JP6789297B2 - Magnesium oxide granules - Google Patents

Description

The present invention relates to magnesium oxide granules and tablets containing magnesium oxide granules.

Magnesium oxide is widely used in various industrial fields such as pharmaceuticals, foods, vulcanization accelerators, pigments for paints and inks, and in particular, magnesium oxide tablets are widely used as pharmaceutical laxatives and mineral supplements. It has been used (for example, Patent Documents 1 to 3).

Generally, tablets are manufactured by compression molding raw materials into tablets. Further, this compression molding process is called a locking process. In the locking process, the compression operation is continuous and performed at high speed. Under such conditions, stress and density are distributed inside the tablet, and the internal structure is never uniform, which is considered to be the main cause of tableting failure and abnormal quality characteristics. ..

The locking obstacles include capping, laminating, sticking, picking and the like. Capping is a phenomenon in which a tablet is ejected from a mortar after molding, or the tablet is exfoliated like a hat after being ejected, and laminating is a phenomenon in which capping becomes worse and the tablet is exfoliated in layers along the side surface instead of the upper surface of the tablet. Is. Sticking is a phenomenon in which powder adheres to a pestle (compression rod) during a compression stroke and damages the tablet surface as if it were dented, and chipping is also a phenomenon in which the tablet surface is slightly damaged for the same reason. These locking disorders occur mainly due to the nature of the raw materials.

In addition, as the quality characteristic abnormality, there is a state in which the tablet is cracked, chipped, powdered off, or the like even under normal use conditions. Such abnormal quality characteristics occur mainly due to insufficient strength (hardness) of tablets.

Also in the production of magnesium oxide tablets, when magnesium oxide having a particularly high purity is used as a raw material, there is a problem that the above-mentioned tableting obstacles and abnormal quality characteristics are likely to occur.

Under these circumstances, Patent Document 4 describes that tableting disorders and tablet strength can be improved by setting the specific surface area and activity of magnesium oxide granules for addition to pharmaceuticals and foods within a specific range.

It should be noted that magnesium oxide is particularly high as magnesium oxide when it is assumed that it is directly or indirectly ingested by the human body or comes into contact with the human body, such as fertilizers, foods, cosmetics, and pharmaceutical raw materials. Purity is desired.

Japanese Unexamined Patent Publication No. 2003-1468889 WO2011 / 030659 Pamphlet JP-A-2009-13113 WO2015 / 128940 Pamphlet

An object of the present invention is to provide a tablet containing magnesium oxide (granule) having excellent elution property, a method for producing the same, and the magnesium oxide (granule).

Another object of the present invention is to provide magnesium oxide (granule) having few manufacturing defects (chips, cracks, etc.), a method for producing the same, and a tablet containing the magnesium oxide (granule).

Still another object of the present invention is to provide a tablet containing magnesium oxide (granule), a method for producing the same, and the magnesium oxide (granule), which can improve elution and manufacturing defects while maintaining high purity.

Another object of the present invention is to provide a method for efficiently producing magnesium oxide (granule) as described above.

The present inventors examined magnesium oxide granules of Patent Document 4, and found that there is room for improvement in dissolution property, which is an important property of tablets. It was also found that there is room for further improvement in terms of chipping and cracking of tablets.

On the other hand, as described above, high purity is particularly required for pharmaceuticals and food applications, but according to the studies by the present inventors, there is a relationship between the amount of impurities and the elution property and manufacturing defects. It was found that it is difficult to improve elution and manufacturing defects simply by reducing the amount of impurities to a high level.

Under these circumstances, as a result of diligent research conducted by the present inventors in order to solve the above problems, surprisingly, among various elements other than magnesium in magnesium oxide (MgO) granules, B (boron) and Ca Finding out that (calcium) is related to elution and manufacturing defects, adjusting the content of these to a specific range, and not dare to make it ultra-high purity of over 99%, it is sufficiently pharmaceutical. We have found that the elution of magnesium oxide and manufacturing defects can be efficiently improved in tablets by adjusting the purity to a predetermined high purity range that can be applied to applications (particularly, both of these can be improved), and further studies will be conducted. The present invention was completed again.

