Preparation method of glycine magnesium particles and application thereof

Abstract

This invention discloses a method for preparing magnesium glycinate granules and its application, relating to the field of magnesium glycinate granulation technology. The method uses polyvinyl alcohol and polyvinyl alcohol as binders for wet granulation. Polyvinyl alcohol is prepared into a 10% concentration slurry. Magnesium glycinate and polyvinyl alcohol are mixed evenly in a wet granulator, and the 10% concentration polyvinyl alcohol slurry is added for further wet granulation. The resulting granules are then subjected to fluidized bed drying in a dryer. The dried granules are then sieved to obtain the finished magnesium glycinate granules. This invention, by optimizing the use of binders, effectively avoids the Maillard reaction of magnesium glycinate during storage and shelf life, maintaining product stability and appearance while improving product quality and market competitiveness. The magnesium glycinate granules using this invention exhibit significantly improved compressibility, resulting in high-strength tablets suitable for mass production.

Description

Technical Field

[0001] This invention relates to the field of glycine magnesium particle preparation technology, and in particular to a method for preparing glycine magnesium particles and its application. Background Technology

[0002] Magnesium glycinate, with the molecular formula Mg(C2H4NO2)2·H2O and a molecular weight of 190.44, is a white powder, readily soluble in water but sparingly soluble in ethanol. It is a common organomagnesium salt widely used in the food, beverage, and pharmaceutical industries as a buffer, stabilizer, and flavoring agent. It is also used in the production of some pharmaceuticals, such as antibiotics and antiviral drugs.

[0003] Magnesium glycinate plays multiple roles in the body, including participating in protein synthesis, regulating neurotransmitters, protecting the heart, and maintaining bone health. Magnesium glycinate increases the body's absorption and utilization of magnesium by forming soluble compounds with magnesium ions in the body. Magnesium is an important cofactor in many enzymatic reactions, participating in processes such as protein synthesis and nerve conduction, and playing a crucial role in maintaining normal physiological functions. Magnesium deficiency may lead to symptoms such as muscle cramps and fatigue; excessive intake may cause digestive discomfort such as diarrhea and nausea. These symptoms may vary from person to person.

[0004] Magnesium glycinate helps with carbohydrate metabolism, and the magnesium it contains can improve insulin sensitivity, thus reducing the risk of diabetes to some extent. Secondly, magnesium glycinate can regulate brain function and has a calming and sleep-inducing effect. Magnesium glycinate should generally be taken under the guidance of a professional physician. As a dietary supplement, it is not a treatment, so long-term use is not recommended. If you experience any discomfort after taking it, it is advisable to seek medical attention promptly.

[0005] In existing technologies, magnesium glycine is typically produced by direct compression into tablets or by dry granulation.

[0006] Chinese patent publication CN109608349A discloses a green preparation method for magnesium glycinate, belonging to the field of magnesium supplementation technology. The method includes the following steps: A. Adding glycinate and water to a reaction vessel and heating to dissolve the glycinate; B. Adding magnesium hydroxide when the temperature reaches 83-87°C, reacting for 2-3 hours, and then filtering to remove insoluble matter to obtain a filtrate; C. Cooling the filtrate to room temperature and then filtering again to obtain wet magnesium glycinate and a circulating mother liquor; D. Vacuum drying the wet magnesium glycinate to obtain the final product, magnesium glycinate.

[0007] Chinese patent publication CN113121375A discloses a method and apparatus for preparing food-grade and feed-grade magnesium glycinate. The method involves contacting a mother liquor from the hydantoin process for glycine crystallization with a zirconium feedstock in the presence of one or more magnesium compounds selected from magnesium oxide, magnesium hydroxide, and magnesium carbonate to perform hydrolysis and chelation reactions, yielding an aqueous solution of magnesium glycinate. This solution is then concentrated and cooled to crystallize, resulting in a solid precipitate of food-grade magnesium glycinate, and co-producing feed-grade magnesium glycinate. The purity of the obtained food-grade magnesium glycinate can reach over 98.0%, and the glycine recovery rate can reach over 99%.

