201041824 六、發明說明： 【發明所屬之技術領域】 本發明係有關由鈦酸鋁系陶瓷形成之燒成體的製造方 法，更詳細而言之，係有關燒成含有鋁源粉末、鈦源粉末 及鎂源粉末之原料混合物的成形體，製造由鈦酸鋁系陶瓷 形成之燒成體的方法。 Q 【先前技術】 已知鈦酸系陶瓷爲含有構成元素之鈦及鋁，X射線繞 射光譜中具有鈦酸鋁之結晶圖型的陶瓷中，具有耐熱性優 異之陶瓷。先前鈦酸鋁系陶瓷係可作爲坩堝般燒結用器具 等’但近年來作爲，構成捕集由柴油機等內燃機關排出之 排氣所含的微粒子用之陶瓷濾器的材料，以提高產業上之 利用價値。 已知鈦酸鋁系陶瓷係例如由鈦酸鋁鎂結晶形成之陶瓷 Ο 。日本專利文獻1中揭示藉由燒成含有二氧化鈦陶瓷等之 含有τ i化合物、氧化鋁陶瓷等之含有A1化合物、氧化鎂 陶瓷等之含有Mg化合物的原料混合物或是該成形體，調 製鈦酸鋁鎂燒成體。 先前技術文獻 [專利文獻] [專利文獻1 ]日本國際公開第05/ 1 〇57〇4號文獻 201041824 【發明內容】 發明所欲解決之課題 如上所述，使用含有各種金屬成份之陶瓷粉末混合物 ，藉由將該混合物預先成形爲成形體後進行燒成，得到鈦 鋁鎂系燒成體時，欲得到機械強度高的燒成體，使陶瓷粉 末彼此之間堅固地黏結，必須於上述混合物中添加相當大 量之黏合劑（結合劑）。 但是，一般使用之有機系黏合劑係含有許多碳之化合 物，且藉由在成形體之燒成時的氣化-分解，具有使大量 之碳化物產生之問題。如此之碳化物係藉由在例如燒成過 程中加入大量之熱能，可除去或減低，但是於燒成時之熱 能必須過剩，則產生二氧化碳及招致於燒成體中殘留灰分 與碳分等之問題。 因此，本發明之目的係提供不使用黏合劑、或是即使 黏合劑之使用量少時，可製造具有良好的機械特性之鈦酸 鋁鎂燒成體的方法。 用以解決課題之手段 本發明係提供備有將含有鋁源粉末 '鈦源粉末及鎂源 粉末之原料混合物的成形體進行燒成之步驟，且該鎂源粉 末爲含有水滑石系化合物之鈦酸鋁系燒成體的製造方法。 本發明中上述原料混合物係可不含黏合劑。依據本發 明，不使用黏合劑，可得機械強度高之鈦酸鋁系燒成體。 另一方面，本發明中上述原料混合物係可含有黏合劑，但 -6- 201041824 是依據本發明，即使該使用量十分低時，可得機械強度優 異之鈦酸鋁系燒成體。上述原料混合物含有黏合劑時，黏 合劑之使用量係對於鋁源粉末、鈦源粉末及鎂源粉末之合 計量100質量份而言，可爲0.3質量份以下。 鎂源粉末中之水滑石系化合物以外之鎂源的含有量係 以MgO換算爲40質量。/。以下爲佳。又，MgO換算之鎂源 粉末的使用量係對於Ti〇2換算之鈦源粉末的使用量與 0 Al2〇3換算之鋁源粉末的使用量之合計量10〇質量份而言 ’ 0.1〜I5質量份爲佳。鎂源粉末之體積基準的累積百分 比5 0 %相當粒子徑（D 5 0 )係0 . 1〜1 ο μηι爲佳。201041824 VI. Description of the Invention: [Technical Field] The present invention relates to a method for producing a fired body formed of an aluminum titanate-based ceramic, and more particularly, relates to a powder containing aluminum source powder and titanium source powder. And a molded body of a raw material mixture of a magnesium source powder, and a method of producing a fired body formed of an aluminum titanate-based ceramic. Q [Prior Art] It is known that a titanic acid-based ceramic is a ceramic having a composition of titanium and aluminum and having a crystal pattern of aluminum titanate in an X-ray diffraction spectrum, and has a ceramic having excellent heat resistance. In the past, the aluminum titanate-based ceramics can be used as a ceramic-like device for the like, but in recent years, it is used as a ceramic filter for collecting fine particles contained in exhaust gas discharged from an internal combustion engine such as a diesel engine to improve industrial use. Price. Aluminum titanate-based ceramics are known, for example, ceramics formed of crystals of aluminum magnesium titanate. Japanese Laid-Open Patent Publication No. 1 discloses the preparation of a raw material mixture containing a Mn compound or the like, an alumina ceramic or the like, a raw material mixture containing an Mg compound such as an alumina compound, or the like, or a molded body thereof to prepare an aluminum titanate. Magnesium fired body. [Patent Document] [Patent Document 1] Japanese International Publication No. 05/1, No. 57, No. 4, 201041824 [Disclosure] Problems to be Solved by the Invention As described above, a ceramic powder mixture containing various metal components is used. When the mixture is previously molded into a molded body and then fired to obtain a titanium aluminum-magnesium-based fired