JP3623660B2 - Synthetic lapis lazuli raw material and method for producing synthetic lapis lazuli - Google Patents
Synthetic lapis lazuli raw material and method for producing synthetic lapis lazuli Download PDFInfo
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Description
【０００１】
【発明の属する技術分野】
本発明は合成ラピスラズリ原料とそれを用いた合成ラピスラズリの製造方法に関する。
【０００２】
【従来の技術】
ラピスラズリは、日本名を青金石といい、古くから装身具や飾り石として珍重されるとともに、粉末にして絵の具などの顔料としても用いられてきた。ラピスラズリは、方ソーダ石族として一括される鉱物のひとつである。方ソーダ石族の鉱物はどれも同じ結晶構造をもっており、アルミニウム（Ａｌ）または珪素（Ｓｉ）を四つの酸素（Ｏ）が囲む四面体の中に、ナトリウム（Ｎａ）、カルシウム（Ｃａ）と、硫黄（Ｓ）、四酸化硫黄、塩素（Ｃｌ）が入った構造を有している。結晶系は立法晶系であり、モース硬度は５〜６で、比重は２．４程度である。
【０００３】
このようなラピスラズリを人工的に製造するために、本発明者は、特願平９−２９７０５７号において、ウルトラマリン１０〜９０質量％、炭酸カルシウム５〜６０質量％、ポルトランドセメント５〜８５質量％から成る基本原料１００質量％に対し、粒径４０〜１０００μｍのパイライトを１５質量％以下となるように添加して調製、水で養生して合成する方法を提案した。
【０００４】
【発明が解決しようとする課題】
ところが、この従来の合成ラピスラズリは、天然のラピスラズリと同様の結晶相を持ち、同様の色と質感を呈するものの、天然ラピスラズリに比べると硬度が低いため（モース硬度：天然５〜６、合成３）、湿式研磨では鏡面が出しにくく、また通常のゴミ（砂埃などは殆ど珪酸塩鉱物であるため、モース硬度は５程度）等で傷が入りやすいという問題があった。
【０００５】
そこで、本発明者はかかる課題を解決するべく鋭意研究を行った結果、発色調整剤の炭酸カルシウムを添加することなく、結合剤をポルトランドセメント以外に粉末珪酸ソーダを添加し、粉末珪酸ソーダのＮａ溶出抑制剤としてトリポリリン酸二水素アルミニウムを添加し、粉末珪酸ソーダとトリポリリン酸二水素アルミニウムの化学反応とポルトランドセメントの水和反応を促進させるために水を添加して１５０℃〜２５０℃、１時間、１ｔｆ／ｃｍ２ の条件でホットプレスして合成することにより上記課題を解決することができることを知見した。
【０００６】
本発明は、このような知見に基づいてなされたものであり、天然のラピスラズリと同様の結晶相と色彩と質感をもち、かつ天然のラピスラズリと同等の硬度を有する合成ラピスラズリ原料とそれを用いた合成ラピスラズリの製造方法を提供することを目的とする。
【０００７】
【課題を解決するための手段】
上記目的を達成するために、本発明に係る合成ラピスラズリ原料は、ウルトラマリンを４５〜６５質量％、ポルトランドセメントを１５〜３５質量％、粉末珪酸ソーダを１５〜３０質量％、トリポリリン酸二水素アルミニウムを前記粉末珪酸ソーダの３０〜４０質量％添加した基本原料１００質量％に対し、粒径が４０〜１０００μｍのパイライトを１５質量％まで添加すると共に、水を１０〜２０質量％添加して成る。
【０００８】
また、本発明に係る合成ラピスラズリの製造方法によれば、上記原料を１５０〜２５０℃、１時間、１ｔｆ／ｃｍ２ でホットプレスして合成する。
【０００９】
【発明の実施の形態】