[0008] Chinese patent publication CN113321592A discloses a method for preparing magnesium glycine. The method includes: pretreating glycine and magnesium hydroxide or magnesium oxide; adding glycine to a solid-phase reactor; adding magnesium hydroxide or magnesium oxide in three portions to the solid-phase reactor under certain conditions at a molar ratio of 2:(0.6-1):(0.08-0.4); including: adding magnesium hydroxide or magnesium oxide at a molar ratio of 2, grinding and reacting for 20-40 minutes; adding magnesium hydroxide or magnesium oxide at a molar ratio of (0.6-1), grinding and reacting for 50-70 minutes; adding magnesium hydroxide or magnesium oxide at a molar ratio of (0.08-0.4), grinding and reacting for 30-50 minutes; washing the product after the reaction with ethanol and drying to obtain magnesium glycine.

[0009] The above-mentioned preparation method of magnesium glycine has the following disadvantages: 1) Insufficient compressibility: magnesium glycine has poor compressibility, resulting in insufficient strength of the finished tablets, which affects mass production; 2) Maillard reaction problem: magnesium glycine is prone to Maillard reaction during storage and shelf life, which leads to discoloration and affects the stability and appearance of the product. Summary of the Invention

[0010] The purpose of this invention is to provide a method for preparing glycine magnesium granules with good compressibility, high tablet strength, and resistance to discoloration, and its application. By adding a suitable binder to wet granulate the glycine magnesium raw material, the compressibility of glycine magnesium is improved, so that the strength of the compressed glycine magnesium tablets (magnesium content 125mg) can be used for large-scale (800kg) coating, thereby improving production efficiency. At the same time, by selecting a suitable binder, the problem of discoloration caused by Maillard reaction during storage, shelf life, and accelerated stabilization of glycine magnesium is solved, thereby improving the stability and appearance of the product.

[0011] To achieve the above-mentioned technical objectives and requirements, the technical solution adopted by this invention is: a method for preparing magnesium glycinate particles, using polyvinyl ketone and polyvinyl alcohol as binders for wet granulation, the preparation method specifically including the following steps:

[0012] Step 1: Prepare the raw materials: magnesium glycine, polyvinyl alcohol, and mix them together.

[0013] Step 2: Prepare a 10% concentration slurry from polyvinyl alcohol; mix magnesium glycine and povidone in a wet granulator, add the 10% concentration polyvinyl alcohol slurry to prepare the slurry, and then perform wet granulation.

[0014] Step 3: Place the prepared granules into a dryer for fluidized bed drying until the moisture content of the granules is below 2%;

[0015] Step 4: After drying, the granules are sized through a 16-mesh or 20-mesh sieve to obtain the finished glycine magnesium granules.

[0016] Preferably, the mass ratio of polyvinyl alcohol to polyvinyl alcohol is 1:1 to 3:1, preferably 2:1.

[0017] A method for preparing glycine magnesium particles was used to prepare glycine magnesium particles.

[0018] Magnesium glycinate particles were used in the preparation of Magnesium Glycinate Tablets.

[0019] Stability tests were conducted on the prepared magnesium glycinate particles and magnesium glycinate flakes under different storage conditions.

[0020] Stability test storage conditions for magnesium glycinate particles: ① The prepared particles were dried at 80℃ to constant weight, and no discoloration occurred under high temperature and high humidity conditions; ② The dried particles were exposed to 40℃ and 75% humidity for 1 month and no discoloration reaction occurred.

[0021] Stability test storage conditions for magnesium glycinate tablets: ① The prepared tablets were exposed to 40℃ and 75% humidity for 1 month and no discoloration reaction occurred; ② The prepared tablets were packed into HDPE high-density polyethylene bottles and observed at 40℃ and 75% humidity for 6 months and no discoloration reaction occurred.

