WO2014054257A1 - Dentifrice composition - Google Patents

Dentifrice composition Download PDF

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Publication number
WO2014054257A1
WO2014054257A1 PCT/JP2013/005778 JP2013005778W WO2014054257A1 WO 2014054257 A1 WO2014054257 A1 WO 2014054257A1 JP 2013005778 W JP2013005778 W JP 2013005778W WO 2014054257 A1 WO2014054257 A1 WO 2014054257A1
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Prior art keywords
remineralization
composition
hydroxyapatite
ultramarine
dentifrice
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PCT/JP2013/005778
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French (fr)
Japanese (ja)
Inventor
佐久間　周治
恵二郎 藤田
理絵 高松
真理子 小吹
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株式会社サンギ
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    • A—HUMAN NECESSITIES
    • A61—MEDICAL OR VETERINARY SCIENCE; HYGIENE
    • A61K—PREPARATIONS FOR MEDICAL, DENTAL OR TOILETRY PURPOSES
    • A61K8/00—Cosmetics or similar toiletry preparations
    • A61K8/18—Cosmetics or similar toiletry preparations characterised by the composition
    • A61K8/19—Cosmetics or similar toiletry preparations characterised by the composition containing inorganic ingredients
    • A61K8/24—Phosphorous; Compounds thereof
    • A—HUMAN NECESSITIES
    • A61—MEDICAL OR VETERINARY SCIENCE; HYGIENE
    • A61Q—SPECIFIC USE OF COSMETICS OR SIMILAR TOILETRY PREPARATIONS
    • A61Q11/00—Preparations for care of the teeth, of the oral cavity or of dentures; Dentifrices, e.g. toothpastes; Mouth rinses

Definitions

  • the present invention relates to a dentifrice composition having an effect of promoting recalcification of teeth.
  • Caries start from the formation of dental plaque by caries bacteria such as Streptococcus mutans adhering to the tooth surface, and organic acids produced by the metabolism of food by dental caries in dental plaque
  • the enamel is decalcified and an initial caries state is obtained.
  • Saliva has the function of remineralizing the demineralized part by the action of calcium and phosphorus in the saliva and returning the teeth to the original state. If the decalcified teeth can be sufficiently regenerated by remineralization, the occurrence of caries can be suppressed.
  • a dentifrice containing one kind of fluoride and calcium phosphate and hydroxyapatite having a crystal structure similar to the inorganic components of teeth is manufactured and sold.
  • oral compositions such as dentifrices that can sufficiently realize the promotion of remineralization because remineralization of the demineralized part is not sufficient only by using saliva or a dentifrice containing fluoride or hydroxyapatite. Development is required.
  • Dentifrice composition for oral cavity (Patent Document 2) that can retain hydroxyapatite fine powder on the tooth surface for a long time by blending hydroxyapatite fine powder with water-soluble cellulose solution, Oral bacteria (Patent Document 3) that can significantly promote remineralization by using a sugar alcohol such as xylitol and dicalcium phosphate in combination, and oral bacteria containing low crystalline hydroxyapatite Oral composition (Patent Document 4) that can prevent oral diseases and discomfort by adsorbing and sterilizing -Oral composition (patent document 5), micellar calcium phosphate-phosphopeptide which can prevent tooth decay and periodontal disease by tooth whitening, remineralization promotion, which contains calcium compounds such as hydroxya
  • Patent Document 7 Can promote remineralization and suppress caries (Patent Document 7), and pH 5 to 5 in which tricalcium phosphate is blended as calcium salt powder having the ability to convert into hydroxyapatite by contact with water in the oral cavity.
  • No. 8 dentifrice composition (Patent Document 8) and the like have been proposed.
  • ultramarine is composed of aluminum and sodium silicates, sulfide ions and sulfate ions, and is naturally present as the main component of lapis lazuli, and is known as an inorganic pigment.
  • Speaking of ultramarine meant blue ultramarine, but now there are green and purple (varieties called ultramarine violet or ultramarine red) and red (ultramarine pink) .
  • This ultramarine is used in paints, printing inks, paper, rubber, plastic coloring, wallpaper and tanning dyeing, detergents, cosmetics, liquid crystal display color filters, and the like.
  • ultramarine blue is used as a substance that modifies the color of teeth in a composition for delivering an oral care substance to the oral cavity (Patent Document 9). Furthermore, as a poorly water-soluble component in an oral composition for use in an applicator-integrated container that can stably disperse a poorly water-soluble powder component in the composition by using xanthan gum as a thickener, ultramarine, hydroxy, Apatite is exemplified (Patent Document 10). Here, unlike the present invention, the compositions in Patent Documents 9 and 10 are not used for dentifrice.
  • sodium silicate is also used as a component of oral compositions, and has been proposed as a component that stabilizes the properties of aluminum lactate, for example, for preventing hypersensitivity and for tightening gingival tissues. (Patent Document 11).
  • An object of the present invention is to provide a dentifrice composition having a high remineralization effect of demineralized tooth enamel.
  • the inventors of the present invention formulated a ultramarine composition usually used as a colorant in calcium phosphate selected from hydroxyapatite and tricalcium phosphate, and this was used as a dentifrice. Surprisingly, it was found that the remineralization of teeth was remarkably promoted, and the present invention was completed. Moreover, it discovered that these effects were further accelerated
  • the present invention relates to a dentifrice composition containing (1) ultramarine composition and calcium phosphate selected from hydroxyapatite and tricalcium phosphate, and (2) ultramarine composition comprising Na ( 6-10) it or dentifrice composition according to the above (1), characterized in a composition represented by Al 6 Si 6 O 24 S ( 2 ⁇ 4), formulation (3) ultramarine composition
  • the dentifrice composition according to the above (1) or (2), wherein the amount is 0.0001 to 0.5% by weight, and (4) the amount of hydroxyapatite is 0.001 to The dentifrice composition according to any one of the above (1) to (3), which is 30% by weight, and (5) the above (1), wherein the blending amount of tricalcium phosphate is 0.001 to 30% by weight Toothpaste composition according to any of (3), (6) and Silica The dentifrice composition according to any one of (1) to (5) above, wherein (7) sodium silicate is blended in an amount of 0.01 to 20.0% by weight, wherein sodium is blended It is related
  • the dentifrice composition of the present invention is composed of ultramarine composition, calcium phosphate selected from hydroxyapatite and tricalcium phosphate as an active ingredient, and is excellent in remineralization of decalcified tooth enamel. .
  • FIG. 4 is a diagram in which the photographs shown in FIG. 1 and FIG. 3 are drawn using dark ink and descriptions of the state of each part are added.
  • the dentifrice composition of the present invention is not particularly limited as long as it contains an ultramarine composition and a calcium phosphate selected from hydroxyapatite and tricalcium phosphate.
  • a toothpaste, A powder dentifrice, a liquid dentifrice, etc. can be illustrated. Hydroxyapatite and tricalcium phosphate may be used alone or in combination.
  • the dentifrice composition of the present invention significantly promotes the remineralization of teeth because the ultramarine composition usually used as a colorant is blended with calcium phosphate selected from hydroxyapatite and tricalcium phosphate. be able to.
  • Hydroxyapatite used in the present invention is a kind of calcium phosphate, and is obtained from fish bones of pork, pork bones, cow bones, etc. of edible fish such as salmon as natural hard tissues in addition to those synthesized by ordinary methods. There may be.
  • hydroxyapatite is stoichiometrically represented by a composition composed of Ca 10 (PO 4 ) 6 (OH) 2 , but is non-stoichiometric with a Ca / P molar ratio of not 1.67. Even in this case, it exhibits the properties of hydroxyapatite and can have an apatite structure.
  • synthetic hydroxyapatite having a Ca / P molar ratio of about 1.4 to 1.8 is also included in the hydroxyapatite in the present invention.
  • the hydroxyapatite used in the present invention may be crystalline, low crystalline, or amorphous, but it is low crystalline or amorphous hydroxyapatite from the viewpoint of caries prevention effect.
  • low crystalline hydroxyapatite and amorphous hydroxyapatite are referred to as “amorphous hydroxyapatite”.
  • “Low crystallinity” means that the X-ray diffraction peak is broader than that of highly crystalline powder, and “amorphous” means that the X-ray diffraction pattern has a wide halo. The diffraction pattern showing the characteristics of the crystal cannot be obtained.
  • Such amorphous hydroxyapatite can be obtained, for example, by freeze-drying apatite synthesized by a wet synthesis method, drying at a temperature of 100 ° C. or lower, or baking at about 300 ° C. or lower.
  • the amount of hydroxyapatite blended in the present invention is preferably 0.001 to 30% by weight, preferably 0.01 to 20% by weight of the entire dentifrice composition, from the viewpoint of the remineralization promoting effect and the feeling of use. More preferred is 0.1 to 20% by weight.
  • Tricalcium phosphate used in the present invention is also referred to as tricalcium phosphate, and is a composition represented by the chemical formula 3Ca 3 (PO 4 ) 2 .Ca (OH) 2 , including pharmaceuticals and cosmetics, foods, It is widely used in general goods and petrochemical industries.
  • the tricalcium phosphate used in the present invention may be anything such as a pharmaceutical additive standard, a quasi-drug raw material standard, and a combination component standard for each cosmetic variety.
  • the blending amount of tricalcium phosphate in the present invention is preferably 0.001 to 30% by weight, and 0.01 to 20% by weight of the entire dentifrice composition, from the viewpoint of the remineralization promoting effect and the feeling of use. %, More preferably 0.1 to 20% by weight.
  • the ultramarine composition used in the present invention is, for example, an inorganic pigment represented by the chemical formula Na ( 6-10 ) Al 6 Si 6 O 24 S (2-4) .
  • the ultramarine composition used in the present invention can be used from blue to near pink. Specifically, blue CB-80: manufactured by Daiichi Kasei Kogyo Co., Ltd., Daiichi Pink DP-3: Daiichi Kasei Kogyo ( Examples thereof include powder pigments manufactured by UNIPURE PINK LC589, manufactured by Daito Kasei Kogyo Co., Ltd.