That is, in the present invention, the content of B (boron) is 0.05% by weight or less, the content of Ca (calcium) is 0.03 to 1.8% by weight, and the pure content (Assay) is 95 to 99%. Includes magnesium oxide (granule).

In such magnesium oxide, the BET specific surface area may be, for example, about 5 to 60 m ² / g.

Typical magnesium oxides of the present invention have a B content of 0.03% by weight or less, a Ca content of 0.05 to 1.5% by weight, a pure content (Assay) of 96 to 99%, and BET. It contains magnesium oxide (granule) having a specific surface area of 10 to 50 m ² / g.

Magnesium oxide may be derived from seawater.

In addition, the present invention has been selected from applications (for example, food, pharmaceutical, and cosmetics) that satisfy the following (1) and / or (2) and are directly or indirectly ingested or contacted with an animal. Includes magnesium oxide (granule) for use in at least one application).
(1) B content is 0.05% by weight or less (2) Ca content is 0.03 to 1.8% by weight

The pure content (Assay) of such magnesium oxide may be particularly about 95 to 99%.

The present invention also includes a method for producing the above-mentioned magnesium oxide (granule). Such a method may include at least a step of removing B from seawater. In such a method, B may be removed from seawater with a chelate resin.

The present invention also includes tablets containing the magnesium oxide (granule).

In the present invention, magnesium oxide and tablets containing the same can be improved by adjusting the content of B, the content of Ca, and the pure content.
Therefore, the present invention also includes, for example, the following methods.

A method for adjusting the content of B in magnesium oxide (granule) to 0.05% by weight or less to improve or improve the elution of tablets containing magnesium oxide granules.

A method for adjusting the Ca content in magnesium oxide (granule) to 0.03 to 1.8% by weight to reduce manufacturing defects (for example, chipping and / or cracking of tablets) of tablets containing magnesium oxide (granule). ..

The content of B in magnesium oxide (granule) was adjusted to 0.03% by weight or less, the content of Ca was adjusted to 0.05 to 1.5% by weight, and the pure content (Assay) was adjusted to 95 to 99%. A method for improving or improving the dissolution property of a tablet containing (granule) and reducing manufacturing defects (for example, chipping and / or cracking of the tablet).

In the present invention, magnesium oxide (granule) having excellent elution property can be provided.

In addition, the present invention can also provide magnesium oxide (granule) with few manufacturing defects (chips, cracks, etc.).

In particular, such magnesium oxide can improve elution and manufacturing defects while maintaining high purity (95% or more, preferably 96% or more). Further, even if the dissolution property and the production defect are improved, the tablet hardness is not impaired, and the improvement of the dissolution property and the production defect and the high hardness can be achieved at the same time.

Therefore, the magnesium oxide and magnesium oxide tablets of the present invention are particularly useful in applications (for example, fertilizers, foods, pharmaceuticals, cosmetics, etc.) in which they are directly or indirectly ingested or contacted with animals (particularly humans).

Further, the present invention can provide a method for efficiently producing magnesium oxide (granule) as described above. In particular, in such a method, since a raw material such as seawater can be used, it can be manufactured easily (and inexpensively), and is extremely useful and practical.

[Magnesium oxide]
The magnesium oxide of the present invention satisfies a specific B (boron) and / or Ca (calcium) content.

The content (content ratio) of B in magnesium oxide is, for example, 0.1% by weight or less (for example, 0.08% by weight or less), preferably 0.05% by weight or less (for example, 0.04% by weight or less). ), More preferably 0.03% by weight or less (for example, 0.02% by weight or less), particularly 0.015% by weight or less.

The lower limit of the B content is not particularly limited, and may be, for example, 0% by weight (or detection limit), such as 0.00001% by weight, 0.0001% by weight, 0.001% by weight, and the like. It may be.
In addition, you may set an appropriate range by appropriately combining these numerical values (for example, 0.00001 to 0.05% by weight, etc., the same applies to the description of numerical values below).