[0022] Compared with the traditional structure, the beneficial effects of the present invention are as follows:

[0023] 1. This invention optimizes the use of adhesives, employing polyvinyl alcohol and polyvinyl alcohol as adhesives, effectively preventing the Maillard reaction of magnesium glycinate during storage and shelf life. This not only maintains the stability and appearance of the product but also improves its quality and market competitiveness. The magnesium glycinate granules provided by this invention have significantly improved compressibility, resulting in high-strength tablets that can be mass-produced.

[0024] 2. The preparation process of this invention is simple, requires little equipment investment, and has low production costs. It not only improves the compressibility of magnesium glycine and avoids the Maillard reaction, but also maintains the stability and appearance of the product, demonstrating significant advantages. Detailed Implementation

[0025] The present invention will be further illustrated below using glycine magnesium granules with an effective ingredient content of 90.28% as an example.

[0026] The particle size distribution of 90.28% glycine magnesium granules is shown in Table 1:

[0027] Table 1. Indicators of Magnesium Glycine Particles

[0028] project index Appearance White to off-white granules or particulate powder Moisture 1.5%-2.0% (Detection temperature: 105℃) Particle size distribution <10% on 20 mesh, <30% on 100 mesh

[0029] Example 1: Polyvinyl alcohol was made into a 10% concentration slurry. Magnesium glycine and hydroxypropyl methylcellulose (HPMC) were put into a wet granulator and mixed for 5 minutes. The slurry-mixing agent (10% PVA polyvinyl alcohol) was added for wet granulation. The resulting granules were put into a dryer for drying. The dried granules were passed through a 16 or 20 mesh sieve.

[0030] The resulting 90.28% glycine magnesium granules are off-white granular powder with a moisture content of 1.81%. After sieving, the moisture content is 7% for particles larger than 20 mesh and 24% for particles smaller than 100 mesh.

[0031] The prepared 90.28% glycine magnesium granules were subjected to stability tests under different storage conditions. The results showed that the granules using hydroxypropyl methylcellulose (HPMC) and polyvinyl alcohol as binders did not undergo Maillard reaction during the test and could proceed to the next step of tableting test.

[0032] 90.28% magnesium glycinate granules were used in the preparation of Magnesium Glycinate Tablets, and the formulation is shown in Table 2:

[0033] Table 2 Formulations for preparing glycine magnesium tablets using glycine magnesium particles

[0034] Serial Number Material Name Dosage per 10,000 tablets (g) Dosage ratio (%) 1 90.28% glycine magnesium granules 13095.47 91.385 2 microcrystalline cellulose 1104.53 7.708 3 magnesium stearate 80.000 0.558 4 silicon dioxide 50.000 0.349 total 14330.00 100.000

[0035] The prepared magnesium glycine sheets were tested using instruments such as a hardness tester and a friability tester. The results are shown in Table 3.

[0036] Table 3. Data on glycine magnesium flakes prepared using glycine magnesium particles from Example 1

[0037] Serial Number Indicator Name data 1 Average hardness (N) 200N 2 Friability (%) 0.18 3 Disintegration timeout (min, with baffle) 23 4 Difference in slice weight -0.82%~+0.71% 5 Number of free-fall fragments (20 pieces) 0

[0038] As shown in the table above, the glycine magnesium flakes prepared using glycine magnesium particles with hydroxypropyl methylcellulose (HPMC) and polyvinyl alcohol as binders have an average hardness of 200N, and this product can achieve large-scale coating of 700kg / batch.

[0039] The prepared magnesium glycine tablets were subjected to stability tests under different storage conditions. The results showed that the tablets using hydroxypropyl methylcellulose (HPMC) and polyvinyl alcohol as binders did not undergo Maillard reaction during storage and shelf life, and maintained good stability and appearance.

[0040] Example 2: Polyvinyl alcohol was made into a 10% concentration slurry. Magnesium glycine and methyl cellulose (MC) were put into a wet granulator and mixed for 5 minutes. Slurry-mixing (10% PVA polyvinyl alcohol) was added for wet granulation. The resulting granules were put into a dryer for drying. The dried granules were passed through a 16 or 20 mesh sieve.