body, a sintered body having high mechanical strength is obtained, and the ceramic powders are strongly bonded to each other, and must be in the above mixture. Add a considerable amount of binder (binder). However, the organic binder generally used contains a large amount of a carbon compound, and has a problem that a large amount of carbides are generated by vaporization-decomposition at the time of firing of the formed body. Such a carbide can be removed or reduced by adding a large amount of heat energy during, for example, the firing process, but the heat energy at the time of firing must be excessive, and carbon dioxide is generated and the residual ash and carbon in the fired body are caused. problem. Accordingly, an object of the present invention is to provide a method of producing a calcined aluminum titanate having good mechanical properties without using a binder or even when the amount of the binder used is small. Means for Solving the Problems The present invention provides a step of firing a molded body containing a raw material mixture of an aluminum source powder 'titanium source powder and a magnesium source powder, and the magnesium source powder is titanium containing a hydrotalcite-based compound. A method for producing an alumina-based fired body. In the present invention, the above raw material mixture may be free of a binder. According to the present invention, an aluminum titanate-based fired body having high mechanical strength can be obtained without using a binder. On the other hand, in the present invention, the raw material mixture may contain a binder, but -6-201041824 is based on the present invention, and even when the amount used is extremely low, an aluminum titanate-based fired body excellent in mechanical strength can be obtained. When the raw material mixture contains a binder, the amount of the binder used may be 0.3 parts by mass or less based on 100 parts by mass of the total of the aluminum source powder, the titanium source powder and the magnesium source powder. The content of the magnesium source other than the hydrotalcite-based compound in the magnesium source powder is 40 mass in terms of MgO. /. The following is better. In addition, the amount of the Mg source-converted magnesium source powder is 0.1 to I5 in terms of the total amount of the titanium source powder in terms of Ti〇2 and the amount of the aluminum source powder in terms of 0 Al2〇3. The quality is preferred. The cumulative percentage of the volume basis of the magnesium source powder is 50%, and the particle diameter (D 5 0 ) is preferably 0.1 to 1 ο μηι.