The content (content ratio) of Ca in magnesium oxide can be selected from the range of, for example, 0.03% by weight or more (for example, 0.03 to 2% by weight), and 0.03 to 1.8% by weight (for example). , 0.04 to 1.6% by weight), preferably 0.05 to 1.5% by weight (for example, 0.08 to 1.5% by weight), still more preferably 0.1 to 1.5% by weight (. For example, it may be about 0.2 to 1.5% by weight, particularly 0.3 to 1.5% by weight (for example, 0.4 to 1.5% by weight), and 0.5% by weight or more (for example, 0.4 to 1.5% by weight). For example, it may be 0.5 to 1.5% by weight).

It is preferable that magnesium oxide satisfies both the range of B content and the range of Ca content, but as long as one of these is satisfied, the content ratio of the other is not necessarily satisfied. ..

The magnesium oxide of the present invention may contain elements other than Mg, B and Ca. Such elements are not particularly limited, but are non-metallic elements [eg, C (carbon), S (sulfur), halogens (eg, Cl (chlorine), etc.)], metallic elements or semi-metallic elements [eg, , Typical metal elements (eg, alkali or alkaline earth metals such as Na (sodium); Al (aluminum), Si (silicon), etc.), Transition metal elements (eg, Fe (iron), Zn (zinc), etc.), etc. ] And so on. These elements may be contained in magnesium oxide alone or in combination of two or more.

Among these, typical elements are silicon, sodium, halogen (chlorine, etc.) and the like. Magnesium oxide containing such an element may be derived from seawater, for example. In the present invention, desired physical properties and properties (excellent elution property, few manufacturing defects, etc.) can be obtained even if such other elements are contained.

The content of other elements in magnesium oxide can be appropriately selected depending on the type of element and the like. For example, the silicon content is, for example, 0.001% by weight or more (for example, 0.001 to 0.1% by weight), preferably 0.005 to 0.07% by weight, and more preferably 0.01 to 0%. It may be about 0.05% by weight.

The sodium content is, for example, 0.0001% by weight or more (for example, 0.0001 to 0.1% by weight), preferably 0.0005 to 0.05% by weight, and more preferably 0.001 to 0. It may be about 0.01% by weight.

Further, the chlorine content is, for example, 0.0001% by weight or more (for example, 0.0001 to 0.1% by weight), preferably 0.0005 to 0.05% by weight, and further preferably 0.001 to 0. It may be about 0.01% by weight.

Depending on the application, it is preferable that the amount of elements such as lead and arsenic is as small as possible. For example, the content of Pb (lead) in magnesium oxide may be 1 ppm or less (for example, about 0.1 ppm). The content of As (arsenic) may be 4 ppm or less (for example, about 1 ppm).

The ratio of each element in magnesium oxide can be measured by, for example, ICP emission spectroscopic analysis method (ICP-AES method), ICP mass spectrometry method (ICP-MS method), or the like.

The purity of magnesium oxide is not particularly limited, but high purity may be required depending on the application. On the other hand, if the purity is too high, the desired physical properties and properties may be impaired.

From this point of view, the magnesium oxide assay can be selected from a high purity range, for example, 90% or more (for example, 93 to 99.5%), and preferably 95% or more (for example, 95%). ~ 99%), more preferably 96 ~ 99% (eg 96.3 ~ 98.5%), and in particular 96 ~ 98%.

The net content may be determined according to, for example, the United States Pharmacopeia (USP). Specifically, the constant amount of magnesium oxide was calcined at 800-900 ° C. ± 25 ° C., and 320 mg of the constant amount of magnesium oxide was weighed and 20 ml of 2N hydrochloric acid was added to dissolve the mixture to make 100 ml. May be obtained by adding and titrating with 0.1 mol / L EDTA standard solution.

The BET specific surface area of magnesium oxide can be selected from the range of, for example, about 1 to 100 m ² / g (for example, 3 to 80 m ² / g), preferably 5 to 60 m ² / g (for example, 8 to 55 m ² / g). ), More preferably 10 to 50 m ² / g (for example, 12 to 45 m ² / g), particularly 15 to 40 m ² / g (for example, 20 to 35 m ² / g).

