of 120-200°C and outlet air temperature of 80-90°C.

[0111] Performance test and method:

[0112] (1) Average particle size: The particle size of the microcapsules was measured using a laser particle size analyzer, with the particle refractive index set to 1.414 and the particle absorptivity set to 0.001, and pure water used as the dispersant.

[0113] (2) Water content: The water content of the microcapsules was measured using a moisture meter. Weigh 0.50 g of microcapsule sample and place it in the sample tray of the instrument. Set the instrument temperature to 105°C, set the timer to automatic (until dried to constant weight), and read the value. Each sample was measured three times, and the average value was taken for comparison. The water content was calculated as follows: Water content of microcapsules (%) = (M-M1) ÷ M × 100%; where: M is the original mass of the microcapsules (g); M1 is the mass of the microcapsules dried to constant weight at 105°C (g).

[0114] (3) Water activity: The water activity of the sample was measured at 25°C using a water activity meter. The measurements were repeated three times and the average value was taken.

[0115] (4) Lactic acid bacteria entrapment survival rate: 0.5 g of microcapsule sample was weighed and added to 30 mL of sterilized encapsulation solution (0.1 mol / L Na2 HPO4 and 0.05 mol / L citric acid were accurately prepared, adjusted to pH = 7.25, and sterilized at 121°C for 15 min before use). The solution was shaken at 37°C for 2-3 h at a speed of 180 rpm to completely release the bacteria. 1 mL was then transferred from the solution for gradient dilution. The viable bacteria were counted using the agar medium pouring culture method. The lactic acid bacteria entrapment survival rate in the microcapsules was calculated according to the following formula:

[0116] Lactic acid bacteria encapsulation survival rate (%) = number of viable bacteria in microcapsules / number of viable bacteria initially added × 100%

[0117] (5) HydroMg effective embedding rate: During the (4) lactic acid bacteria embedding survival rate test, the hydrogen concentration of the microcapsules was measured using a hydrogen concentration tester. After converting the hydrogen mass, the effective embedding rate of HydroMg was estimated according to the following formula:

[0118]

[0119] Where M H2 To measure the mass of hydrogen, M MgH2 is the initial mass of HydroMg negative hydrogen ion material.

[0120] (5) Gastric acid resistance test: Weigh 0.5 g of microcapsule sample and place it in 10 mL of artificial gastric juice (16.4 mL of hydrochloric acid, 10 g of pepsin, add water and stir to 1000 mL, pH 1.2). Incubate with shaking at 37°C. Every 0.5 h, transfer the sample solution to the encapsulation fluid and incubate with shaking for 2 h to allow the bacteria to be completely released. Transfer 1 mL of the solution for gradient dilution and use the agar medium pouring culture method to count the viable bacteria. After 2.5 h of digestion in gastric juice:

[0121] △: The number of viable bacteria decreased by less than 1%, and the bacteria were well resistant to gastric acid.

[0122] ○: The number of viable bacteria is reduced by 1-5%, and the bacteria can better tolerate the effects of gastric acid;

[0123] ×: The number of viable cells decreased by more than 5%.

[0124] (6) Intestinal fluid release test: Weigh 0.5 g of microcapsule sample and place it in 30 mL of simulated intestinal fluid (dissolve 6.8 g of potassium dihydrogen phosphate in 500 mL of water and adjust the pH to 6.8 with 0.4% sodium hydroxide solution; dissolve 10 g of pancreatic enzyme in an appropriate amount of water, mix the two solutions and add water to 1000 mL). Incubate at 37°C with shaking for 2.5 h. Every 0.5 h, 1 mL of the sample solution was removed for serial dilution counting to determine the number of viable bacteria released into the simulated intestinal fluid. The results showed that after 1.5 h:

[0125] ▲: The number of viable bacteria is greater than 10 9 cfu / mL;

[0126] ●:Viable bacteria count 10 8 -10 9 cfu / mL;

[0127] ×: Viable bacteria count is less than 10 8 cfu / mL.

[0128] Table 1 Test results of Examples 1-5 and Comparative Examples 1-2

[0129]

[0130] According to the test results, the samples of the Examples and Comparative Examples all met the requirements for chemical and physical stability, such as a water content of less than 4% and a water activity of less than 0.4aw, meeting the storage requirements and having good gastric acid resistance, indicating that the material selection and preparation methods of the present invention are generally more scientific. Among them, the average particle size of Examples 3-5 using composite wall materials increased relatively, mainly because some components of the wall materials have slightly higher hygroscopicity, resulting in better fluidity and adhesion. The use of monoglyceride of laurate helps improve the stability of the microcapsules, resulting in lower water activity and better storage stability in Examples 4 and 5.

[0131] The present invention uses polyethylene glycol to coat HydroMg, further reducing premature loss of HydroMg from solvent contact during spray drying. Consequently, the final measured effective encapsulation efficiency of HydroMg is significantly improved. The present invention employs negative pressure, low-temperature spray drying to form microcapsules. While the preparation speed is slightly slower than high-temperature drying, it is more effective in protecting active ingredients such as lactic acid bacteria, resulting in a better encapsulated survival rate for lactic acid bacteria and relatively better effective intestinal fluid release.