  • the ultramarine composition of the present invention may be of any type for cosmetics, quasi-drug raw material standards, and the like.
  • the blending amount of the ultramarine composition in the present invention is preferably 0.0001 to 0.5% by weight of the entire dentifrice composition from the viewpoint of the remineralization promoting effect and the feeling of use, and is preferably 0.001 to 0. More preferably, it is 1% by weight.
  • the dentifrice composition of the present invention preferably further contains sodium silicate. By containing sodium silicate, remineralization of teeth can be further promoted.
  • Examples of the sodium silicate used in the present invention include Na 4 SiO 4 , Na 2 Si 2 O 5 , Na 2 Si 4 O 9 and the like, in addition to the sodium salt of metasilicic acid Na 2 SiO 3 . More specifically, for example, a quasi-drug raw material standard can be used.
  • the blending amount of sodium silicate in the present invention is preferably 0.01 to 20% by weight, and more preferably 0.1 to 10% by weight, from the viewpoint of remineralization promoting effect and feeling of use.
  • the dentifrice composition of the present invention contains additives, humectants, foaming agents, fragrances, sweeteners, preservatives and various active ingredients that are usually used in dentifrice compositions in addition to the aforementioned components. Can do. Specific examples of these components are shown below. In addition to the components shown below, appropriate components according to the purpose, the type of the composition, and the like can be further blended.
  • dibasic calcium phosphate, calcium carbonate, calcium pyrophosphate, abrasive precipitated silica, abrasive gel silica and other silica calcium silicate, aluminum silicate, aluminum oxide, aluminum hydroxide, alumina, zeolite, titanium oxide, silica
  • examples thereof include zirconium acid, insoluble sodium metaphosphate, tribasic magnesium phosphate, magnesium carbonate, calcium sulfate, magnesium sulfate, polymethyl methacrylate, bentonite, and a synthetic resin.
  • wetting agent examples include polyhydric alcohols such as glycerin, propylene glycol, polyethylene glycol, sorbitol, xylitol, ethylene glycol, 1,3-butylene glycol, and isopropylene glycol.
  • polyhydric alcohols such as glycerin, propylene glycol, polyethylene glycol, sorbitol, xylitol, ethylene glycol, 1,3-butylene glycol, and isopropylene glycol.
  • foaming agent examples include sodium lauryl sulfate, sodium N-lauroyl sarcosine, a nonionic surfactant, and the like.
  • thickeners examples include hydroxyethylcellulose, sodium carboxymethylcellulose, carrageenan, carboxyvinyl polymer, xanthan gum, gelatin, pullulan, sodium alginate, sodium polyacrylate, polyvinyl alcohol, locust bean gum, guar gum, hydroxypropyl methylcellulose, etc. Can do.
  • Binders include methylcellulose, propylene glycol alginate, pullulan, tragacanth gum, xanthan gum, pectin, fercelan, chitosan, polyethylene oxide, polyvinylpyrrolidone, polyacrylic acid, polymethacrylic acid, peptone, casein, collagen, albumin, gum arabic, karaya gum Eudragit, ethyl cellulose, cellulose acetate, sodium polyacrylate, polyvinyl alcohol, polyvinyl acetal / dimethylaminoacetate, cellulose acetate / dibutylhydroxypropyl ether, and the like.
  • polyoxyethylene hydrogenated castor oil sorbitan monostearate, glycerin fatty acid ester, propylene glycol fatty acid ester, alkyl glyceryl ether, polyoxyethylene sorbitol fatty acid ester, polysorbate, polyoxyethylene, lauromacrogol, sodium alkyl sulfate
  • examples include alkyl phosphate esters, sodium alkylbenzene sulfonates, sodium N-acyl sarcosine, N-acyl glutamates, sucrose fatty acid esters, alkyl glycosides, alkyl dimethyl amine oxides, alkyl betaines and the like.
  • Oils and fats include liquid paraffin, paraffin, cetyl alcohol, higher alcohols such as stearyl alcohol, fatty acid esters such as isopropyl myristate, lanolin, whale wax, carnauba wax, fatty acids, octyldodecyl myristate, diisopropyl adipate, hexadecyl isostearate And ester compounds such as decyl oleate, squalane, squalene, medium chain fatty acid triglycerides, silicon and the like.
  • alcohols such as stearyl alcohol, fatty acid esters such as isopropyl myristate, lanolin, whale wax, carnauba wax, fatty acids, octyldodecyl myristate, diisopropyl adipate, hexadecyl isostearate
  • ester compounds such as decyl oleate, squalane,
  • Alcohols include lower alcohols such as ethanol, propyl alcohol, isopropyl alcohol, butanol, isobutanol, ethylene glycol, diethylene glycol, propylene glycol, dipropylene glycol, 1,3-butylene glycol, glycerin, 1,5-pentadiol, sorbit Examples thereof include polyhydric alcohols such as polyethylene glycol.
  • Surfactants include nonionic surfactants such as sorbitan fatty acid ester, glycerin fatty acid ester, decaglycerin fatty acid ester, polyglycerin fatty acid ester, propylene glycol / pentaerythritol fatty acid ester, polyoxyethylene sorbitan fatty acid ester, polyoxyethylene.
  • nonionic surfactants such as sorbitan fatty acid ester, glycerin fatty acid ester, decaglycerin fatty acid ester, polyglycerin fatty acid ester, propylene glycol / pentaerythritol fatty acid ester, polyoxyethylene sorbitan fatty acid ester, polyoxyethylene.
  • pH adjusters examples include citric acid and its salts, phosphoric acid and its salts, malic acid and its salts, gluconic acid and its salts, maleic acid and its salts, aspartic acid and its salts, gluconic acid and its salts, succinic acid And salts thereof, glucuronic acid and salts thereof, fumaric acid and salts thereof, glutamic acid and salts thereof, adipic acid and salts thereof, inorganic acids such as hydrochloric acid, hydrofluoric acid, sodium hydroxide, potassium hydroxide, etc. Examples include alkali metals, amines such as triethanolamine, diethanolamine, and diisopropanolamine.
  • preservative examples include paraoxybenzoic acid ester, alkyldiaminoethylglycine hydrochloride, methylparaben, ethylparaben, sodium benzoate and the like.
  • the stabilizer examples include sodium sulfite, sodium hydrogen sulfite, dibutylhydroxytoluene, butylhydroxyanisole, edetic acid or salts thereof.
  • Perfumes include essential oils such as menthol, peppermint, spearmint, eucalyptus oil, orange oil, lemon oil, winder green oil, clove oil, peppermint oil, thyme oil, carvone, linalool, eugenol, anethole, herb mint, etc. Can be illustrated.
  • stabilizers include vitamin C, vitamin E and derivatives thereof, sodium sulfite, sodium pyrosulfite, sodium hydrogen sulfite, butylhydroxytoluene, butylhydroxyanisole and the like.
  • sweetening agents include saccharin sodium, aspartame, stevioside, neohesperidyl dihydrochalcone, glycyrrhizin, asparatylphenylalanine methyl ester, acesulfame potassium, perilartine, p-methoxycinnamic aldehyde, xylitol and the like.
  • Other medicinal ingredients include allantoin, tocopherol acetate, isopropylphenol, triclosan, chlorhexidine, chlorophyll, flavonoids, tranexamic acid, hinokitiol, cetylpyridinium chloride, sodium fluoride, stannous fluoride, sodium monofluorophosphate, dextranase
  • examples include mutanase, protease, aminocaproic acid, glycyrrhizic acid, glycyrrhetinic acid, azulene, allantoin, lysozyme chloride, psyllium extract, polyphosphoric acid, sodium chloride and the like.
  • the compounding quantity of these arbitrary components is used suitably in the range accept
  • the ultramarine composition, hydroxyapatite, tricalcium phosphate, sodium silicate, and other components may be added in any process of the production process.
  • a toothpaste (Examples 1 to 48) and a liquid dentifrice (Examples 49 to 88) containing a combination of ultramarine composition and hydroxyapatite or tricalcium phosphate and sodium silicate were further prepared. Acceleration test was conducted.
  • the obtained hydroxyapatite powder had a maximum particle size of about 40 ⁇ m, a minimum particle size of about 0.05 ⁇ m, and an average particle size of about 5 ⁇ m.
  • This hydroxyapatite powder was used.
  • Tricalcium phosphate As the tricalcium phosphate, ⁇ -TCP-100 (Taihei Chemical Industry Co., Ltd.) was used.
  • ultramarine composition hydroxyapatite, tricalcium phosphate, dicalcium phosphate, hydroxyapatite and sodium silicate, tricalcium phosphate and sodium silicate, ultramarine composition and sodium silicate, ultramarine
  • a remineralization acceleration test was conducted by preparing a toothpaste and a liquid dentifrice containing the composition and dicalcium phosphate and the group composition blue, sodium silicate and dicalcium phosphate.
  • an artificial initial caries test sample prepared in advance was used for the preparation of the artificial initial caries test sample.
  • bovine anterior teeth and crown labial enamel were used for the preparation of the artificial initial caries test sample.
  • the enamel surface was polished with # 1000, # 2400, and # 4000 polishing paper.
  • a 3.5 ⁇ 3.0 mm window was prepared by using Nail Enamel (Maybelin Co., Ltd.) as a test target site on the polished enamel surface, and 0.1 M lactate buffer (pH 4.5, 3.0 mM CaCl 2 , 1. 8 mM KH 2 PO 4 , 0.5% CMC) was immersed for 4 days at 37 ° C. to prepare an artificial initial caries.
  • test solution was prepared by mixing toothpaste and liquid dentifrice with artificial saliva to form a suspension solution.
  • the artificial initial caries test specimen prepared above was immersed in each test solution for 12 days, and then the specimen was about 500 ⁇ m thick so that it was parallel to the tooth axis with a microcutter. After cutting, this slice was ground using a grindstone and a natural grindstone to form parallel thin slices of about 100 ⁇ m thickness under water injection.