The method for measuring the BET specific surface area may be any method usually used in this field and is not particularly limited, but may be, for example, a nitrogen adsorption method. Specifically, for example, a measurement sample (magnesium oxide granules) heat-treated in a nitrogen gas atmosphere as a pretreatment may be measured by a nitrogen gas adsorption method with a BET specific surface area measuring device. The pretreatment may be carried out, for example, in a nitrogen gas atmosphere at about 130 ° C. for about 30 minutes. The device used for performing the pretreatment and the BET specific surface area measuring device are not particularly limited, and any device usually used in this field may be used.

By adjusting the BET specific surface area to the above range, it seems that the hardness of the tablet can be easily increased without impairing the effect of improving the dissolution property and the manufacturing defect.

The bulk density of magnesium oxide may be, for example, 700 to 1200 g / L, preferably 850 to 1000 g / L, and more preferably 900 to 950 g / L.
The bulk density may be the bulk density specified in the Japanese Pharmacopoeia.

The shape of magnesium oxide may usually be granules (granular, powdery or powdery). The average particle size of magnesium oxide is not particularly limited and can be selected depending on the intended use, and may be, for example, 200 to 700 μm, preferably 250 to 600 μm, and more preferably about 300 to 500 μm.
The range of the particle size (minimum diameter to maximum diameter) is not particularly limited and can be selected depending on the application and the like. For example, from the viewpoint of elution, 100 to 850 μm, preferably 150 to 500 μm, and more preferably 250. It may be about 350 μm. The particle size may be measured by, for example, a sieve shaker.

The method for producing magnesium oxide of the present invention is not particularly limited as long as the above-mentioned characteristics and physical properties can be obtained, and a conventional method may be used.

In particular, the magnesium oxide of the present invention has a step of adding an alkali to a magnesium source to obtain magnesium hydroxide (magnesium hydroxide production step) and a step of calcining the obtained magnesium hydroxide to obtain magnesium oxide (firing step). It is preferable to manufacture the product after the above.

In the magnesium hydroxide production step, examples of the magnesium source include seawater and an aqueous magnesium chloride solution (brine), and in particular, seawater may be preferably used. By using seawater, it is easy to obtain magnesium oxide having a predetermined concentration of calcium.

Although it depends on the type of magnesium source, when magnesium oxide having a low B (boron) content is obtained as described above, a magnesium oxide source having a reduced B content may be used in advance. In particular, as the magnesium source, seawater from which boron has been removed may be used.

In such a case, the production method of the present invention may include at least a step (boron separation step) of removing (or separating) boron from a magnesium source (particularly seawater).

In the boron separation step, the method for removing boron is not particularly limited, but for example, B may be removed (separated) from the magnesium source with a chelate resin. Specifically, B can be removed by passing (passing) a magnesium source (seawater) through the chelate resin.

Examples of the chelating resin include resins having a chelating functional group (for example, N-methyleneglucamine, etc.) (for example, styrene-divinylbenzene copolymer, cellulose, etc.). As a commercially available chelate resin (chelate fiber), it can be obtained from Kirest Co., Ltd. and the like.

In the magnesium hydroxide production step, the alkali is not particularly limited, but a calcium hydroxide source may be typically used. In particular, the calcium hydroxide source may be slaked lime, which may be in the form of lime milk. By using a calcium hydroxide source, it is easy to obtain magnesium oxide having a predetermined concentration of calcium.

In the firing step, the firing temperature is not particularly limited, but may be, for example, 500 to 2000 ° C, preferably 600 to 1500 ° C, and more preferably 700 to 1200 ° C. The firing time can also be appropriately selected, and may be, for example, 10 minutes to 10 hours, preferably 30 minutes to 5 hours, and more preferably about 1 to 3 hours.

Magnesium oxide obtained in the firing step may usually be pulverized according to a desired shape (for example, granular shape). Therefore, the method of the present invention may further include a pulverization step of pulverizing magnesium oxide obtained in the calcination step after the calcination step.

The firing state of magnesium oxide obtained in the firing step is preferably light firing (light firing state). The activity of magnesium oxide (lightly baked magnesium) in such a lightly baked state is, for example, about several to several hundred m ² / g (for example, 1 to 300 m ² / g, preferably ² to 100 m) in terms of BET specific surface area. ^It may be about ² / g).

In the pulverization step, magnesium oxide may be pressurized and pulverized if necessary. The pressurizing conditions can be appropriately selected, the pressurizing device is not particularly limited, and a roller compactor or the like may be used.