以下、本発明の実施形態を詳細に説明する。本発明では、着色剤として合成ウルトラマリン（Ｎａ６ Ａｌ６ Ｓｉ６ Ｏ２ Ｓｘ ）を４５〜６５質量％添加する。ラピスラズリが美しい青色に発色するには、ウルトラマリンが不可欠である。この発色の原因は、珪酸塩中にコロイド状の遊離硫黄が分散しているためである。ウルトラマリンは、耐熱性、耐アルカリ性が小さく、容易に硫黄が珪酸塩の中から遊離して脱色し易い着色剤である。したがって、ウルトラマリンの添加量が４５質量％未満であるとポルトランドセメントや粉末珪酸ソーダのアルカリ成分が多くなり、しかもホットプレスにより加熱されるため、ウルトラマリンが脱色してしまう。また、このウルトラマリンが６５質量％を超えると必然的に結合剤の添加量が減り、硬度が小さくなってクラックも多発する。
【００１０】
結合剤としてポルトランドセメントを１５〜３５質量％と粉末珪酸ソーダを１５〜３０質量％添加し、助材としてトリポリリン酸二水素アルミニウムを粉末珪酸ソーダの３０〜４０質量％の範囲で使用する。ポルトランドセメントだけでは天然ラピスと同じ硬さ（モース硬度５）まで向上させることができないが、粉末珪酸ソーダを加えることにより、硬度を大幅に向上させることができる。
【００１１】
但し、粉末珪酸ソーダは不安定な材料であるため、助材が必要である。まず、耐水性を向上させるためにゲル化剤が必要であるが、これはポルトランドセメントがゲル化剤の役割を果たす（水和反応時にアルカリ性になり、そのとき珪酸ソーダがゲル化する）。
【００１２】
次に、ナトリウム（Ｎａ）が析出して白華が生じるため、トリポリリン酸二水素アルミニウムを添加して粉末珪酸ソーダ中のナトリウムと化学反応させて（ＡｌＨ２ Ｐ３ ＋２Ｎａ＋ →ＡｌＮａ２ Ｐ３ Ｏ１０＋２Ｈ＋ ）、ナトリウムの析出を防ぐようにした。但し、トリポリリン酸二水素アルミニウムの添加量は、粉末珪酸ソーダの３０〜４０質量％にする。３０質量％未満では白華を完全に抑制することができず、４０質量％を超えると硬度が低くなり、クラックが多発する。
【００１３】
このポルトランドセメントの添加量が１５質量％未満になると、珪酸ソーダを充分にゲル化できないため、合成したラピスは耐水性が悪くなり、湿式研磨では鏡面がでない。一方、ポルトランドセメントの添加量が３５質量％を超えると粉末珪酸ソーダの添加量が１５質量％未満になり、硬度が天然ラピスラズリと同等までには向上せず、湿式研磨で鏡面がでない。さらに、粉末珪酸ソーダの添加量が３０質量％を超えるとポルトランドセメントの添加量が１５質量％未満となり、珪酸ソーダを充分にゲル化することができず、耐水性が悪くなり、湿式研磨では鏡面がでない。
【００１４】
上記基本原料に対し、粒径４０〜１０００μｍのパイライトを１５質量％以下となるように添加する。このパイライトの粒径が４０μｍ未満では、パイライトが目立たず、添加する意味がなくなる。一方、１０００μｍを超えると美観を損ねる。また、このパイライトの添加量については、１５質量％を超えると合成ラピスラズリの色調が非常に暗くなる。
【００１５】
水（Ｈ２ Ｏ）は、粉末珪酸ソーダとトリポリリン酸二水素アルミニウムの化学反応とポルトランドセメントの水和反応を促進させるために１０〜２０質量％添加する。添加量が１０質量％未満では粉末珪酸ソーダとトリポリリン酸二水素アルミニウムが充分にイオン交換できないため、Ｎａの溶出を完全に抑えることができずに白華し、またポルトランドセメントの水和結合および粉末珪酸ソーダの化学結合が不十分となるため、硬度が低くなり、鏡面がでにくくなる。一方、２０質量％を超えるとホットプレス時に水が型から流れ出し、その時水に熔解している結合剤も流れ出るため、クラックが多発する。
【００１６】
この原料を使ってホットプレス法によりラピスラズリを合成する。ホットプレスは１ｔｆ／ｃｍ２ で加圧した後、１５０℃〜２５０℃で１時間程度加熱する。加熱温度が１５０℃未満であると、結合剤を充分に化学反応させることができないため、硬度が上がらず、鏡面が出にくくなる。一方、２５０℃を超えると、ウルトラマリンの硫黄が遊離し、色が脱色するという問題が発生する。
【００１７】
【実施例】