Ti 〇2換算之鈦源粉末的使用量係對於Ti02換算之鈦 源粉末的使用量與A 1 2 0 3換算之銘源粉末的使用量之合計 量100質量份而言’ 30〜70質量份爲佳。鋁源粉末之體 積基準的累積百分比50 %相當粒子徑（〇50)係0.1〜 50μιη爲佳，又，駄源粉末之體積基準的累積百分比50% 〇 相當粒子徑（D50 )係〇· 1〜50μιη爲佳。 上述原料混合物尙可含有矽源粉末。S i Ο 2換算之砂源 粉末之使用量係對於Ti02換算之鈦源粉末的使用量與 Α12〇3換算之鋁源粉末之使用量的合計量100質量份而言 爲0.1〜10質量份爲佳。 發明之效果 依據本發明之製造方法，可製造具有良好機械特性之 鈦鋁鎂系燒成體。又，依據本發明之製造方法，藉由黏合 201041824 劑、特別是有機系黏合劑之減低或不使用，可減低給予燒 成時之熱能同時’可防止或抑制在燒成時之二氧化碳之產 生及對燒成體之灰分、碳分等之殘留。 用以實施本發明之最佳形態 本發明之鈦酸鋁系燒成體係藉由將含有1種以上之鋁 源粉末、1種以上之鈦源粉末及1種以上之鎂源粉末之原 料混合物的成形體進行燒成被製造。使用如此之原料混合 物所得之鈦酸鋁系燒成體係鈦酸鋁鎂結晶形成之燒成體。 本發明所使用的原料混合物所含有之鋁源粉末係，作 爲構成鈦酸鋁系燒成體之鋁成份用的物質粉末，且稱爲僅 含有金屬成份之鋁的物質粉末。鋁源粉末係可舉例如氧化 鋁之粉末。氧化鋁可爲結晶性，或不定形（非晶質）。氧 化鋁爲結晶性時，其結晶係可舉例如r型、<5型、0型、 α型等，較佳爲使用α型之氧化鋁。 本發明所使用的鋁源粉末係，藉由於空氣中燒成而導 入氧化鋁之物質的粉末。如此之物質係可舉例如，鋁鹽、 烷氧化鋁、氫氧化鋁、鋁等。 鋁鹽可爲無機鹽，或有機鹽。鋁無機鹽之具體例如， 硝酸鋁 '硝酸銨鋁等之硝酸鹽；碳酸銨鋁等之碳酸鹽等。 鋁有機鹽係可舉例如，草酸鋁、乙酸鋁、硬脂酸鋁、乳酸 鋁、月桂酸鋁等。 又’烷氧化鋁之具體例如，異丙氧化鋁、乙氧化鋁、 sec-丁氧化鋁、tert_丁氧化鋁等。 201041824 氫氧化錯可爲結晶性，或不定形（非晶質）。氫氧化 鋁爲結晶性時，其結晶型可舉例如爲三水鋁礦型、三羥鋁 石型、二水銘石（Nordstrandite)型、勃姆石型、假軟水 鋁石（PSEUDO-BOEHMITE )型等。非晶質之氫氧化鋁又 可舉例如將鋁鹽、烷氧化鋁等水溶性鋁化合物之水溶液水 解所得之鋁水解物。 上述之中鋁源粉末係以使用氧化鋁粉末及氫氧化鋁粉 0 末爲佳’更佳爲α型之氧化鋁粉末。該鋁源粉末可含有製 造過程中無法避免含有的微量成份。 鋁源粉末之粒徑並不特別被限定，但是藉由雷射繞射 法被測定，可使用體積基準之累積百分比50%相當粒子徑 (D50)爲0.1〜50μπι者爲佳。由使鈦酸鋁鎂有效率生成 之觀點看來，鋁源粉末之D50係0.3〜30μπι更佳。 上述原料混合物所含的鈦源粉末爲，作爲構成鈦酸鋁 系燒成體之鈦成份用的物質粉末，且稱爲含有金屬元素之 D 鈦的物質。如此之物質係可舉例如氧化鈦之粉末。氧化鈦 係可舉例如，氧化鈦（IV )、氧化鈦（III )、氧化鈦（II )等，較佳爲使用氧化鈦（IV)。氧化鈦（IV )可爲結晶 性，或不定形（非晶質）。氧化鈦（IV )爲結晶性時，其 結晶型係可舉例例如爲銳鈦礦型、金紅石型、板鈦礦型等 ，較佳爲銳鈦礦型、金紅石型之氧化鈦（IV)。 本發明所使用的鈦源粉末可爲，藉由於空氣中燒成而 導入氧化鈦之物質粉末。如此之物質係可舉例如，鈦鹽、 烷氧化鈦、氫氧化鈦、氧化鈦、硫化鈦、鈦等。 -9- 201041824The use amount of the titanium source powder in terms of Ti 〇 2 is 30 to 70 parts by mass based on 100 parts by mass of the total amount of the Ti02-converted titanium source powder and the amount of the source powder of the A 1 2 0 3 conversion source. It is better. The cumulative percentage of the volume reference of the aluminum source powder is 50%. The particle diameter (〇50) is preferably 0.1 to 50 μm, and the cumulative percentage of the volume basis of the bismuth powder is 50%. 〇 The equivalent particle diameter (D50) is 〇·1~ 50μιη is preferred. The above raw material mixture 尙 may contain a ruthenium source powder. The use amount of the sand source powder in the range of SiO 2 is 0.1 to 10 parts by mass based on 100 parts by mass of the total amount of the titanium source powder in terms of Ti02 conversion and the amount of the aluminum source powder in terms of Α12〇3. good. EFFECT OF THE INVENTION According to the production method of the present invention, a titanium aluminum magnesium-based fired body having good mechanical properties can be produced. Moreover, according to the manufacturing method of the present invention, by reducing or not using the 201041824 agent, particularly the organic binder, the heat energy at the time of firing can be reduced while preventing or suppressing the generation of carbon dioxide during firing. Residues of ash, carbon, etc. of the fired body. BEST MODE FOR CARRYING OUT THE INVENTION The aluminum titanate-based firing system of the present invention comprises a raw material mixture containing one or more kinds of aluminum source powders, one or more kinds of titanium source powders, and one or more kinds of magnesium source powders. The formed body is fired and manufactured. A fired body formed by crystallizing an aluminum titanate-based calcination system of aluminum titanate obtained by using such a raw material mixture. The aluminum source powder contained in the raw material mixture used in the present