The pulverization method is not particularly limited, and for example, pulverization may be performed using a granulator. The granulator is not particularly limited, and examples thereof include a roll granulator. Specifically, the pulverization method may be a method in which pressurized magnesium oxide is passed through the gaps between the rotated rolls by using a roll granulator in which three rolls are set vertically to pulverize the rolls.

The pulverized magnesium oxide (granule) may have the same particle size or particle size, if necessary, by sieving or the like.

The use of the magnesium oxide (granule) of the present invention is not particularly limited, and various uses [for example,
It can be used for pigments, rubber additives (vulcanization accelerators, etc.), fertilizers, foods, cosmetics, pharmaceuticals, etc.]).

In particular, in the present invention, since high-purity magnesium oxide can be obtained, in particular, the magnesium oxide (granule) and tablets of the present invention are used for direct or indirect ingestion or contact with animals (for example, for foods). , For pharmaceuticals, cosmetics, fertilizers, etc.).

In addition to general foods including health foods, foods also include foods for specified health use, foods with nutritional function and other foods with health claims. Foods also include supplements (dietary supplements), feeds, and the like.

[tablet]
The magnesium oxide of the present invention may be molded into a desired form, and may particularly form a tablet, depending on the intended use. That is, the magnesium oxide (tablet) of the present invention may be for tablets (for example, for direct tableting). Therefore, the present invention includes the above-mentioned tablets containing magnesium oxide.

The tablets may contain magnesium oxide and may be formed together with conventional additives (binders, disintegrants, etc.) depending on the intended use.

The binder is not particularly limited, and examples thereof include sodium carboxymethyl cellulose, low-substituted hydroxypropyl cellulose, crystalline cellulose, starch (for example, corn starch) and the like.

The disintegrant is not particularly limited, and examples thereof include carboxymethyl cellulose calcium, carmellose, low-substituted hydroxypropyl cellulose, croscarmellose sodium, carmellose calcium, and carboxystarch sodium.

In addition, the tablets may further contain excipients, lubricants and the like. The excipient is not particularly limited, and examples thereof include lactose, sucrose, mannitol, cornstarch, and crystalline cellulose. The lubricant is not particularly limited, and examples thereof include sucrose fatty acid ester, polyethylene glycol, talc, stearic acid or stearic acid salt (Na, Mg, or Ca salt).

In addition, tablets can optionally be plastics, coatings, anti-coagulation agents, solubilizers, sweeteners, acidulants, flavoring agents, pH regulators, solubilizers, colorants, flavors, mineral sources (eg, calcium carbonate). It may contain one or more additives such as (calcium source such as).

Examples of the plasticizer include triethyl citrate, glycerin fatty acid ester, polyethylene glycol and the like. Examples of the coating agent include ethyl cellulose and hydroxypropyl methyl cellulose. Examples of the anti-aggregation agent include talc and calcium stearate. Examples of the solubilizer include sucrose fatty acid ester, sorbitan monostearate, and sodium lauryl sulfate. Examples of the sweetener include aspartame, saccharin, dipotassium glycyrrhizinate, stevia and the like. Examples of the acidulant (organic acid) include citric acid, malic acid, ascorbic acid, fumaric acid and the like. Examples of the flavoring agent include l-menthol, sodium chloride, acesulfame potassium, sucralose and the like. Examples of the pH adjuster include citrate, phosphate, carbonate, acetate and the like. Examples of the solubilizing agent include cyclodextrin, arginine, lysine, trisaminomethane and the like. Examples of the colorant include yellow iron sesquioxide, iron sesquioxide, and sodium copper chlorophyllin. Examples of the fragrance include orange oil, lemon oil, peppermint oil, eucalyptus oil and the like.

These additives may be used alone or in combination of two or more, or different additives may be combined.