平均粒径１．５μｍのウルトラマリン（ＳｉＯ２ ：３８．１％、Ａｌ２ Ｏ３ ：２３．７％、Ｎａ２ Ｏ：２６．０％、Ｓ：１２．０％）、平均粒径４μｍのポルトランドセメント（ＳｉＯ２ ：２９．０％、Ａｌ２ Ｏ３ ：１３．２％、Ｆｅ２ Ｏ３ ：１．２％、ＣａＯ：４９．２％、ＭｇＯ：５．６％、ＳＯ３ ：１．２％）、平均粒径１２μｍの粉末珪酸ソーダ（ＳｉＯ２ ：５７〜６１％、Ｎａ２ Ｏ：１８〜２０％）、平均粒径６μｍのトリポリリン酸二水素アルミニウム（ＡｌＨ２ Ｐ３ Ｏ１６・２Ｈ２ Ｏ）を所定の組成となるように混合して基本原料を作り、これにパイライト粉末とイオン交換水を基本原料に対し所定量添加した後、攪拌機で混合してラピスラズリ原料を作製した。この原料を型にチャージし、１ｔｆ／ｃｍ２ 加圧後、所定の温度１時間でホットプレスして合成ラピスラズリを作製した。
【００１８】
これをラッピング研磨した後、色調・鏡面・クラック・白華について官能検査し、また硬度を調べた。その結果を表１に示す。なお、質感はパイライトが美しく混入しているものは○に、パイライトの量が多すぎたり、大きすぎたり、小さすぎたりして美観を損ねるものは×に、パイライトが無添加のものは−にそれぞれ分類した。色調は天然のラピスラズリと同じものは○に、異なるものは×に分類した。白華はデシケータの底に純水を張り、その中で合成したラピスラズリを１ケ月間保管し、白華しなかったものは○に、白華したものは×に分類した。鏡面は美しいものは○に、汚いものは×に、評価できなかったものは−に分類した。硬度はモース硬度を調べた。総合評価は良かったものは○、悪かったものは×に分類した。
【００１９】
また、この合成ラピスラズリをＸＲＤ（Ｘ線回折）分析した結果、ｈａｕｙｎｉｔｅ（藍方石）、ｎｏｓｅｌｉｔｅ（ノゼアン）、ｌａｚｕｒｉｔｅ（天藍石）、ｐｙｒｉｔｅ（パイライト）が検出され、天然ラピスを同じであることが確認された。
【００２０】
【表１】
表１から明らかなように、ウルトラマリンを４５〜６５質量％、ポルトランドセメントを１５〜３５質量％、粉末珪酸ソーダを１５〜３０質量％、トリポリリン酸二水素アルミニウムを粉末珪酸ソーダの３０〜４０質量％添加した基本原料１００質量％に対し、粒径が４０〜１０００μｍのパイライトを１５質量％まで添加すると共に、水を１０〜２０質量％添加して成る合成ラピスラズリ原料を用いた場合、質感、色調もよく、モース硬度も天然ラピスラズリとほぼ同等のラピスラズリが得られる。
【００２２】
【発明の効果】
以上のように、本発明に係る合成ラピスラズリ原料によれば、ウルトラマリンを４５〜６５質量％、ポルトランドセメントを１５〜３５質量％、粉末珪酸ソーダを１５〜３０質量％、トリポリリン酸二水素アルミニウムを粉末珪酸ソーダの３０〜４０質量％添加した基本原料１００質量％に対し、粒径が４０〜１０００μｍのパイライトを１５質量％まで添加すると共に、水を１０〜２０質量％添加して成ることから、天然と同レベルの硬度（モース硬度５）を有するラピスラズリが合成できるようになり、従来の合成ラピスラズリよりも傷つきにくく、湿式研磨できれいに鏡面ができるようになる。また、天然と同等の色彩と質感を有する合成ラピスラズリが合成できる。さらに、天然と同じ結晶相のラピスラズリが合成できる。
【００２３】
また、本発明の合成ラピスラズリの製造方法によれば、上記合成ラピスラズリ原料を１５０〜２５０℃、１時間、１ｔｆ／ｃｍ２ でホットプレスして合成することから、天然と同レベルの硬度（モース硬度５）を有するラピスラズリが合成できるようになり、従来の合成ラピスラズリよりも傷つきにくく、湿式研磨できれいに鏡面ができるようになる。また、天然と同等の色彩と質感を有する合成ラピスラズリが合成できる。さらに、天然と同じ結晶相のラピスラズリが合成できる。[0001]
BACKGROUND OF THE INVENTION
The present invention relates to a synthetic lapis lazuli raw material and a method for producing a synthetic lapis lazuli using the raw material.