[0132] The above introduces the preferred embodiments of the present invention, which is intended to make the spirit of the present invention clearer and easier to understand, and is not intended to limit the present invention. Any modifications, replacements, and improvements made within the spirit and principles of the present invention should be included in the scope of protection outlined by the claims attached to the present invention.

Claims

1. A HydroMg negative hydrogen ion sustained-release microcapsule, characterized in that: Including core material and wall material, the mass ratio of core material to wall material is 1: (1.0-2.5); The wall material includes resistant dextrin; The core material comprises the following components in parts by mass: The magnesium-based hydrogen storage material is prepared by reacting a magnesium oxide raw material with hydrogen to obtain a HydroMg negative hydrogen ion material, and then pre-coating the HydroMg negative hydrogen ion material. The pre-coating process includes the following steps: Grinding HydroMg negative hydrogen ion material; The HydroMg negative hydrogen ion material is dispersed in liquid polyethylene glycol and vacuum dried; The microcapsules are prepared by a negative pressure low-temperature spray drying method.

2. The sustained-release microcapsule according to claim 1, wherein The composite lactic acid bacteria comprises thermophilic streptococcus and bulgaricus lactobacillus in a mass ratio of 1: (1-2).

3. The sustained-release microcapsule according to claim 1, wherein The wall material also includes wall material ingredients, which are selected from at least one of gelatin, chitosan, sodium alginate, and monoglyceride of lauric acid, and the total mass ratio of the wall material ingredients to the mass of the resistant dextrin is (5-15):

10.

4. The sustained-release microcapsule according to any one of claims 1 to 3, characterized in that The negative pressure low temperature spray drying method comprises the following steps: (1): Add the wall material raw materials into 60-80℃ deionized water and stir to obtain a wall material solution; (2): Add bird's nest acid and sodium hyaluronate to the wall material solution, homogenize at high speed, and cool to room temperature; (3): Adding the composite lactic acid bacteria and the magnesium-based hydrogen storage material to the solution of step (2) in sequence, and pressurizing and homogenizing; (4): The material homogenized in step (3) is atomized in a negative pressure drying chamber, and a 20-40°C drying gas is introduced for spray drying.

5. The sustained-release microcapsule according to claim 4, characterized in that Before step (2), sodium dihydrogen phosphate (1-5% by weight of the wall material raw material) is added to the wall material solution; when the temperature in step (2) drops to 35-45° C., collagen peptide (1-5% by weight of the sodium hyaluronate) is added with stirring.

6. The sustained-release microcapsule according to claim 5, characterized in that The magnesium-based hydrogen storage material further includes a hydrogen storage auxiliary material selected from at least one of magnesium gluconate, yeast beta-glucose, and oyster powder; and the pre-coating process includes the following steps: (1) Grinding HydroMg negative hydrogen ion material; (2) Dispersing the HydroMg negative hydrogen ion material and hydrogen storage auxiliary materials in liquid polyethylene glycol and vacuum drying.

7. The sustained-release microcapsule according to claim 5 or 6, characterized in that The average particle size of the microcapsules is 5-50 μm, the moisture content is below 3.5 wt%, the water activity is below 0.38 aw, and the microcapsule embedding rate is greater than 90%.

8. A method for preparing the sustained-release microcapsules according to any one of claims 1 to 7, characterized in that: The following steps are involved: S1. Preparation of magnesium-based hydrogen storage materials: S1.1 Heat magnesium oxide powder, introduce hydrogen, cool the product to room temperature, and grind it to obtain HydroMg negative hydrogen ion material; S1.2 The HydroMg negative hydrogen ion material is dispersed in liquid polyethylene glycol with a molecular weight of 400-600 for pre-coating, and vacuum dried; S2. Preparation of sustained-release microcapsules by negative pressure low-temperature spray drying: S2.1 Add the wall material raw materials into 60-80℃ deionized water and stir to obtain a wall material solution; S2.2 Add sialic acid and sodium hyaluronate to the wall material solution, homogenize at high speed, and cool to room temperature; S2.3 Add the composite lactic acid bacteria and magnesium-based hydrogen storage material to the solution of step S2.2 in sequence and homogenize under pressure; S2.4 Atomize the material homogenized in step S2.3 in a negative pressure drying chamber while introducing dry gas. The vacuum degree in the drying chamber is -0.1 to -0.01 MPa, the air inlet temperature in the drying chamber is 20-40°C, and the air outlet temperature is 10-25°C.

9. The preparation method according to claim 8, wherein The speed of the high-speed homogenizer is 15000-25000 rpm, and the time of high-speed homogenization is 0.5-5 minutes; the speed of the pressurized homogenizer is 10000-15000 r / min, and the homogenization is performed at 30-50 MPa for 1-3 times.

10. Use of the sustained-release microcapsule according to any one of claims 1 to 7 in food, medicine or skin care products.

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