  • CMR contact microradiogram
  • Control surface in the figure is a part for comparing the degree of remineralization effect of the dentifrice compositions of Examples and Comparative Examples, and maintained the state of artificial initial caries. Is. Half of the artificial initial caries (3.5 ⁇ 3.0 mm window) region.
  • the “treated surface” in the figure is a portion on which the test solutions (test substances) of Examples and Comparative Examples are applied.
  • Tables 33 and 34 show the results of confirming the effect of promoting remineralization of the dentifrice composition by the computer image analysis method.
  • Example 1 (remineralization rate: 19.9%) and Comparative Example 1 and Comparative Example 12 (total remineralization rate: 14.5%)
  • Example 2 (remineralization rate: 20.0%)
  • Comparative Example 2 and Comparative Example 7 (total remineralization rate: 9.4%)
  • Example 5 (remineralization rate: 34.3%)
  • Comparative Example 3 and Comparative Example 9 (total remineralization rate: 11.5%)
  • Example 10 (remineralization rate: 24.8%)
  • Comparative Example 4 and Comparative Example 11 (total remineralization rate: 13.2%)
  • Example 11 (remineralization rate: 20.7%)
  • Comparative Example 5 and Comparative Example 8 (total remineralization rate: 9.8%)
  • Example 12 (remineralization rate: 23.6%) and Comparative Example 6 and Comparative Example 12 (
  • the dentifrice composition of the present invention is very excellent in remineralization of teeth and has high industrial utility.

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Abstract

The present invention addresses the problem of providing a dentifrice composition having a high effect of remineralizing decalcified dental enamel. The dentifrice composition according to the present invention is characterized by comprising an ultramarine composition and a calcium phosphate component selected from hydroxylapatite and calcium triphosphate.

Description

歯磨用組成物Dentifrice composition
　本発明は、歯牙の再石灰化促進効果を有する歯磨用組成物に関する。 The present invention relates to a dentifrice composition having an effect of promoting recalcification of teeth.
　う蝕は、ストレプトコッカス・ミュータンス菌等の虫歯菌が、歯牙表面に付着し歯垢を形成することから始まり、歯垢中で虫歯菌が食物を代謝することにより産生される有機酸が、歯牙エナメル質を脱灰して、初期う蝕状態となる。唾液は、この脱灰部を、唾液中のカルシウムやリンの働きで再石灰化し、歯を元の状態に戻す働きを有している。再石灰化により、脱灰した歯牙を十分に再生することができれば、う蝕の発生を抑えることが可能となる。 Caries start from the formation of dental plaque by caries bacteria such as Streptococcus mutans adhering to the tooth surface, and organic acids produced by the metabolism of food by dental caries in dental plaque The enamel is decalcified and an initial caries state is obtained. Saliva has the function of remineralizing the demineralized part by the action of calcium and phosphorus in the saliva and returning the teeth to the original state. If the decalcified teeth can be sufficiently regenerated by remineralization, the occurrence of caries can be suppressed.
　そこで、歯牙の再石灰化を促進するために、フッ化物や、リン酸カルシウムの１種で、歯牙の無機成分と類似の結晶構造を有するハイドロキシアパタイトを配合した歯磨剤が製造販売されている。 Therefore, in order to promote the remineralization of teeth, a dentifrice containing one kind of fluoride and calcium phosphate and hydroxyapatite having a crystal structure similar to the inorganic components of teeth is manufactured and sold.
　しかしながら、唾液や、フッ化物又はハイドロキシアパタイトを配合した歯磨剤の使用だけでは脱灰部の再石灰化が十分ではなく、再石灰化の促進を十分に実現しうる歯磨剤等の口腔用組成物の開発が求められている。 However, oral compositions such as dentifrices that can sufficiently realize the promotion of remineralization because remineralization of the demineralized part is not sufficient only by using saliva or a dentifrice containing fluoride or hydroxyapatite. Development is required.
　そこで、粒子径が０．０５μｍ～１．０μｍのハイドロキシアパタイトやリン酸三カルシウムを配合した、歯表面の微小な凹凸の修復、保護、虫歯予防、歯質強化、美白効果を高めることができる口腔用歯磨剤（特許文献１）や、ハイドロキシアパタイト微粉末を水溶性セルロース溶液に配合することにより、歯面上にハイドロキシアパタイト微粉末を長く滞留させることができる口腔用組成物（特許文献２）や、キシリトール等の糖アルコールと第２リン酸カルシウムを併用することにより、再石灰化を著しく促進させることができる口腔用組成物（特許文献３）や、低結晶性ハイドロキシアパタイトを配合した、口腔内細菌に吸着して除菌することにより口腔内の疾患、不快感を予防することができる口腔用組成物（特許文献４）や、ローヤルゼリー又はその抽出物に、ハイドロキシアパタイト等のカルシウム化合物を配合した歯牙の美白、再石灰化促進による虫歯予防、歯周病予防できる口腔用組成物（特許文献５）や、ミセル性リン酸カルシウム－ホスホペプチド複合体を含む抗う蝕機能を有する再石灰化促進剤（特許文献６）や、フッ化物イオンを含む歯磨剤を用いて歯牙を洗浄した後に、カルシウムイオンを含む口腔用液体組成物を作用させることによって、再石灰化を促進、う蝕を抑制できる方法（特許文献７）や、口腔内で水と接触してハイドロキシアパタイトへの転化能を有するカルシウム塩粉末としてリン酸三カルシウムを配合したｐＨ５～８の歯磨用組成物（特許文献８）等が提案されている。 Therefore, oral cavity that can repair and protect minute irregularities on the tooth surface, prevent dental caries, strengthen teeth and enhance whitening effect by combining hydroxyapatite and tricalcium phosphate with particle size of 0.05μm to 1.0μm. Dentifrice (Patent Document 1), composition for oral cavity (Patent Document 2) that can retain hydroxyapatite fine powder on the tooth surface for a long time by blending hydroxyapatite fine powder with water-soluble cellulose solution, Oral bacteria (Patent Document 3) that can significantly promote remineralization by using a sugar alcohol such as xylitol and dicalcium phosphate in combination, and oral bacteria containing low crystalline hydroxyapatite Oral composition (Patent Document 4) that can prevent oral diseases and discomfort by adsorbing and sterilizing -Oral composition (patent document 5), micellar calcium phosphate-phosphopeptide which can prevent tooth decay and periodontal disease by tooth whitening, remineralization promotion, which contains calcium compounds such as hydroxyapatite in Yal Jelly or its extract After washing a tooth using a remineralization accelerator (Patent Document 6) having an anti-cariogenic function including a complex or a dentifrice containing fluoride ions, an oral liquid composition containing calcium ions is allowed to act. Can promote remineralization and suppress caries (Patent Document 7), and pH 5 to 5 in which tricalcium phosphate is blended as calcium salt powder having the ability to convert into hydroxyapatite by contact with water in the oral cavity. No. 8 dentifrice composition (Patent Document 8) and the like have been proposed.
　また、再石灰化を促進するために、キシリトールとリン酸カルシウム、非結晶性リン酸カルシウム又はリン酸化オリゴ糖カルシウムとを配合したチューインガム等も製造されているが、再石灰化が必ずしも十分ではない。 In order to promote remineralization, chewing gum or the like containing xylitol and calcium phosphate, amorphous calcium phosphate or phosphorylated oligosaccharide calcium is also produced, but remineralization is not always sufficient.
　他方、群青（ウルトラマリン）は、アルミニウムとナトリウムのケイ酸塩に硫化物イオンや硫酸イオンからなり、天然にはラピスラズリの主成分として存在するものであり、無機顔料として知られている。合成ウルトラマリンが普及する以前は、ウルトラマリンと言えば、青色のウルトラマリンを指したが、現在では、緑色や紫色(ウルトラマリン バイオレット若しくはウルトラマリン レッドという品種)、赤色(ウルトラマリン ピンク)がある。この群青（ウルトラマリン）は、塗料、印刷インキ、紙、ゴム、プラスチックの着色、壁紙や更紗の染色、洗剤等の他、化粧料、液晶表示装置のカラーフィルター等に用いられている。 On the other hand, ultramarine is composed of aluminum and sodium silicates, sulfide ions and sulfate ions, and is naturally present as the main component of lapis lazuli, and is known as an inorganic pigment. Before the synthesis of ultramarine, Speaking of ultramarine meant blue ultramarine, but now there are green and purple (varieties called ultramarine violet or ultramarine red) and red (ultramarine pink) . This ultramarine is used in paints, printing inks, paper, rubber, plastic coloring, wallpaper and tanning dyeing, detergents, cosmetics, liquid crystal display color filters, and the like.
　また、群青は、例えば、口腔に口中ケア物質を送達するための組成物において歯の色を改質する物質として用いられている（特許文献９）。さらに、増粘剤としてキサンタンガムを用いることにより難水溶性粉体成分を組成物中に安定に分散させることができるアプリケーター一体型容器に用いるための口腔用組成物における難水溶成分として、群青、ハイドロキシアパタイトが例示されている（特許文献１０）。ここで、特許文献９及び１０における組成物は、本発明とは異なり、歯磨に用いられるものではない。 Further, ultramarine blue is used as a substance that modifies the color of teeth in a composition for delivering an oral care substance to the oral cavity (Patent Document 9). Furthermore, as a poorly water-soluble component in an oral composition for use in an applicator-integrated container that can stably disperse a poorly water-soluble powder component in the composition by using xanthan gum as a thickener, ultramarine, hydroxy, Apatite is exemplified (Patent Document 10). Here, unlike the present invention, the compositions in Patent Documents 9 and 10 are not used for dentifrice.
　また、珪酸ナトリウムも口腔用組成物の成分として用いられており、例えば、知覚過敏症の予防効果や歯肉組織の引き締め効果のために配合する乳酸アルミニウムの性状を安定性させる成分として提案されている（特許文献１１）。 In addition, sodium silicate is also used as a component of oral compositions, and has been proposed as a component that stabilizes the properties of aluminum lactate, for example, for preventing hypersensitivity and for tightening gingival tissues. (Patent Document 11).