invention is a material powder for the aluminum component constituting the aluminum titanate-based fired body, and is referred to as a material powder containing only metal component aluminum. The aluminum source powder may, for example, be a powder of aluminum oxide. Alumina may be crystalline or amorphous (amorphous). When the aluminum oxide is crystalline, the crystal system may be, for example, an r-type, a <5 type, a 0 type, or an α type. Preferably, an α-type alumina is used. The aluminum source powder used in the present invention is a powder of a substance which is introduced into alumina by firing in air. Examples of such a substance include an aluminum salt, an alkane alumina, aluminum hydroxide, aluminum, and the like. The aluminum salt may be an inorganic salt or an organic salt. Specific examples of the aluminum inorganic salt include a nitrate such as aluminum nitrate 'ammonium nitrate or the like; a carbonate such as ammonium aluminum carbonate. The aluminum organic salt may, for example, be aluminum oxalate, aluminum acetate, aluminum stearate, aluminum lactate or aluminum laurate. Further, specific examples of the alkane alumina include, for example, isopropyl alumina, acetonitrile, sec-butyl alumina, tert-butadiene alumina, and the like. 201041824 Hydrogen chloride can be crystalline or amorphous (amorphous). When the aluminum hydroxide is crystalline, the crystal form thereof may be, for example, a gibbsite type, a bayerite type, a Nordstrandite type, a boehmite type, or a pseudo soft boehmite (PSEUDO-BOEHMITE). Type and so on. Further, the amorphous aluminum hydroxide may, for example, be an aluminum hydrolyzate obtained by hydrolyzing an aqueous solution of a water-soluble aluminum compound such as an aluminum salt or an alkane alumina. Among the above, the aluminum source powder is preferably an alumina powder having an alumina powder and an aluminum hydroxide powder. The aluminum source powder may contain minor components that cannot be avoided during the manufacturing process. The particle diameter of the aluminum source powder is not particularly limited, but it is preferably measured by a laser diffraction method using a cumulative percentage of the volume basis of 50% of the equivalent particle diameter (D50) of 0.1 to 50 μm. From the viewpoint of efficiently producing aluminum magnesium titanate, the D50 of the aluminum source powder is preferably 0.3 to 30 μm. The titanium source powder contained in the raw material mixture is a material powder for a titanium component constituting the aluminum titanate-based fired body, and is referred to as a metal element-containing D titanium. Such a substance may, for example, be a powder of titanium oxide. The titanium oxide layer may, for example, be titanium oxide (IV), titanium oxide (III) or titanium oxide (II), and titanium oxide (IV) is preferably used. The titanium oxide (IV) may be crystalline or amorphous (amorphous). When the titanium oxide (IV) is crystalline, the crystalline form may, for example, be anatase, rutile or brookite, preferably anatase or rutile titanium oxide (IV). . The titanium source powder used in the present invention may be a substance powder into which titanium oxide is introduced by firing in air. Examples of such a substance include a titanium salt, a titanium alkoxide, a titanium hydroxide, titanium oxide, titanium sulfide, titanium, and the like. -9- 201041824