[0041] The resulting 90.28% glycine magnesium granules are white granules with a moisture content of 1.78%. After sieving, the moisture content is 6% for particles larger than 20 mesh and 25% for particles smaller than 100 mesh.

[0042] The prepared 90.28% glycine magnesium granules were subjected to stability tests under different storage conditions. The results showed that the granules using methyl cellulose (MC) and polyvinyl alcohol as binders did not undergo Maillard reaction during the test and could proceed to the next step of tableting test.

[0043] Magnesium glycinate granules (90.28%) were used in the preparation of Magnesium Glycinate Tablets, with the same formulation as in Example 1. The tablet performance data are shown in Table 4.

[0044] Table 4. Data on glycine magnesium flakes prepared using glycine magnesium particles from Example 2

[0045] Serial Number Indicator Name data 1 Average hardness (N) 220N 2 Friability (%) 0.18 3 Disintegration timeout (min, with baffle) 13 4 Difference in slice weight -0.55%~+0.91% 5 Number of free-fall fragments (20 pieces) 0

[0046] As shown in the table above, the glycine magnesium flakes prepared using glycine magnesium particles with methyl cellulose (MC) and polyvinyl alcohol as binders have an average hardness of 220 N, and the product can achieve large-scale coating of 770 kg / batch.

[0047] The prepared magnesium glycine tablets were subjected to stability tests under different storage conditions. The results showed that the tablets using methylcellulose (MC) and polyvinyl alcohol as binders did not undergo Maillard reaction during storage and shelf life, and maintained good stability and appearance.

[0048] Example 3: Polyvinyl alcohol was prepared into a 10% concentration slurry. Magnesium glycine and maltodextrin were placed in a wet granulator and mixed for 5 minutes. The slurry-mixing agent (10% PVA polyvinyl alcohol) was then added for wet granulation. The resulting granules were placed in a dryer for drying and then passed through a 16 or 20 mesh sieve.

[0049] The resulting 90.28% glycine magnesium granules are white granules with a moisture content of 1.77%. After sieving, the moisture content is 5% for particles larger than 20 mesh and 23% for particles smaller than 100 mesh.

[0050] The stability of the prepared 90.28% glycine magnesium granules was tested under different storage conditions. The results showed that the granules using maltodextrin and polyvinyl alcohol as binders changed color slightly during the test and underwent Maillard reaction, so there was no need to conduct tableting tests.

[0051] Example 4: Polyvinyl alcohol was prepared into a 10% concentration slurry. Magnesium glycine and povidone (K30) were placed in a wet granulator and mixed for 5 minutes. The slurry-mixing agent (10% PVA polyvinyl alcohol) was then added for wet granulation. The resulting granules were placed in a dryer for drying and then passed through a 16 or 20 mesh sieve.

[0052] The resulting 90.28% glycine magnesium granules are white granules with a moisture content of 1.63%. After sieving, the moisture content is 4% for particles larger than 20 mesh and 22% for particles smaller than 100 mesh.

[0053] The prepared 90.28% glycine magnesium granules were subjected to stability tests under different storage conditions. The results showed that the granules using polyvinylpyrrolidone (K30) and polyvinyl alcohol as binders did not undergo Maillard reaction during the test and could proceed to the next step of tableting test.

[0054] Magnesium glycinate granules (90.28%) were used in the preparation of Magnesium Glycinate Tablets, with the same formulation as in Example 1. The tablet performance data are shown in Table 5.

[0055] Table 5. Data on glycine magnesium flakes prepared using glycine magnesium particles from Example 4

[0056] Serial Number Indicator Name data 1 Average hardness (N) 250N 2 Friability (%) 0.10 3 Disintegration timeout (min, with baffle) 14 4 Difference in slice weight -0.42%~+0.59% 5 Number of free-fall fragments (20 pieces) 0

[0057] As shown in the table above, the glycine magnesium flakes prepared using glycine magnesium particles with polyvinyl alcohol as binders have an average hardness of 250N, and this product can achieve large-scale coating of 800kg / batch.