特開平９－２０２７１７号公報JP-A-9-202717 特開平１０－５９８１４号公報JP-A-10-59814 特開２０００－１２８７５２号公報JP 2000-128752 A 特開２００１－１２２７４８号公報JP 2001-122748 A 特開２００５－３１４２６６号公報JP 2005-314266 A 特開２００６－２１３６６８号公報JP 2006-213668 A 特開２００７－９９６３２号公報JP 2007-99632 A 特開平７－２２３９３０号公報JP-A-7-223930 特表２００４－５１３０６５号公報Japanese translation of PCT publication No. 2004-513065 特開２０１１－５１９２７号公報JP 2011-51927 A 特開平７－２９１８４４号公報JP-A-7-291844
　本発明の課題は、脱灰した歯牙エナメル質の再石灰化効果の高い歯磨用組成物を提供することにある。 An object of the present invention is to provide a dentifrice composition having a high remineralization effect of demineralized tooth enamel.
　本発明者らは、上記課題を解決するために鋭意検討した結果、ハイドロキシアパタイト及びリン酸三カルシウムから選ばれるリン酸カルシウムに、通常着色剤として用いられている群青組成物を配合し、これを歯磨剤として用いることにより、意外にも、歯牙の再石灰化が顕著に促進されることを見いだし、本発明を完成するに至った。また、珪酸ナトリウムをさらに含有させることにより、これらの効果がさらに促進されることを見いだした。 As a result of intensive studies to solve the above-mentioned problems, the inventors of the present invention formulated a ultramarine composition usually used as a colorant in calcium phosphate selected from hydroxyapatite and tricalcium phosphate, and this was used as a dentifrice. Surprisingly, it was found that the remineralization of teeth was remarkably promoted, and the present invention was completed. Moreover, it discovered that these effects were further accelerated | stimulated by further containing sodium silicate.
　すなわち、本発明は、（１）群青組成物と、ハイドロキシアパタイト及びリン酸三カルシウムから選ばれるリン酸カルシウムとを含有することを特徴とする歯磨用組成物や、（２）群青組成物が、Ｎａ（６～10）Ａｌ６Ｓｉ６Ｏ２４Ｓ（２～４）で表される組成物であることを特徴とする上記（１）に記載の歯磨用組成物や、（３）群青組成物の配合量が、０．０００１～０．５重量％であることを特徴とする上記（１）又は（２）に記載の歯磨用組成物や、（４）ハイドロキシアパタイトの配合量が、０．００１～３０重量％である上記（１）及至（３）の何れかに記載の歯磨用組成物や、（５）リン酸三カルシウムの配合量が、０．００１～３０重量％である上記（１）及至（３）の何れかに記載の歯磨用組成物や、（６）更に珪酸ナトリウムを配合したことを特徴とする上記（１）及至（５）の何れかに記載の歯磨用組成物や、（７）珪酸ナトリウムの配合量が、０．０１～２０．０重量％であることを特徴とする上記（６）に記載の歯磨用組成物に関する。 That is, the present invention relates to a dentifrice composition containing (1) ultramarine composition and calcium phosphate selected from hydroxyapatite and tricalcium phosphate, and (2) ultramarine composition comprising Na ( 6-10) it or dentifrice composition according to the above (1), characterized in a composition represented by Al 6 Si 6 O 24 S ( 2 ~ 4), formulation (3) ultramarine composition The dentifrice composition according to the above (1) or (2), wherein the amount is 0.0001 to 0.5% by weight, and (4) the amount of hydroxyapatite is 0.001 to The dentifrice composition according to any one of the above (1) to (3), which is 30% by weight, and (5) the above (1), wherein the blending amount of tricalcium phosphate is 0.001 to 30% by weight Toothpaste composition according to any of (3), (6) and Silica The dentifrice composition according to any one of (1) to (5) above, wherein (7) sodium silicate is blended in an amount of 0.01 to 20.0% by weight, wherein sodium is blended It is related with the composition for dentifrice as described in said (6) characterized by the above-mentioned.
　本発明の歯磨用組成物は、群青組成物と、ハイドロキシアパタイト、リン酸三カルシウムから選ばれるリン酸カルシウムを有効成分としたものであって、脱灰した歯牙エナメル質の再石灰化に大変優れている。 The dentifrice composition of the present invention is composed of ultramarine composition, calcium phosphate selected from hydroxyapatite and tricalcium phosphate as an active ingredient, and is excellent in remineralization of decalcified tooth enamel. .
コンタクトマイクロラジオグラム（ＣＭＲ）による実施例５の歯冠部のコントロール面と処理面を示す写真である。It is a photograph which shows the control surface and processing surface of the crown part of Example 5 by a contact microradiogram (CMR). コンタクトマイクロラジオグラム（ＣＭＲ）による実施例２９の歯冠部のコントロール面と処理面を示す写真である。It is a photograph which shows the control surface and processed surface of the crown part of Example 29 by a contact microradiogram (CMR). 図１及び図３に示す写真を、濃墨を用いて描きかつ各部の状態の説明を付加した図である。FIG. 4 is a diagram in which the photographs shown in FIG. 1 and FIG. 3 are drawn using dark ink and descriptions of the state of each part are added.
　本発明の歯磨用組成物としては、群青組成物と、ハイドロキシアパタイト及びリン酸三カルシウムから選ばれるリン酸カルシウムとを含有するものであれば特に制限されるものではなく、具体的に、練り歯磨剤、粉歯磨剤、液体歯磨剤等を例示することができる。また、ハイドロキシアパタイト及びリン酸三カルシウムは、それぞれ単独で用いてもよいし、両者を併用してもよい。 The dentifrice composition of the present invention is not particularly limited as long as it contains an ultramarine composition and a calcium phosphate selected from hydroxyapatite and tricalcium phosphate. Specifically, a toothpaste, A powder dentifrice, a liquid dentifrice, etc. can be illustrated. Hydroxyapatite and tricalcium phosphate may be used alone or in combination.
　本発明の歯磨用組成物は、ハイドロキシアパタイト及びリン酸三カルシウムから選ばれるリン酸カルシウムに、通常着色剤として用いられている群青組成物を配合しているので、歯牙の再石灰化を顕著に促進することができる。 The dentifrice composition of the present invention significantly promotes the remineralization of teeth because the ultramarine composition usually used as a colorant is blended with calcium phosphate selected from hydroxyapatite and tricalcium phosphate. be able to.
　本発明において使用されるハイドロキシアパタイトは、リン酸カルシウムの１種であり、通常の方法で合成されるものの他、天然硬組織としてサケ等の食用魚の魚骨、豚骨、牛骨等から得られるものであってもよい。通常、ハイドロキシアパタイトは、化学量論的にはＣａ１０（ＰＯ４）６（ＯＨ）２からなる組成で示されるが、Ｃａ／Ｐモル比が１．６７にならない非化学量論的なものであっても、ハイドロキシアパタイトの性質を示すと共にアパタイト構造をとることができ、例えば、Ｃａ／Ｐモル比１．４～１．８程度の合成ハイドロキシアパタイトも本発明におけるハイドロキシアパタイトに含まれる。 Hydroxyapatite used in the present invention is a kind of calcium phosphate, and is obtained from fish bones of pork, pork bones, cow bones, etc. of edible fish such as salmon as natural hard tissues in addition to those synthesized by ordinary methods. There may be. Usually, hydroxyapatite is stoichiometrically represented by a composition composed of Ca 10 (PO 4 ) 6 (OH) 2 , but is non-stoichiometric with a Ca / P molar ratio of not 1.67. Even in this case, it exhibits the properties of hydroxyapatite and can have an apatite structure. For example, synthetic hydroxyapatite having a Ca / P molar ratio of about 1.4 to 1.8 is also included in the hydroxyapatite in the present invention.
　本発明において使用されるハイドロキシアパタイトは、結晶性、低結晶性、非晶質のいずれであってもよいが、う蝕予防効果の点から、低結晶性又は非晶質のハイドロキシアパタイトであることが好ましい（以下、低結晶性ハイドロキシアパタイト及び非晶質のハイドロキシアパタイトを「アモルファスハイドロキシアパタイト」と称する。）。なお、「低結晶性」とは、Ｘ線回折ピークが、高結晶性の粉体に比べてブロードな結晶質のものをいい、「非晶質」とは、Ｘ線回折パターンが幅広いハローを示し、結晶の特徴を示す回折パターンが得られないものをいう。このようなアモルファスハイドロキシアパタイトは、例えば、湿式合成法により合成したアパタイトを凍結乾燥若しくは１００℃以下の温度で乾燥し、又は３００℃程度以下の温度で焼成して得ることができる。 The hydroxyapatite used in the present invention may be crystalline, low crystalline, or amorphous, but it is low crystalline or amorphous hydroxyapatite from the viewpoint of caries prevention effect. (Hereinafter, low crystalline hydroxyapatite and amorphous hydroxyapatite are referred to as “amorphous hydroxyapatite”). “Low crystallinity” means that the X-ray diffraction peak is broader than that of highly crystalline powder, and “amorphous” means that the X-ray diffraction pattern has a wide halo. The diffraction pattern showing the characteristics of the crystal cannot be obtained. Such amorphous hydroxyapatite can be obtained, for example, by freeze-drying apatite synthesized by a wet synthesis method, drying at a temperature of 100 ° C. or lower, or baking at about 300 ° C. or lower.
　本発明におけるハイドロキシアパタイトの配合量としては、再石灰化促進効果、使用感の観点から、歯磨用組成物全体の０．００１～３０重量％であることが好ましく、０．０１～２０重量％であることがより好ましく、０．１～２０重量％であることがさらに好ましい。 The amount of hydroxyapatite blended in the present invention is preferably 0.001 to 30% by weight, preferably 0.01 to 20% by weight of the entire dentifrice composition, from the viewpoint of the remineralization promoting effect and the feeling of use. More preferred is 0.1 to 20% by weight.