[0002]
[Prior art]
Lapis lazuli is called Japanese blue gold stone, and has long been prized as a jewelery and ornamental stone. It has also been used as a pigment for paints in powder form. Lapis lazuli is one of the minerals grouped as the sodalite group. All the sodalite group minerals have the same crystal structure, and in the tetrahedron surrounded by four oxygen (O) aluminum (Al) or silicon (Si), sodium (Na), calcium (Ca), It has a structure containing sulfur (S), sulfur tetroxide, and chlorine (Cl). The crystal system is a cubic system, the Mohs hardness is 5 to 6, and the specific gravity is about 2.4.
[0003]
In order to artificially produce such a lapis lazuli, the present inventor in Japanese Patent Application No. 9-297057, Ultramarine 10-90 mass%, calcium carbonate 5-60 mass%, Portland cement 5-85 mass% A method was proposed in which pyrite with a particle size of 40 to 1000 μm was added to 100% by mass of the basic raw material consisting of the above, and was synthesized by curing with water.
[0004]
[Problems to be solved by the invention]
However, although this conventional synthetic lapis lazuli has the same crystal phase as natural lapis lazuli and exhibits the same color and texture, it has lower hardness than natural lapis lazuli (Mohs hardness: natural 5-6, synthetic 3). However, there is a problem that the mirror surface is difficult to be obtained by wet polishing, and scratches are likely to occur due to ordinary dust (Most hardness is about 5 because sand dust and the like are mostly silicate minerals).
[0005]
Therefore, as a result of intensive studies to solve such problems, the present inventor added powdered sodium silicate in addition to Portland cement, without adding calcium carbonate as a color adjusting agent, and added sodium silicate in powdered sodium silicate. Aluminum dihydrogen phosphate as an elution inhibitor was added, and water was added at 150 ° C. to 250 ° C. for 1 hour in order to promote chemical reaction between powdered sodium silicate and aluminum trihydrogen phosphate and hydration reaction of Portland cement. It has been found that the above-mentioned problems can be solved by hot pressing under a condition of 1 tf / cm 2 and synthesis.
[0006]
The present invention has been made based on such knowledge, and a synthetic lapis lazuli raw material having a crystal phase, color and texture similar to those of natural lapis lazuli and having a hardness equivalent to that of natural lapis lazuli, and the same are used. It aims at providing the manufacturing method of synthetic lapis lazuli.
[0007]
[Means for Solving the Problems]
In order to achieve the above object, the synthetic lapis lazuli raw material according to the present invention comprises 45 to 65% by mass of ultramarine, 15 to 35% by mass of Portland cement, 15 to 30% by mass of powdered sodium silicate, and aluminum dihydrogen tripolyphosphate. Is added to 15% by mass of pyrite having a particle size of 40 to 1000 μm and 10 to 20% by mass of water with respect to 100% by mass of the basic raw material to which 30 to 40% by mass of the powdered sodium silicate is added.
[0008]
Further, according to the method for producing a synthetic lapis lazuli according to the present invention, the raw materials are synthesized by hot pressing at 150 to 250 ° C. for 1 hour at 1 tf / cm 2 .
[0009]
DETAILED DESCRIPTION OF THE INVENTION
Hereinafter, embodiments of the present invention will be described in detail. In the present invention, 45 to 65% by mass of synthetic ultramarine (Na 6 Al 6 Si 6 O 2 S x ) is added as a colorant. Ultramarine is indispensable in order for lapis lazuli to develop a beautiful blue color. The cause of this color development is that colloidal free sulfur is dispersed in the silicate. Ultramarine is a colorant that has low heat resistance and alkali resistance, and easily releases sulfur from silicates and easily decolorizes. Accordingly, when the amount of ultramarine added is less than 45% by mass, the alkali components of Portland cement and powdered sodium silicate increase, and the ultramarine is decolored because it is heated by hot pressing. Moreover, when this ultramarine exceeds 65 mass%, the addition amount of a binder will inevitably decrease, hardness will become small and a crack will occur frequently.