The content (blending amount, content ratio) of the additive can be appropriately selected depending on the type of the additive and the like. For example, the blending amount of the binder is not particularly limited, but for example, 0.1 to 30 weight in a tablet. %, preferably 0.5 to 20% by weight, more preferably about 1 to 15% by weight. The amount of the disintegrant is not particularly limited, but may be, for example, 0.1 to 30% by weight, preferably 0.5 to 10% by weight, and more preferably 1 to 5% by weight in the tablet.
The proportion of magnesium oxide (granule) in the tablet can be selected according to the intended use and is not particularly limited, but is, for example, 50% by weight or more (for example, 60% by weight or more), preferably 70% by weight or more (for example). , 75% by weight or more), 80% by weight or more, 85% by weight or more, 90% by weight or more, 95% by weight or more, and the like.

The method for producing tablets may follow a conventionally known method. For example, the magnesium oxide tablet of the present invention may be produced by mixing magnesium oxide (granule), a binder and a disintegrant (and other additives if necessary), and tableting (tableting). Good.

The locking method is not particularly limited, and may be a direct striking method (direct powder compression method), a wet granule compression method, or the like, but in the present invention, the direct striking method may be particularly preferably used.

The strength of the tablet can be selected depending on the application, and is, for example, 50 N or more (for example, 55 to 200 N), preferably 60 N or more (for example, 65 to 180 N), and more preferably 70 N or more (for example, 70 to 150 N). In particular, it may be about 75 N or more (for example, 75 to 120 N).

Next, the present invention will be described in more detail with reference to examples, but the present invention is not limited to these examples, and many modifications are made in the art within the technical idea of the present invention. It is possible by a person with ordinary knowledge.

Various physical properties and characteristics were measured or evaluated as follows.

Impurity analysis method (content): Measured by ICP-AES method.

Method of measuring assay: The pure content was measured according to the United States Pharmacopeia (USP).

BET specific surface area measurement method: Measured by the nitrogen adsorption method.

Molding method of tablet sample: Formulation (magnesium oxide: 75%, crystalline cellulose: 10%, light calcium carbonate: 10%, croscarmellose sodium: 3%, magnesium stearate: 1%, citric acid: 1%) A rotary type tableting machine equipped with a punch having a diameter of φ8 mm and a radius of curvature of R10 mm was used for tableting at a tableting pressure of 5 kN to obtain magnesium oxide tablets having a weight of 300 mg and a thickness of 4.0 mm per tablet.

Dissolution rate measurement method: Using an dissolution tester (manufacturer name: VK7025 manufactured by VARIAN), the dissolution test was performed according to the dissolution test paddle method listed in the Japanese Pharmacopoeia (test solution: Japanese Pharmacopoeia Disintegration Test Method No. 1). 1 liquid, liquid temperature: 37 ° C., rotation speed: 50 rpm, measurement time: 45 minutes). The amount of eluted magnesium oxide was measured by the ICP-AES method. The measurement was performed with 3 vessels, and the average value was taken as the average elution rate.

Tablet hardness measuring method: The tablet hardness was measured using a tablet breaking strength measuring device (Toyama Sangyo: TH303MP). Ten tablets were measured and the average value was calculated.

Method of measuring the defect rate of cracks: Continuous tableting was performed, the cracks and cracks of the tablets were checked, and the number of shots at which defects began to occur was counted. It is judged that the larger the number of shots, the smaller the defective rate.

(Example 1)
Seawater is filtered and 9600 mL of seawater is passed through a column-filled chelate fiber (trade name: Kirest fiber GRY-HW) manufactured by Kirest at a constant rate of 15 mL / mL-fiber / h, and B in the seawater. Was removed.

In a 20 L capacity polyethylene container, 4720 mL of seawater from which B had been removed (corresponding to 0.24 mol as Mg ²⁺ ) was weighed and stirred, and sulfuric acid was added thereto to adjust the pH to 3 and decarboxylate. Then, it was transferred to a polyethylene container having a capacity of 100 L. This milk of lime adjusted to CaO concentration equivalent 11.9 g / dL as alkaline material was added slowly under 100mL stirring ^{(Mg 2+} moles: OH ^- moles was 1.0: 1.8) , Mg (OH) ₂ suspension was prepared. Using this Mg (OH) ₂ suspension as a seed, add 4720 mL of seawater from which B has been removed and decarboxylated in the same manner as described above, and further stir 100 mL of lime milk adjusted to a CaO concentration equivalent to 11.9 g / dL. After slowly adding below, the mixture was stirred for 5 minutes to carry out the first seed crystal reaction. Such a seed crystal reaction was repeated 10 times in total.