　本発明において使用されるリン酸三カルシウムは、第三リン酸カルシウムとも称され、化学式で３Ｃａ3（ＰＯ4）2・Ｃａ（ＯＨ）2で表される組成物で、医薬品や化粧品をはじめ、食品、雑貨品、石油化学工業など広く一般的に使用されている。本発明において使用されるリン酸三カルシウムは、医薬品添加物規格、医薬部外品原料規格、化粧品種別配合成分規格等、どのようなものであってもよい。 Tricalcium phosphate used in the present invention is also referred to as tricalcium phosphate, and is a composition represented by the chemical formula 3Ca 3 (PO 4 ) 2 .Ca (OH) 2 , including pharmaceuticals and cosmetics, foods, It is widely used in general goods and petrochemical industries. The tricalcium phosphate used in the present invention may be anything such as a pharmaceutical additive standard, a quasi-drug raw material standard, and a combination component standard for each cosmetic variety.
　本発明におけるリン酸三カルシウムの配合量としては、再石灰化促進効果、使用感の観点から、歯磨用組成物全体の０．００１～３０重量％であることが好ましく、０．０１～２０重量％であることがより好ましく、０．１～２０重量％であることがさらに好ましい。 The blending amount of tricalcium phosphate in the present invention is preferably 0.001 to 30% by weight, and 0.01 to 20% by weight of the entire dentifrice composition, from the viewpoint of the remineralization promoting effect and the feeling of use. %, More preferably 0.1 to 20% by weight.
　本発明において使用される群青組成物は、例えば、化学式でＮａ（６～10）Ａｌ６Ｓｉ６Ｏ２４Ｓ（２～４）で表される無機顔料である。本発明において使用される群青組成物は、青色からピンクに近いものまで使用でき、具体的に、青ＣＢ－８０：第一化成工業（株）製、ダイイチピンクＤＰ－３：第一化成工業（株）製、ＵＮＩＰＵＲＥ ＰＩＮＫ ＬＣ５８９：大東化成工業（株）製等の粉末顔料を例示することができる。また、本発明の群青組成物は、化粧品用、医薬部外品原料規格等、どのようなものであってもよい。 The ultramarine composition used in the present invention is, for example, an inorganic pigment represented by the chemical formula Na ( 6-10 ) Al 6 Si 6 O 24 S (2-4) . The ultramarine composition used in the present invention can be used from blue to near pink. Specifically, blue CB-80: manufactured by Daiichi Kasei Kogyo Co., Ltd., Daiichi Pink DP-3: Daiichi Kasei Kogyo ( Examples thereof include powder pigments manufactured by UNIPURE PINK LC589, manufactured by Daito Kasei Kogyo Co., Ltd. Further, the ultramarine composition of the present invention may be of any type for cosmetics, quasi-drug raw material standards, and the like.
　本発明における群青組成物の配合量としては、再石灰化促進効果、使用感の観点から、歯磨用組成物全体の０．０００１～０．５重量％であることが好ましく、０．００１～０．１重量％であることがより好ましい。 The blending amount of the ultramarine composition in the present invention is preferably 0.0001 to 0.5% by weight of the entire dentifrice composition from the viewpoint of the remineralization promoting effect and the feeling of use, and is preferably 0.001 to 0. More preferably, it is 1% by weight.
　本発明の歯磨用組成物は、さらに珪酸ナトリウムを含有することが好ましい。珪酸ナトリウムを含有させることにより、歯牙の再石灰化をより促進させることができる。 The dentifrice composition of the present invention preferably further contains sodium silicate. By containing sodium silicate, remineralization of teeth can be further promoted.
　本発明において使用される珪酸ナトリウムとしては、メタケイ酸のナトリウム塩Ｎａ２ＳｉＯ３の他、Ｎａ４ＳｉＯ４，Ｎａ２Ｓｉ２Ｏ５，Ｎａ２Ｓｉ４Ｏ９等も含まれる。より具体的には、例えば、医薬部外品原料規格を使用することができる。本発明における珪酸ナトリウムの配合量としては、再石灰化促進効果、使用感の観点から、０．０１～２０重量％であることが好ましく、０．１～１０重量％であることがより好ましい。 Examples of the sodium silicate used in the present invention include Na 4 SiO 4 , Na 2 Si 2 O 5 , Na 2 Si 4 O 9 and the like, in addition to the sodium salt of metasilicic acid Na 2 SiO 3 . More specifically, for example, a quasi-drug raw material standard can be used. The blending amount of sodium silicate in the present invention is preferably 0.01 to 20% by weight, and more preferably 0.1 to 10% by weight, from the viewpoint of remineralization promoting effect and feeling of use.
　本発明の歯磨用組成物は、前述の成分に加えて、歯磨用組成物に通常使用される添加剤、湿潤剤、発泡剤、香料、甘味料、防腐剤及び各種有効成分などを含有することができる。これらの成分の具体例を下記に示す。これら下記に示す成分に加えて、更にその目的、組成物の種類等に応じた適宜な成分を配合することができる。 The dentifrice composition of the present invention contains additives, humectants, foaming agents, fragrances, sweeteners, preservatives and various active ingredients that are usually used in dentifrice compositions in addition to the aforementioned components. Can do. Specific examples of these components are shown below. In addition to the components shown below, appropriate components according to the purpose, the type of the composition, and the like can be further blended.
　研磨剤としては、第２リン酸カルシウム、炭酸カルシウム、ピロリン酸カルシウム、研磨性沈降シリカ、研磨性ゲルシリカなどのシリカ、ケイ酸カルシウム、ケイ酸アルミニウム、酸化アルミニウム、水酸化アルミニウム、アルミナ、ゼオライト、酸化チタン、ケイ酸ジルコニウム、不溶性メタリン酸ナトリウム、第３リン酸マグネシウム、炭酸マグネシウム、硫酸カルシウム、硫酸マグネシウム、ポリメタクリル酸メチル、ベントナイト、合成樹脂等を例示することができる。 As abrasives, dibasic calcium phosphate, calcium carbonate, calcium pyrophosphate, abrasive precipitated silica, abrasive gel silica and other silica, calcium silicate, aluminum silicate, aluminum oxide, aluminum hydroxide, alumina, zeolite, titanium oxide, silica Examples thereof include zirconium acid, insoluble sodium metaphosphate, tribasic magnesium phosphate, magnesium carbonate, calcium sulfate, magnesium sulfate, polymethyl methacrylate, bentonite, and a synthetic resin.
　湿潤剤としては、グリセリン、プロピレングリコール、ポリエチレングリコール、ソルビトール、キシリトール、エチレングリコール、１，３－ブチレングリコール、イソプロピレングリコールなどの多価アルコール等を例示することができる。 Examples of the wetting agent include polyhydric alcohols such as glycerin, propylene glycol, polyethylene glycol, sorbitol, xylitol, ethylene glycol, 1,3-butylene glycol, and isopropylene glycol.
　発泡剤としては、ラウリル硫酸ナトリウム、Ｎ－ラウロイルサルコシンナトリウム、非イオン性界面活性剤等を例示することができる。 Examples of the foaming agent include sodium lauryl sulfate, sodium N-lauroyl sarcosine, a nonionic surfactant, and the like.
　増粘剤としては、ヒドロキシエチルセルロース、カルボキシメチルセルロースナトリウム、カラギーナン、カルボキシビニルポリマー、キサンタンガム、ゼラチン、プルラン、アルギン酸ナトリウム、ポリアクリル酸ナトリウム、ポリビニルアルコール、ローカストビーンガム、グアーガム、ヒドロキシプロピルメチルセルロース等を例示することができる。 Examples of thickeners include hydroxyethylcellulose, sodium carboxymethylcellulose, carrageenan, carboxyvinyl polymer, xanthan gum, gelatin, pullulan, sodium alginate, sodium polyacrylate, polyvinyl alcohol, locust bean gum, guar gum, hydroxypropyl methylcellulose, etc. Can do.
　結合剤としては、メチルセルロース、アルギン酸プロピレングリコールエステル、プルラン、トラガントガム、キサンタンガム、ペクチン、ファーセラン、キトサン、ポリエチレンオキシド、ポリビニルピロリドン、ポリアクリル酸、ポリメタクリル酸、ペプトン、カゼイン、コラーゲン、アルブミン、アラビアガム、カラヤガム、オイドラギット、エチルセルロース、酢酸セルロース、ポリアクリル酸ナトリウム、ポリビニルアルコール、ポリビニルアセタール・ジメチルアミノアセテート、セルロースアセテート・ジブチルヒドロキシプロピルエーテル等を例示することができる。 Binders include methylcellulose, propylene glycol alginate, pullulan, tragacanth gum, xanthan gum, pectin, fercelan, chitosan, polyethylene oxide, polyvinylpyrrolidone, polyacrylic acid, polymethacrylic acid, peptone, casein, collagen, albumin, gum arabic, karaya gum Eudragit, ethyl cellulose, cellulose acetate, sodium polyacrylate, polyvinyl alcohol, polyvinyl acetal / dimethylaminoacetate, cellulose acetate / dibutylhydroxypropyl ether, and the like.
　乳化剤としては、ポリオキシエチレン硬化ヒマシ油、モノステアリン酸ソルビタン、グリセリン脂肪酸エステル、プロピレングリコール脂肪酸エステル、アルキルグリセリルエーテル、ポリオキシエチレンソルビトール脂肪酸エステル、ポリソルベート、ポリオキシエチレン、ラウロマクロゴール、アルキル硫酸ナトリウム、アルキルリン酸エステル、アルキルベンゼンスルホン酸ナトリウム、Ｎ－アシルザルコシン酸ナトリウム、Ｎ－アシルグルタミン酸塩、ショ糖脂肪酸エステル、アルキルグリコシド類、アルキルジメチルアミンオキシド、アルキルベタイン類等を例示することができる。 As an emulsifier, polyoxyethylene hydrogenated castor oil, sorbitan monostearate, glycerin fatty acid ester, propylene glycol fatty acid ester, alkyl glyceryl ether, polyoxyethylene sorbitol fatty acid ester, polysorbate, polyoxyethylene, lauromacrogol, sodium alkyl sulfate, Examples include alkyl phosphate esters, sodium alkylbenzene sulfonates, sodium N-acyl sarcosine, N-acyl glutamates, sucrose fatty acid esters, alkyl glycosides, alkyl dimethyl amine oxides, alkyl betaines and the like.