鈦鹽之具體例如，三氯化鈦、四氯化鈦、硫化鈦（IV )、硫化鈦（VI )、硫酸鈦（IV )等。烷氧化鈦之具體例 如，乙氧化鈦（IV)、甲氧化鈦（IV ) 、t-丁氧化鈦（IV )、異丁氧化鈦（IV ) 、η-丙氧化鈦（IV )、四異丙氧化 鈦（IV )及此等之螯合化合物等。 上述中鈦源粉末以使用氧化鈦粉末爲佳，更佳爲氧化 鈦（IV)粉末。又，鈦源粉末可含有製造過程中無可避免 含有之微量成份。又，鈦源粉末係亦可使用於該表面上被 塗佈氧化鋁、二氧化矽、氧化鍩、氫氧化鋁等形成之薄的 表面層者。又，鈦源粉末係亦可使用鈦酸鋁與鈦酸鋁鎂這 般鈦的複合氧化物。 鈦源粉末之粒徑並不特別地被限定，但是藉由雷射繞 射法被測定，可使用體積基準之累積百分比5 0%相當粒子 徑（D50 )爲0.1〜50μιη者爲佳。由有效率地使鈦酸鋁鎂 生成之觀點來看，鈦源粉末之D50係0.1〜30μιη更佳。 對於二氧化鈦[T i 〇 2 ]換算之鈦源粉末的使用量與氧化 鋁[Al2〇3]換算之鋁源粉末的使用量之合計量100質量份 而言，一般二氧化鈦換算之鈦源粉末的使用量爲30質量 份〜70質量份、氧化鋁換算之鋁源粉末的使用量爲70質 量份〜3 0質量份，較佳爲二氧化鈦換算之鈦源粉末的使 用量爲40質量份〜60質量份、氧化鋁換算之鋁源粉末的 使用量爲60質量份〜40質量份。 本發明中氧化鋁[Al2〇3]換算之鋁源粉末的質量XI係 可藉由下述式（A)被求得。 -10- 201041824 χ 1 = N 1 〇 XX 1 〇 . . · (A) 式（Α)中Νιο係表示Α12〇3之式量，χΐ0係表示氧化 鋁[αι2ο3]換算之鋁源粉末的莫耳量。氧化鋁[Al2〇3]換算 之鋁源粉末之莫耳量Mo係可藉由下述式（Α-1 )被求得 0 x10= (wixMi) / (Ntx2) · · · ( A -1 ) 式（A-1)中wi係表示鋁源粉末之使用量（g) > Μι 係表示鋁源粉末1莫耳中之鋁的莫耳數，N 1係表示已使 用之鋁源粉末之式量。使用本發明中2種以上之鋁源粉末 時，可藉由式（A-1 )求得各鋁源粉末之氧化鋁[Al2〇3]換 算之莫耳量，可藉由合計各莫耳量，求得使用之鋁源粉末 Q 的氧化鋁[Al2〇3]換算之莫耳量。 本發明中二氧化鈦[Ti〇2]換算之鈦源粉末的質量X2係 可藉由下述式（B)求得。 x2 = Ν2〇Χχ2〇 . · · ( Β) 式（Β )中Ν2〇係表示Ti〇2之式量、X2Q係表示二氧 化鈦[Ti02]換算之鈦源粉末的莫耳量。二氧化鈦[Ti02]換 算之鈦源粉末的莫耳量X20係可藉由下述式（B-1 )求得 -11 - 201041824 X2〇= (w2xM2) /N2 . · . (B-l) 式（B-l)中W2係表示鈦源粉末之使用量（g) 、M2 係表示鈦源粉末1莫耳中之鈦的莫耳數、N 2係表示已使 用之鈦源粉末的式量。使用本發明中2種以上之鈦源粉末 時，可藉由式（B-1 ) ’求得各鈦源粉末之二氧化欽 [Ti02]換算的莫耳量’可藉由合計各莫耳量’求得使用之 鈦源粉末的二氧化鈦[Ti〇2]換算之莫耳量。 接者，對於鎂源粉末進行說明。本發明使用之鎂源粉 末係含有1種以上之水滑石系化合物。於此’ 「水滑石系 化合物」係包含水滑石及水滑石類化合物。「水滑石」係 具有式：Mg6Al2(〇H) 16C03. 4H20(Mg、A1 係各自爲 2價、3價）表示之層狀的結晶構造之層狀雙氫氧化合物 。又，本發明中「水滑石類化合物」被定義爲含有2價之 Mg及3價之A1，具有與水滑石相同之層狀結晶構造的化 合物。藉由將這般的水滑石系化合物使用作爲鎂源，不使 用黏合劑、或是即使黏合劑之添加量少時，可得機械強度 高的鈦酸鋁系燒成體。又，可減低或省略黏合劑、特別是 有機黏合劑之使用量，故可減低給予燒成時之熱能的同時 ，可防止或抑制在燒成時之二酸化碳的產生及對燒成體中 灰分、碳分等之殘留。 水滑石類化合物比較容易取得，故可使用一般式· -12- 201041824Specific examples of the titanium salt include titanium trichloride, titanium tetrachloride, titanium (IV) sulfide, titanium (VI) sulfide, titanium (IV) sulfate, and the like. Specific examples of the titanium alkoxide include, for example, titanium oxide (IV), titanium oxide (IV), t-butyl titanium oxide (IV), titanium isobutoxide (IV), η-propylene titanium oxide (IV), tetraisopropyl Titanium oxide (IV) and such chelating compounds and the like. The above-mentioned medium titanium source powder is preferably a titanium oxide powder, more preferably a titanium oxide (IV) powder. Further, the titanium source powder may contain trace components which are inevitably contained in the manufacturing process. Further, the titanium source powder may be used for a thin surface layer formed of alumina, cerium oxide, cerium oxide, aluminum hydroxide or the like coated on the surface. Further, as the titanium source powder, a composite oxide of titanium such as aluminum titanate and aluminum