[0010]
Portland cement is added in an amount of 15 to 35% by mass and powdered sodium silicate in an amount of 15 to 30% by mass, and aluminum tripolyphosphate is used as an auxiliary agent in the range of 30 to 40% by mass of the powdered sodium silicate. Portland cement alone cannot be improved to the same hardness as natural lapis (Mohs hardness 5), but by adding powdered sodium silicate, the hardness can be greatly improved.
[0011]
However, since powdered sodium silicate is an unstable material, an auxiliary material is required. First, in order to improve water resistance, a gelling agent is necessary. This is because Portland cement plays the role of a gelling agent (becomes alkaline during the hydration reaction, and then sodium silicate gels).
[0012]
Next, since sodium (Na) is precipitated and white flower is generated, aluminum dihydrogen phosphate is added and chemically reacted with sodium in powdered sodium silicate (AlH 2 P 3 + 2Na + → AlNa 2 P 3 O 10 + 2H + ) to prevent precipitation of sodium. However, the addition amount of aluminum dihydrogen tripolyphosphate is 30 to 40% by mass of powdered sodium silicate. If it is less than 30% by mass, white flower cannot be completely suppressed, and if it exceeds 40% by mass, the hardness decreases and cracks occur frequently.
[0013]
When the amount of Portland cement added is less than 15% by mass, sodium silicate cannot be sufficiently gelled, so that the synthesized lapis has poor water resistance, and does not have a mirror surface in wet polishing. On the other hand, when the addition amount of Portland cement exceeds 35% by mass, the addition amount of powdered sodium silicate becomes less than 15% by mass, the hardness is not improved to the same level as natural lapis lazuli, and the mirror surface is not obtained by wet polishing. Further, if the amount of powdered sodium silicate exceeds 30% by mass, the amount of Portland cement added is less than 15% by mass, so that the sodium silicate cannot be sufficiently gelled, resulting in poor water resistance. Is not.
[0014]
Pyrite having a particle size of 40 to 1000 μm is added to the basic raw material so as to be 15% by mass or less. If the particle size of the pyrite is less than 40 μm, the pyrite is not conspicuous and the meaning of adding is lost. On the other hand, if it exceeds 1000 μm, the beauty is impaired. Further, when the amount of pyrite added exceeds 15% by mass, the color tone of the synthetic lapis lazuli becomes very dark.
[0015]
Water (H 2 O) is added in an amount of 10 to 20% by mass in order to promote the chemical reaction between powdered sodium silicate and aluminum dihydrogen triphosphate and the hydration reaction of Portland cement. If the addition amount is less than 10% by mass, the powdered sodium silicate and aluminum dihydrogen tripolyphosphate cannot be sufficiently ion-exchanged, so that the elution of Na cannot be completely suppressed and whitening occurs. Since the chemical bond of sodium silicate becomes insufficient, the hardness is lowered and the mirror surface is difficult to be seen. On the other hand, when it exceeds 20% by mass, water flows out from the mold during hot pressing, and the binder dissolved in the water also flows out at that time, so that cracks frequently occur.
[0016]
Using this raw material, lapis lazuli is synthesized by hot pressing. The hot press is pressurized at 1 tf / cm 2 and then heated at 150 to 250 ° C. for about 1 hour. When the heating temperature is less than 150 ° C., the binder cannot be sufficiently chemically reacted, so the hardness does not increase and the mirror surface is difficult to appear. On the other hand, when it exceeds 250 degreeC, the sulfur of ultramarine will liberate and the problem that a color decolorizes will generate | occur | produce.