Then, it was dehydrated, washed with 10 times as much pure water as the solid content, and dried to obtain a raw material. A 300 mL volume of an alumina crucible was filled with 100 g of a raw material and calcined at 820 ° C. for 2 hours using an electric furnace to obtain an MgO sample.

A roll pressure of 1 MPa was applied to the MgO sample using a horizontal roller compactor manufactured by Freund Turbo. Then, pulverization was performed using a granulator (Japan Granulator: GRN1031).

After pulverization, sieving was performed with a vibrating sieve (20 mesh and 60 mesh), and granules over 20 mesh and under 60 mesh were removed to prepare magnesium oxide granules (average particle size of about 400 μm).

Various properties and physical properties were measured or evaluated using the obtained magnesium oxide granules.

(Example 2)
Magnesium oxide granules were obtained by performing the same operation as in Example 1 except that 10500 mL of seawater was passed through the chelated fibers at a constant rate of 15 mL / mL-fiber / h to remove B in the seawater. Using this, various characteristics and physical properties were measured or evaluated.

(Example 3)
Magnesium oxide granules were obtained by performing the same operation as in Example 1 except that 11400 mL of seawater was passed through the chelated fibers at a constant rate of 15 mL / mL-fiber / h to remove B in the seawater. Using this, various characteristics and physical properties were measured or evaluated.

(Example 4)
Magnesium oxide was subjected to the same operation as in Example 1 except that 51 mL of an 8.3 N NaOH aqueous solution was added as an alkaline raw material (Mg 2 ⁺ number of moles: OH ⁻ number of moles was 1.0: 1.8). Granules were obtained, and various properties and physical properties were measured or evaluated using them.

(Example 5)
Magnesium oxide was subjected to the same operation as in Example 1 except that 54 mL of an 8.3 N NaOH aqueous solution was added as an alkaline raw material (Mg 2 ⁺ number of moles: OH ⁻ number of moles was 1.0: 1.9). Granules were obtained, and various properties and physical properties were measured or evaluated using them.

(Example 6)
Milk of lime a 111mL addition adjusted to CaO concentration equivalent 11.9 g / dL as alkaline material ^{(Mg 2+} moles: OH ^- moles 1.0: a which was 2.0) and other than the can, as in Example 1 Magnesium oxide granules were obtained by performing the same operation, and various properties and physical properties were measured or evaluated using the magnesium oxide granules.

(Example 7)
Magnesium oxide granules were obtained in the same manner as in Example 1 except that they were calcined at 850 ° C. for 2 hours, and various properties and physical properties were measured or evaluated using them.

(Example 8)
Magnesium oxide granules were obtained by performing the same operation as in Example 1 except that they were calcined at 760 ° C. for 2 hours, and various properties and physical properties were measured or evaluated using them.

(Example 9)
Magnesium oxide granules were obtained in the same manner as in Example 1 except that they were calcined at 1000 ° C. for 2 hours, and various properties and physical properties were measured or evaluated using them.

(Example 10)
Magnesium oxide granules were obtained in the same manner as in Example 1 except that they were calcined at 710 ° C. for 2 hours, and various properties and physical properties were measured or evaluated using them.

(Example 11)
The polyethylene container 2L capacity, a MgCl ₂ · 6H ₂ O and 48g weighed as the magnesium material was stirred with deionized water 100 mL, to prepare a MgCl ₂ solution. This aqueous NaOH 51mL of 8.3N was added slowly with stirring as an alkali material ^{(Mg 2+} moles: OH ^- moles was 1.0: 1.8), Mg a _{(OH) 2} suspension Prepared.

The Mg _{(OH) 2} suspension as a seed, MgCl ₂ · 6H ₂ O was added the MgCl ₂ aqueous solution prepared by dissolving in 48g of pure water 100 mL, and after another slow addition of aqueous NaOH 51mL of 8.3N under stirring thereon The first seed crystal reaction was carried out with stirring for 5 minutes. Such a seed crystal reaction was repeated 10 times in total.