　油脂成分としては、流動パラフィン、パラフィン、セチルアルコール、及びステアリルアルコール等の高級アルコール、イソプロピルミリステート等脂肪酸エステル、ラノリン、鯨ロウ、カルナウバロウ、脂肪酸類、ミリスチン酸オクチルドデシル、アジピン酸ジイソプロピル、イソステアリン酸ヘキサデシル、オレイン酸デシル等のエステル化合物、スクワラン、スクワレン、中鎖脂肪酸トリグリセリド、シリコン等を例示することができる。 Oils and fats include liquid paraffin, paraffin, cetyl alcohol, higher alcohols such as stearyl alcohol, fatty acid esters such as isopropyl myristate, lanolin, whale wax, carnauba wax, fatty acids, octyldodecyl myristate, diisopropyl adipate, hexadecyl isostearate And ester compounds such as decyl oleate, squalane, squalene, medium chain fatty acid triglycerides, silicon and the like.
　アルコールとしては、エタノール、プロピルアルコール、イソプロピルアルコール、ブタノール、イソブタノール等の低級アルコール、エチレングリコール、ジエチレングリコール、プロピレングリコール、ジプロピレングリコール、１，３－ブチレングリコール、グリセリン、１，５－ペンタジオール、ソルビット、ポリエチレングリコール等の多価アルコール等を例示することができる。 Alcohols include lower alcohols such as ethanol, propyl alcohol, isopropyl alcohol, butanol, isobutanol, ethylene glycol, diethylene glycol, propylene glycol, dipropylene glycol, 1,3-butylene glycol, glycerin, 1,5-pentadiol, sorbit Examples thereof include polyhydric alcohols such as polyethylene glycol.
　界面活性剤としては、非イオン性界面活性剤の、ソルビタン脂肪酸エステル、グリセリン脂肪酸エステル、デカグリセリン脂肪酸エステル、ポリグリセリン脂肪酸エステル、プロピレングリコール・ペンタエリスリトール脂肪酸エステル、ポリオキシエチレンソルビタン脂肪酸エステル、ポリオキシエチレングリセリン脂肪酸エステル、ポリオキシエチレンソルビット脂肪酸エステル、ポリエチレングリコール脂肪酸エステル、ポリオキシエチレンアルキルエーテル、ポリオキシエチレンポリオキシプロピレングリコール、ポリオキシプロピレンアルキルエーテル、ポリオキシエチレンポリオキシプロピレンアルキルエーテル、ポリオキシエチレンアルキルフェニルエーテル、ポリオキシエチレンヒマシ油・硬化ヒマシ油、ポリオキシエチレンラノリン・ラノリンアルコール・ミツロウ誘導体、ポリオキシエチレンアルキルアミン・脂肪酸アミド、ポリオキシエチレンアルキルフェニルホルムアルデヒド縮合物、単一鎖長ポリオキシエチレンアルキルエーテル、アニオン性界面活性剤の、ラウリル硫酸ナトリウム、ミリスチル硫酸ナトリウム、アルキル硫酸塩、ポリオキシエチレンアルキル硫酸塩、Ｎ－アシルアミノ酸及びその塩、Ｎ－アシルメチルタウリン及びその塩、ポリオキシエチレンアルキルエーテル酢酸塩、アルキルスルホカルボン酸塩、α－オレフィンスルホン酸塩、アルキルリン酸塩、ポリオキシエチレンアルキルエーテルリン酸塩、カチオン性界面活性剤の、アルキルアンモニウム、アルキルベンジルアンモニウム塩、両性界面活性剤の、酢酸ベタイン、イミダゾリニウムベタイン、レシチン、非イオン性界面活性剤としては、ショ糖脂肪酸エステル、ラウリル酸デカグリセリル等を例示することができる。 Surfactants include nonionic surfactants such as sorbitan fatty acid ester, glycerin fatty acid ester, decaglycerin fatty acid ester, polyglycerin fatty acid ester, propylene glycol / pentaerythritol fatty acid ester, polyoxyethylene sorbitan fatty acid ester, polyoxyethylene. Glycerin fatty acid ester, polyoxyethylene sorbite fatty acid ester, polyethylene glycol fatty acid ester, polyoxyethylene alkyl ether, polyoxyethylene polyoxypropylene glycol, polyoxypropylene alkyl ether, polyoxyethylene polyoxypropylene alkyl ether, polyoxyethylene alkylphenyl Ether, polyoxyethylene castor oil / hardened castor oil, polyoxyethylene Lanolin, lanolin alcohol, beeswax derivative, polyoxyethylene alkylamine, fatty acid amide, polyoxyethylene alkylphenyl formaldehyde condensate, single chain length polyoxyethylene alkyl ether, anionic surfactant, sodium lauryl sulfate, sodium myristyl sulfate Alkyl sulfates, polyoxyethylene alkyl sulfates, N-acyl amino acids and salts thereof, N-acyl methyl taurines and salts thereof, polyoxyethylene alkyl ether acetates, alkyl sulfocarboxylates, α-olefin sulfonates, Alkyl phosphate, polyoxyethylene alkyl ether phosphate, cationic surfactant, alkyl ammonium, alkyl benzyl ammonium salt, amphoteric surfactant, betaine acetate, imidazo Examples of linium betaine, lecithin, and nonionic surfactants include sucrose fatty acid esters and decaglyceryl laurate.
　ｐＨ調整剤としては、クエン酸及びその塩、リン酸及びその塩、リンゴ酸及びその塩、グルコン酸及びその塩、マレイン酸及びその塩、アスパラギン酸及びその塩、グルコン酸及びその塩、コハク酸及びその塩、グルクロン酸及びその塩、フマル酸及びその塩、グルタミン酸及びその塩、アジピン酸及びその塩、塩酸などの無機酸、フッ化水素酸、水酸化ナトリウム、水酸化カリウム等などの水酸化アルカリ金属、トリエタノールアミン、ジエタノールアミン、ジイソプロパノールアミンなどのアミン類等を例示することができる。 Examples of pH adjusters include citric acid and its salts, phosphoric acid and its salts, malic acid and its salts, gluconic acid and its salts, maleic acid and its salts, aspartic acid and its salts, gluconic acid and its salts, succinic acid And salts thereof, glucuronic acid and salts thereof, fumaric acid and salts thereof, glutamic acid and salts thereof, adipic acid and salts thereof, inorganic acids such as hydrochloric acid, hydrofluoric acid, sodium hydroxide, potassium hydroxide, etc. Examples include alkali metals, amines such as triethanolamine, diethanolamine, and diisopropanolamine.
　防腐剤としては、パラオキシ安息香酸エステル、塩酸アルキルジアミノエチルグリシン、メチルパラベン、エチルパラベン、安息香酸ナトリウム等を例示することができる。 Examples of the preservative include paraoxybenzoic acid ester, alkyldiaminoethylglycine hydrochloride, methylparaben, ethylparaben, sodium benzoate and the like.
　安定化剤としては、亜硫酸ナトリウム、亜硫酸水素ナトリウム、ジブチルヒドロキシトルエン、ブチルヒドロキシアニソール、エデト酸或いはその塩類等を例示することができる。 Examples of the stabilizer include sodium sulfite, sodium hydrogen sulfite, dibutylhydroxytoluene, butylhydroxyanisole, edetic acid or salts thereof.
　香料としては、メントール、ペパーミント、スペアミント等の精油、ユーカリ油、オレンジ油、レモン油、ウインダーグリーン油、チョウジ油、ハッカ油、タイム油、セージ油、カルボン、リナロール、オイゲノール、アネトール、ハーブミント等を例示することができる。 Perfumes include essential oils such as menthol, peppermint, spearmint, eucalyptus oil, orange oil, lemon oil, winder green oil, clove oil, peppermint oil, thyme oil, carvone, linalool, eugenol, anethole, herb mint, etc. Can be illustrated.
　安定化剤としては、ビタミンＣ、ビタミンＥおよびこれらの誘導体、亜硫酸ナトリウム、ピロ亜硫酸ナトリウム、亜硫酸水素ナトリウム、ブチルヒドロキシトルエン、ブチルヒドロキシアニソール等を例示することができる。 Examples of stabilizers include vitamin C, vitamin E and derivatives thereof, sodium sulfite, sodium pyrosulfite, sodium hydrogen sulfite, butylhydroxytoluene, butylhydroxyanisole and the like.
　甘味剤としては、サッカリンナトリウム、アスパルテーム、ステビオサイド、ネオヘスペリジルジヒドロカルコン、グリチルリチン、アスパラチルフェニルアラニンメチルエステル、アセスルファームカリウム、ペリラルチン、ｐ－メトキシシンナミックアルデヒド、キシリトール等を例示することができる。 Examples of sweetening agents include saccharin sodium, aspartame, stevioside, neohesperidyl dihydrochalcone, glycyrrhizin, asparatylphenylalanine methyl ester, acesulfame potassium, perilartine, p-methoxycinnamic aldehyde, xylitol and the like.
　その他薬効成分としては、アラントイン、酢酸トコフェロール、イソプロピルフェノール、トリクロサン、クロルヘキシジン、クロロフィル、フラボノイド、トラネキサム酸、ヒノキチオール、塩化セチルピリジニウム、フッ化ナトリウム、フッ化第１錫、モノフルオロリン酸ナトリウム、デキストラナーゼ、ムタナーゼ、プロテアーゼ、アミノカプロン酸、グリチルリチン酸、グリチルレチン酸類、アズレン、アラントイン、塩化リゾチーム、オオバクエキス、ポリリン酸類、塩化ナトリウム等を例示することができる。 Other medicinal ingredients include allantoin, tocopherol acetate, isopropylphenol, triclosan, chlorhexidine, chlorophyll, flavonoids, tranexamic acid, hinokitiol, cetylpyridinium chloride, sodium fluoride, stannous fluoride, sodium monofluorophosphate, dextranase Examples include mutanase, protease, aminocaproic acid, glycyrrhizic acid, glycyrrhetinic acid, azulene, allantoin, lysozyme chloride, psyllium extract, polyphosphoric acid, sodium chloride and the like.