[0058] The prepared magnesium glycine tablets were subjected to stability tests under different storage conditions. The results showed that the tablets using povidone and polyvinyl alcohol as binders did not undergo Maillard reaction during storage and shelf life, and maintained good stability and appearance.

[0059] Example 5: Polyvinyl alcohol was prepared into a 10% concentration slurry. Magnesium glycine and copolyvinyl ketone (PVA / A) were placed in a wet granulator and mixed for 5 minutes. The slurry-mixing agent (10% PVA polyvinyl alcohol) was then added for wet granulation. The resulting granules were placed in a dryer for drying, and the dried granules were passed through a 16 or 20 mesh sieve.

[0060] The resulting 90.28% glycine magnesium granules are white granules with a moisture content of 1.66%. After sieving, the moisture content is 6% for particles larger than 20 mesh and 25% for particles smaller than 100 mesh.

[0061] The prepared 90.28% glycine magnesium granules were subjected to stability tests under different storage conditions. The results showed that the granules using copovidone (PVA / A) and polyvinyl alcohol as binders underwent slight discoloration and Maillard reaction during the test, making tableting tests unnecessary.

[0062] As can be seen from Examples 1-5 above, when maltodextrin and copovidone (PVA / A) are used as binders, magnesium glycine particles will undergo Maillard reaction, and these two binders are not suitable for the preparation of magnesium glycine particles.

[0063] When using polyvinylpyrrolidone (K30), hydroxypropyl methylcellulose (HPMC), methylcellulose (MC), and polyvinyl alcohol (PVA) as adhesives, no Maillard reaction occurred during storage and shelf life, maintaining good stability and appearance, resulting in the best performance.

[0064] As shown in Example 4, when polyvinyl alcohol (PVA) and polyvinyl alcohol (PVA) are used as binders, the glycine magnesium tablets prepared from glycine magnesium particles have the highest average hardness and the lowest brittleness. The tablets produced are superior to those in other examples, and can achieve large-scale coating of 800 kg / batch, thus greatly improving production efficiency.

[0065] In summary, through comparison of production efficiency, the most suitable binders were selected: povidone and polyvinyl alcohol. Using povidone (K30) and polyvinyl alcohol (PVA) as binders for wet granulation not only improved the compressibility and production efficiency of magnesium glycinate, but also ensured that the product did not undergo Maillard reaction during storage and shelf life, while maintaining good stability and appearance.

[0066] The above embodiments of the present invention are merely examples to clearly illustrate the present invention, and are not intended to limit the scope of protection of the present invention. All equivalent technical solutions also fall within the scope of the present invention, and the patent protection scope of the present invention should be defined by the claims.

Claims

1. A method for preparing magnesium glycine particles, characterized in that: Wet granulation is performed using polyvinyl chloride and polyvinyl alcohol as binders, wherein the mass ratio of polyvinyl chloride to polyvinyl alcohol is 1:1 to 3:

1. The preparation method specifically includes the following steps: Step 1: Prepare the raw materials: magnesium glycine, polyvinyl alcohol, and polyvinyl alcohol, and mix them together; Step 2: Prepare a 10% concentration slurry from polyvinyl alcohol; mix magnesium glycine and povidone in a wet granulator, add the 10% concentration polyvinyl alcohol slurry to prepare the slurry, and then perform wet granulation. Step 3: Place the prepared granules into a dryer for fluidized bed drying until the moisture content of the granules is below 2%; Step 4: After drying, the granules are sized through a 16-mesh or 20-mesh sieve to obtain the finished glycine magnesium granules.

2. A magnesium glycine granule, characterized in that: The glycine magnesium particles prepared by the method described in claim 1 did not undergo Maillard reaction during storage and shelf life.

3. An application of magnesium glycine granules, characterized in that: Using the glycine magnesium granules described in claim 2 to prepare glycine magnesium sheets, the resulting glycine magnesium sheets have an average hardness of 250N and can achieve batch coating production of 800kg / batch.