Magnesium oxide granules were obtained by performing the same operation as in Example 1 except that the above operation was performed, and various properties and physical properties were measured or evaluated using the magnesium oxide granules.

(Comparative Example 1)
As described below, magnesium oxide granules described in Example 3 of Patent Document 4 (Pamphlet No. WO2015 / 128940) were obtained, and various properties and physical properties were measured or evaluated using the magnesium oxide granules.

That is, magnesium hydroxide (manufactured by Konoshima Chemical Co., Ltd., grade name: # 200) was calcined at 900 ° C. for 2 hours in an electric furnace to produce medium-active MgO. The medium active MgO thus obtained had a BET specific surface area of 51 m ² / g. On the other hand, the same # 200 was fired in an electric furnace at 1100 ° C. for 2 hours to produce low-activity MgO. The low-activity MgO thus obtained had a BET specific surface area of 3 m ² / g.
The BET specific surface area of 51 m ² / g obtained above was mixed so that the ratio of the medium active MgO and the low active MgO of 3 m ² / g was medium active MgO: low active MgO = 40: 60 (% by weight). MgO granules were prepared using the above.

Various characteristics and physical properties are shown in the table below.

As is clear from the results in the above table, magnesium oxide granules having a high purity that can be sufficiently applied to pharmaceuticals and food applications and having a boron content in a predetermined range (for example, 0.05% by weight or less) are used. Therefore, by using tablets having a high dissolution rate and magnesium oxide granules having a calcium content in a predetermined range (for example, 0.03 to 1.8% by weight), tablets with less cracking can be efficiently obtained. I understand.

It was also found that by further adjusting the BET specific surface area, tablets having high hardness can be obtained while improving the dissolution property and cracking.

And, in particular, by adjusting the boron content, calcium content and BET specific surface area (and further purity) in combination, these can be achieved at a high level without impairing excellent elution, crack reduction effect, and high hardness. It turned out to be compatible.

According to the present invention, it is possible to provide magnesium oxide granules that can improve elution and manufacturing defects (such as cracking) while having high purity. Such magnesium oxide granules can be applied to various uses, but because of their sufficiently high purity, they are particularly used for direct or indirect ingestion or contact with animals (for example, for foods, pharmaceuticals, cosmetics). , For fertilizer, etc.).

Claims (14)

Magnesium oxide granules having a B content of 0.05% by weight or less, a Ca content of 0.03 to 1.8% by weight, a pure content of 95 to 99%, and a BET specific surface area of 10 to 60 m ² / g. (However, except for clinker manufacturing) . The magnesium oxide granule according to claim 1, which has a BET specific surface area of 10 to 56 m ² / g. Claim that the content of B is 0.03% by weight or less, the content of Ca is 0.05 to 1.5% by weight, the pure content is 96 to 99%, and the BET specific surface area is 17 to 36 m ² / g. 1 or 2 Magnesium oxide granules. The magnesium oxide granule according to any one of claims 1 to 3, wherein magnesium oxide is derived from seawater. Magnesium oxide granules for use in ingestion or contact with animals directly or indirectly, satisfying the following (1).
(1) B content is 0.05% by weight or less The magnesium oxide granule according to claim 5, further satisfying the following (2).
(2) Ca content is 0.03 to 1.8% by weight The magnesium oxide granule according to claim 5 or 6, which has a pure content of 95 to 99%. The magnesium oxide granule according to any one of claims 5 to 7, which is used for at least one application selected from food, pharmaceutical and cosmetic products. The method for producing magnesium oxide granules according to any one of claims 1 to 8, which comprises at least a step of removing B from seawater. The production method according to claim 9, wherein B is removed from seawater with a chelate resin. A tablet containing magnesium oxide granules according to any one of claims 1 to 8. A method for adjusting the content of B in magnesium oxide granules to 0.05% by weight or less to improve or improve the elution of tablets containing magnesium oxide granules. Adjust the B content in the magnesium oxide granules to 0.03% by weight or less, the Ca content to 0.05 to 1.5% by weight, and the pure content to 95 to 99%, and elute the tablets containing the magnesium oxide granules. A method for improving or improving the properties and reducing manufacturing defects. 13. The method of claim 13, wherein the manufacturing defect is chipping and / or cracking of the tablet.