　なお、これら任意成分の配合量は、本発明の効果を妨げず、薬剤学的に許容できる範囲で適宜使用される。また、本発明の歯磨用組成物の製造において、群青組成物、ハイドロキシアパタイト、リン酸三カルシウム、珪酸ナトリウムや、その他の成分は、製造過程のいかなる過程で添加してもよい。 In addition, the compounding quantity of these arbitrary components is used suitably in the range accept | permitted pharmacologically, without preventing the effect of this invention. In the production of the dentifrice composition of the present invention, the ultramarine composition, hydroxyapatite, tricalcium phosphate, sodium silicate, and other components may be added in any process of the production process.
　群青組成物とハイドロキシアパタイト又はリン酸三カルシウムとを配合し、更に珪酸ナトリウムを配合した練歯磨剤（実施例１～４８）及び液体歯磨剤（実施例４９～８８）を調製して、再石灰化促進試験を行った。 A toothpaste (Examples 1 to 48) and a liquid dentifrice (Examples 49 to 88) containing a combination of ultramarine composition and hydroxyapatite or tricalcium phosphate and sodium silicate were further prepared. Acceleration test was conducted.
［群青組成物］
　群青組成物は、ＣＢ－８０Ｚ（青）及びＤＰ－１（ピンク）（第一化成工業株式会社）を使用した。
［ハイドロキシアパタイト］
　攪拌下の水酸化カルシウム懸濁液中に、３０質量％濃度のリン酸水溶液を、ｐＨ１０になるまで滴下し、生成したゲル状物質を室温で１日間放置して熟成した。その後、ゲル状物質をガラスフィルターで濾過し、残った物質を１００℃の空気中で乾燥を行うことにより、ハイドロキシアパタイト粉末を得た。得られたハイドロキシアパタイト粉末は、最大粒径が約４０μｍ、最小粒径が約０．０５μｍ、平均粒径が約５μｍであった。このハイドロキシアパタイト粉末を使用した。
［リン酸三カルシウム］
　リン酸三カルシウムは、β-ＴＣＰ-１００（太平化学産業株式会社）を使用した。
［珪酸ナトリム］
　珪酸ナトリムは、水ガラス１号（和光純薬工業株式会社）を使用した。 [Ultramarine composition]
As the ultramarine composition, CB-80Z (blue) and DP-1 (pink) (Daiichi Kasei Kogyo Co., Ltd.) were used.
[Hydroxyapatite]
A 30% by mass phosphoric acid aqueous solution was dropped into the calcium hydroxide suspension under stirring until pH 10 was reached, and the resulting gel-like substance was aged at room temperature for 1 day. Thereafter, the gel-like substance was filtered with a glass filter, and the remaining substance was dried in air at 100 ° C. to obtain a hydroxyapatite powder. The obtained hydroxyapatite powder had a maximum particle size of about 40 μm, a minimum particle size of about 0.05 μm, and an average particle size of about 5 μm. This hydroxyapatite powder was used.
[Tricalcium phosphate]
As the tricalcium phosphate, β-TCP-100 (Taihei Chemical Industry Co., Ltd.) was used.
[Natrisilicate]
As the sodium silicate, water glass No. 1 (Wako Pure Chemical Industries, Ltd.) was used.
　また比較例として、群青組成物配合、ハイドロキシアパタイト配合、リン酸三カルシウム配合、第二リン酸カルシウム配合、ハイドロキシアパタイト及び珪酸ナトリウム配合、リン酸三カルシウム及び珪酸ナトリウム配合、群青組成物及び珪酸ナトリウム配合、群青組成物及び第二リン酸カルシウム配合、並びに、群組成物青、珪酸ナトリウム及び第二リン酸カルシウム配合の練歯磨剤、液体歯磨剤を調製して再石灰化促進試験を行なった。 Also, as comparative examples, ultramarine composition, hydroxyapatite, tricalcium phosphate, dicalcium phosphate, hydroxyapatite and sodium silicate, tricalcium phosphate and sodium silicate, ultramarine composition and sodium silicate, ultramarine A remineralization acceleration test was conducted by preparing a toothpaste and a liquid dentifrice containing the composition and dicalcium phosphate and the group composition blue, sodium silicate and dicalcium phosphate.
Figure JPOXMLDOC01-appb-T000001
Figure JPOXMLDOC01-appb-T000001
Figure JPOXMLDOC01-appb-T000002
Figure JPOXMLDOC01-appb-T000002
Figure JPOXMLDOC01-appb-T000003
Figure JPOXMLDOC01-appb-T000003
Figure JPOXMLDOC01-appb-T000004
Figure JPOXMLDOC01-appb-T000004
Figure JPOXMLDOC01-appb-T000005
Figure JPOXMLDOC01-appb-T000005
Figure JPOXMLDOC01-appb-T000006
Figure JPOXMLDOC01-appb-T000006
Figure JPOXMLDOC01-appb-T000007
Figure JPOXMLDOC01-appb-T000007
Figure JPOXMLDOC01-appb-T000008
Figure JPOXMLDOC01-appb-T000008
Figure JPOXMLDOC01-appb-T000009
Figure JPOXMLDOC01-appb-T000009
Figure JPOXMLDOC01-appb-T000010
Figure JPOXMLDOC01-appb-T000010
Figure JPOXMLDOC01-appb-T000011
Figure JPOXMLDOC01-appb-T000011
Figure JPOXMLDOC01-appb-T000012
Figure JPOXMLDOC01-appb-T000012
Figure JPOXMLDOC01-appb-T000013
Figure JPOXMLDOC01-appb-T000013
Figure JPOXMLDOC01-appb-T000014
Figure JPOXMLDOC01-appb-T000014
Figure JPOXMLDOC01-appb-T000015
Figure JPOXMLDOC01-appb-T000015
Figure JPOXMLDOC01-appb-T000016
Figure JPOXMLDOC01-appb-T000016
Figure JPOXMLDOC01-appb-T000017
Figure JPOXMLDOC01-appb-T000017
Figure JPOXMLDOC01-appb-T000018
Figure JPOXMLDOC01-appb-T000018
Figure JPOXMLDOC01-appb-T000019
Figure JPOXMLDOC01-appb-T000019
Figure JPOXMLDOC01-appb-T000020
Figure JPOXMLDOC01-appb-T000020
Figure JPOXMLDOC01-appb-T000021
Figure JPOXMLDOC01-appb-T000021
Figure JPOXMLDOC01-appb-T000022
Figure JPOXMLDOC01-appb-T000022
Figure JPOXMLDOC01-appb-T000023
Figure JPOXMLDOC01-appb-T000023
Figure JPOXMLDOC01-appb-T000024
Figure JPOXMLDOC01-appb-T000024
Figure JPOXMLDOC01-appb-T000025
Figure JPOXMLDOC01-appb-T000025
Figure JPOXMLDOC01-appb-T000026
Figure JPOXMLDOC01-appb-T000026
Figure JPOXMLDOC01-appb-T000027
Figure JPOXMLDOC01-appb-T000027
Figure JPOXMLDOC01-appb-T000028
Figure JPOXMLDOC01-appb-T000028
Figure JPOXMLDOC01-appb-T000029
Figure JPOXMLDOC01-appb-T000029
Figure JPOXMLDOC01-appb-T000030
Figure JPOXMLDOC01-appb-T000030
Figure JPOXMLDOC01-appb-T000031
Figure JPOXMLDOC01-appb-T000031
Figure JPOXMLDOC01-appb-T000032
Figure JPOXMLDOC01-appb-T000032
［再石灰化促進試験方法］
　再石灰化の促進効果を確認するために、予め作製した人工初期う蝕試験試料を用いた。人工初期う蝕試験試料の作製は、牛前歯、歯冠部唇面エナメル質を用いた。エナメル質表面を＃１０００、＃２４００、＃４０００の研磨紙で研磨した。研磨したエナメル質表面の試験対象部位をNail Enamel（メイベリン社製）で３．５×３．０ｍｍのウインドウを作製し、０．１Ｍ乳酸緩衝液（ｐＨ４．５、３．０ｍＭ ＣａＣｌ２、１．８ｍＭ ＫＨ２ＰＯ４、０．５％ ＣＭＣ）に３７℃、４日間浸漬させて、人工初期う蝕を作製した。なお、試験のコントロールには、３．５×３．０ｍｍのウインドウのうち、歯冠頭頂部側の半分をさらにNail Enamel（メイベリン社製）でマスキングし、比較対象部位（コントロール）とした。また、練歯磨剤、液体歯磨剤を人工唾液と混合し懸濁溶液としたものを試験溶液（被検物質）とした。 [Recalcification promotion test method]
In order to confirm the effect of promoting remineralization, an artificial initial caries test sample prepared in advance was used. For the preparation of the artificial initial caries test sample, bovine anterior teeth and crown labial enamel were used. The enamel surface was polished with # 1000, # 2400, and # 4000 polishing paper. A 3.5 × 3.0 mm window was prepared by using Nail Enamel (Maybelin Co., Ltd.) as a test target site on the polished enamel surface, and 0.1 M lactate buffer (pH 4.5, 3.0 mM CaCl 2 , 1. 8 mM KH 2 PO 4 , 0.5% CMC) was immersed for 4 days at 37 ° C. to prepare an artificial initial caries. For control of the test, half of the crown crown side of the 3.5 × 3.0 mm window was further masked with Nail Enamel (manufactured by Maybelline), and used as a comparison target site (control). A test solution (test substance) was prepared by mixing toothpaste and liquid dentifrice with artificial saliva to form a suspension solution.
　再石灰化促進試験は、上記で作製した人工初期う蝕試験体を各々の試験溶液に１２日間浸漬した後、試験体をマイクロカッターにて歯軸に対して平行となるように約５００μｍ厚に切断し、その後、この切片を練り砥石及び天然砥石を用い、注水下にて約１００μｍ厚の平行薄切片となるように研磨を行った。 In the remineralization promotion test, the artificial initial caries test specimen prepared above was immersed in each test solution for 12 days, and then the specimen was about 500 μm thick so that it was parallel to the tooth axis with a microcutter. After cutting, this slice was ground using a grindstone and a natural grindstone to form parallel thin slices of about 100 μm thickness under water injection.