[0017]
【Example】
Ultramarine (SiO 2 : 38.1%, Al 2 O 3 : 23.7%, Na 2 O: 26.0%, S: 12.0%) having an average particle diameter of 1.5 μm, an average particle diameter of 4 μm Portland cement (SiO 2: 29.0%, Al 2 O 3: 13.2%, Fe 2 O 3: 1.2%, CaO: 49.2%, MgO: 5.6%, SO 3: 1. 2%), average particle diameter 12μm powder sodium silicate (SiO 2: 57~61%, Na 2 O: 18~20%), the average particle size 6μm of dihydrogen tripolyphosphate aluminum (AlH 2 P 3 O 16 · 2H A basic raw material was prepared by mixing 2 O) so as to have a predetermined composition. After adding a predetermined amount of pyrite powder and ion-exchanged water to the basic raw material, a lapis lazuli raw material was prepared by mixing with a stirrer. This raw material was charged into a mold, pressed after 1 tf / cm 2 , and hot pressed at a predetermined temperature for 1 hour to produce a synthetic lapis lazuli.
[0018]
After lapping and polishing this, a sensory test was performed on the color tone, mirror surface, cracks, and whiteness, and the hardness was examined. The results are shown in Table 1. In addition, the texture is ◯ when the pyrite is beautifully mixed, ○ when the amount of the pyrite is too large, too large, or too small to impair the aesthetic, and minus if the pyrite is not added. Each was classified. Colors that were the same as natural lapis lazuli were classified as ○, and those that were different were classified as ×. Hakuhana sprinkled pure water on the bottom of the desiccator, and the lapis lazuli synthesized in it was stored for 1 month. The beautiful mirror surface was classified as ○, the dirty one as ×, and the one that could not be evaluated as-. For the hardness, the Mohs hardness was examined. The overall evaluation was classified as “good”, and the poor evaluation was classified as “poor”.
[0019]
In addition, as a result of XRD (X-ray diffraction) analysis of this synthetic lapis lazuli, haunite (indigo stone), noselite (nozean), lazurite (pyrolite) and pyrite (pyrite) are detected, and natural lapis is the same confirmed.
[0020]
[Table 1]
As is apparent from Table 1, Ultramarine is 45 to 65% by mass, Portland cement is 15 to 35% by mass, Powdered sodium silicate is 15 to 30% by mass, Tripolyaluminum dihydrogen phosphate is 30 to 40% by mass of powdered sodium silicate. When using a synthetic lapis lazuli raw material containing up to 15% by weight of pyrite having a particle size of 40 to 1000 μm and 10 to 20% by weight of water based on 100% by weight of the basic raw material added, the texture and color tone A lapis lazuli with a Mohs hardness of almost the same as a natural lapis lazuli can be obtained.
[0022]
【The invention's effect】
As mentioned above, according to the synthetic lapis lazuli raw material which concerns on this invention, ultramarine 45-65 mass%, Portland cement 15-35 mass%, powdered sodium silicate 15-30 mass%, tripolyphosphate aluminum dihydrogen From the addition of up to 15% by mass of pyrite having a particle size of 40-1000 μm and 100% by mass of the basic raw material added by 30-40% by mass of powdered sodium silicate, A lapis lazuli having the same level of hardness (Mohs hardness 5) as natural can be synthesized, and it is less likely to be scratched than a conventional synthetic lapis lazuli, and a fine mirror surface can be formed by wet polishing. In addition, a synthetic lapis lazuli having a color and texture equivalent to those of nature can be synthesized. Furthermore, a lapis lazuli having the same crystal phase as that of nature can be synthesized.
[0023]
In addition, according to the method for producing a synthetic lapis lazuli of the present invention, the synthetic lapis lazuli raw material is synthesized by hot pressing at 150 to 250 ° C. for 1 hour at 1 tf / cm 2. A lapis lazuli having 5) can be synthesized, is less likely to be scratched than a conventional synthetic lapis lazuli, and can be mirror-finished with wet polishing. In addition, a synthetic lapis lazuli having a color and texture equivalent to those of nature can be synthesized. Furthermore, a lapis lazuli having the same crystal phase as that of nature can be synthesized.
Claims (2)
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| JP21466498A JP3623660B2 (en) | 1998-07-29 | 1998-07-29 | Synthetic lapis lazuli raw material and method for producing synthetic lapis lazuli |
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| Application Number | Priority Date | Filing Date | Title |
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| JP21466498A JP3623660B2 (en) | 1998-07-29 | 1998-07-29 | Synthetic lapis lazuli raw material and method for producing synthetic lapis lazuli |
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| JP3623660B2 true JP3623660B2 (en) | 2005-02-23 |
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