　研磨後、歯の再石灰化効果の確認を行うため、コンタクトマイクロラジオグラム（ＣＭＲ）撮影を行った（図１及び図２参照）。図中の「コントロール面」とは、実施例及び比較例の歯磨用組成物がどの程度再石灰化効果を有するかを比較対象とするための部分であり、人工初期う蝕の状態を維持したものである。人工初期う蝕（３．５×３．０mmのウインドウ）領域のうち、半分の部分である。図中の「処理面」とは、実施例及び比較例の試験溶液（被検物質）を作用させた部分である。 After polishing, contact microradiogram (CMR) imaging was performed to confirm the remineralization effect of the teeth (see FIGS. 1 and 2). “Control surface” in the figure is a part for comparing the degree of remineralization effect of the dentifrice compositions of Examples and Comparative Examples, and maintained the state of artificial initial caries. Is. Half of the artificial initial caries (3.5 × 3.0 mm window) region. The “treated surface” in the figure is a portion on which the test solutions (test substances) of Examples and Comparative Examples are applied.
　また、人工初期う蝕部位の再石灰化の効果について、コンピュータを用いて解析を行った。
　コンピュータでの画像解析は、Angmerらの式（B.Angmer, D.Carlstrom and J.E..Glas : Studies on Ultrastructure of Dental Enemel IV : The Mineralization of normal Human Enamel, J. Ultrastructure.Res.8, 12-23, 1963）を基に再石灰化したミネラル量を算出し、Damatoらの方法（F.A. Damato, R.Stang and K.W.Stephen : Effect of Fluoride Concentration on Reminerelization of Carious Enamel : an in vitro pH-CyclingStudy, Caries Res, 24, 174-180,1990）に従って、各切片のコントロール面と処理面のミネラル喪失量△Z（%volume mineral・μｍ）を算出した。なお、再石灰化率は、以下の式により算出した。 In addition, the effect of remineralization of the artificial initial caries site was analyzed using a computer.
Computer image analysis was performed using the equation of Angmer et al. (B. Angmer, D. Carlstrom and JE. Glas: Studies on Ultrastructure of Dental Enemel IV: The Mineralization of normal Human Enamel, J. Ultrastructure. Res. 8, 12-23. , 1963) to calculate the amount of minerals remineralized, and the method of Damato et al. (FA Damato, R. Stang and KW Stephen: Effect of Fluoride Concentration on Reminerelization of Carious Enamel 24, 174-180, 1990), the amount of mineral loss ΔZ (% volume mineral · μm) between the control surface and the treated surface of each section was calculated. In addition, the remineralization rate was computed by the following formula | equation.
Figure JPOXMLDOC01-appb-M000001
Figure JPOXMLDOC01-appb-M000001
　表３３及び３４は、かかるコンピュータ画像解析法により歯磨用組成物の再石灰化の促進効果を確認した結果である。 Tables 33 and 34 show the results of confirming the effect of promoting remineralization of the dentifrice composition by the computer image analysis method.
Figure JPOXMLDOC01-appb-T000033
Figure JPOXMLDOC01-appb-T000033
Figure JPOXMLDOC01-appb-T000034
Figure JPOXMLDOC01-appb-T000034
　比較例１～６に示されるように、群青組成物単独では、歯牙の再石灰化効果はほとんどない。また、比較例３７～３９と比較例４０～４２との比較から明らかなように、第二リン酸カルシウムに群青組成物を加えても、歯牙の再石灰化効果の向上はほとんどみられない。 As shown in Comparative Examples 1 to 6, the ultramarine composition alone has almost no tooth remineralization effect. Further, as is clear from the comparison between Comparative Examples 37 to 39 and Comparative Examples 40 to 42, even when the ultramarine composition is added to dicalcium phosphate, the improvement of the remineralization effect of the teeth is hardly observed.
　これに対して、ハイドロキシアパタイト又はリン酸三カルシウムに群青組成物を加えた場合には、歯牙の再石灰化効果の相乗的な向上効果がみられる。
　具体的に、例えば、
　実施例１（再石灰化率：19.9％）と比較例１及び比較例１２（合計再石灰化率：14.5％）、
　実施例２（再石灰化率：20.0％）と比較例２及び比較例７（合計再石灰化率：9.4％）、
　実施例５（再石灰化率：34.3％）と比較例３及び比較例９（合計再石灰化率：11.5％）、
　実施例１０（再石灰化率：24.8％）と比較例４及び比較例１１（合計再石灰化率：13.2％）、
　実施例１１（再石灰化率:20.7％）と比較例５及び比較例８（合計再石灰化率：9.8％）、
　実施例１２（再石灰化率：23.6％）と比較例６及び比較例１２（合計再石灰化率：15.3％）、
　実施例１３（再石灰化率：11.1％）と比較例１及び比較例１８（合計再石灰化率：7.7％）、
　実施例１４（再石灰化率：11.1％）と比較例２及び比較例１３（合計再石灰化率：3.8％）、
　実施例１７（再石灰化率：21.8％）と比較例３及び比較例１５（合計再石灰化率：7.3％）、
　実施例２２（再石灰化率：15.4％）と比較例４及び比較例１７（合計再石灰化率：8.1％）、
　実施例２３（再石灰化率：11.4％）と比較例５及び比較例１４（合計再石灰化率：4.9％）、
　実施例２４（再石灰化率：14.0％）と比較例６及び比較例１８（合計再石灰化率：8.5％）、
等の比較からその相乗効果は明らかである。 On the other hand, when an ultramarine composition is added to hydroxyapatite or tricalcium phosphate, a synergistic improvement effect of the remineralization effect of the teeth is observed.
Specifically, for example,
Example 1 (remineralization rate: 19.9%) and Comparative Example 1 and Comparative Example 12 (total remineralization rate: 14.5%),
Example 2 (remineralization rate: 20.0%), Comparative Example 2 and Comparative Example 7 (total remineralization rate: 9.4%),
Example 5 (remineralization rate: 34.3%) and Comparative Example 3 and Comparative Example 9 (total remineralization rate: 11.5%),
Example 10 (remineralization rate: 24.8%), Comparative Example 4 and Comparative Example 11 (total remineralization rate: 13.2%),
Example 11 (remineralization rate: 20.7%), Comparative Example 5 and Comparative Example 8 (total remineralization rate: 9.8%),
Example 12 (remineralization rate: 23.6%) and Comparative Example 6 and Comparative Example 12 (total remineralization rate: 15.3%),
Example 13 (remineralization rate: 11.1%) and Comparative Example 1 and Comparative Example 18 (total remineralization rate: 7.7%),
Example 14 (remineralization rate: 11.1%), Comparative Example 2 and Comparative Example 13 (total remineralization rate: 3.8%),
Example 17 (remineralization rate: 21.8%) and Comparative Example 3 and Comparative Example 15 (total remineralization rate: 7.3%)
Example 22 (remineralization rate: 15.4%) and Comparative Example 4 and Comparative Example 17 (total remineralization rate: 8.1%),
Example 23 (remineralization rate: 11.4%), Comparative Example 5 and Comparative Example 14 (total remineralization rate: 4.9%),
Example 24 (remineralization rate: 14.0%) and Comparative Example 6 and Comparative Example 18 (total remineralization rate: 8.5%),
The synergistic effect is clear from the comparison.
　さらに、珪酸ナトリウムを加えた場合には、例えば、実施例２５～３６と実施例１～１２との比較から明らかなように、再石灰化作用はさらに向上する。 Further, when sodium silicate is added, the remineralization action is further improved, as is apparent from the comparison between Examples 25 to 36 and Examples 1 to 12, for example.
　本発明の歯磨用組成物は、歯牙の再石灰化に大変優れており、産業上の有用性は高い。 The dentifrice composition of the present invention is very excellent in remineralization of teeth and has high industrial utility.

Claims (7)

  1. 　群青組成物と、ハイドロキシアパタイト及びリン酸三カルシウムから選ばれるリン酸カルシウムとを含有することを特徴とする歯磨用組成物。 A dentifrice composition comprising an ultramarine composition and calcium phosphate selected from hydroxyapatite and tricalcium phosphate.
  2. 　群青組成物が、Ｎａ（６～10）Ａｌ６Ｓｉ６Ｏ２４Ｓ（２～４）で表される組成物であることを特徴とする請求項１に記載の歯磨用組成物。 The dentifrice composition according to claim 1, wherein the ultramarine composition is a composition represented by Na ( 6-10 ) Al 6 Si 6 O 24 S (2-4) .
  3. 　群青組成物の配合量が、０．０００１～０．５重量％であることを特徴とする請求項１又は２に記載の歯磨用組成物。 The dentifrice composition according to claim 1 or 2, wherein the blending amount of the ultramarine composition is 0.0001 to 0.5% by weight.
  4. 　ハイドロキシアパタイトの配合量が、０．００１～３０重量％である請求項１及至３の何れかに記載の歯磨用組成物。 4. The dentifrice composition according to claim 1, wherein the amount of hydroxyapatite is 0.001 to 30% by weight.
  5. 　リン酸三カルシウムの配合量が、０．００１～３０重量％である請求項１及至３の何れかに記載の歯磨用組成物。 The dentifrice composition according to any one of claims 1 to 3, wherein the amount of tricalcium phosphate is 0.001 to 30% by weight.
  6. 　更に珪酸ナトリウムを配合したことを特徴とする請求項１及至５の何れかに記載の歯磨用組成物。 The dentifrice composition according to any one of claims 1 to 5, further comprising sodium silicate.
  7. 　珪酸ナトリウムの配合量が、０．０１～２０．０重量％であることを特徴とする請求項６に記載の歯磨用組成物。  The dentifrice composition according to claim 6, wherein the amount of sodium silicate is 0.01 to 20.0 wt%.
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