magnesium titanate may be used. The particle diameter of the titanium source powder is not particularly limited, but it is preferably measured by a laser diffraction method using a cumulative percentage of the volume basis of 50% of the equivalent particle diameter (D50) of 0.1 to 50 μm. From the viewpoint of efficiently producing magnesium aluminum titanate, the D50 of the titanium source powder is more preferably 0.1 to 30 μm. For the total amount of the titanium source powder in terms of titanium dioxide [T i 〇 2 ] and the amount of the aluminum source powder in terms of alumina [Al 2 〇 3], 100 parts by mass of the total amount of the titanium source powder in terms of titanium dioxide is used. The amount of use of the aluminum source powder in terms of alumina is 70 parts by mass to 30 parts by mass, and the amount of the titanium source powder in terms of titanium dioxide is preferably 40 parts by mass to 60 parts by mass, based on 30 parts by mass to 70 parts by mass. The amount of the aluminum source powder in terms of alumina is 60 parts by mass to 40 parts by mass. In the present invention, the mass XI of the aluminum source powder in terms of alumina [Al2〇3] can be obtained by the following formula (A). -10- 201041824 χ 1 = N 1 〇 XX 1 〇. . · (A) In the formula (Α), Νιο represents the amount of Α12〇3, and χΐ0 represents the mole of aluminum source powder in the conversion of alumina [αι2ο3] the amount. The Mo content of the aluminum source powder in terms of alumina [Al2〇3] can be obtained by the following formula (Α-1): 0 x 10 = (wixMi) / (Ntx2) · · · ( A -1 ) In the formula (A-1), the wi system represents the amount of the aluminum source powder used (g) > Μι represents the molar number of aluminum in the aluminum source powder 1 mol, and the N 1 system represents the type of the aluminum source powder used. the amount. When two or more kinds of aluminum source powders of the present invention are used, the amount of moles in terms of alumina [Al2〇3] of each aluminum source powder can be determined by the formula (A-1), and the total amount of each mole can be obtained by adding The amount of moles in terms of alumina [Al2〇3] of the aluminum source powder Q used was determined. In the present invention, the mass X2 of the titanium source powder in terms of titanium dioxide [Ti〇2] can be obtained by the following formula (B). X2 = Ν2〇Χχ2〇 . · · ( Β ) In the formula (Β ), the Ν 2 〇 represents the formula of Ti 〇 2 , and the X 2 Q represents the molar amount of the titanium source powder in terms of titanium dioxide [Ti02]. The molar amount X20 of the titanium source powder in terms of titanium dioxide [Ti02] can be obtained by the following formula (B-1): -11 - 201041824 X2 〇 = (w2xM2) / N2 . . . (Bl) Formula (Bl) The middle W2 system represents the amount (g) of the titanium source powder used, the M2 system represents the molar number of titanium in the titanium source powder 1 mol, and the N 2 system represents the formula amount of the used titanium source powder. When two or more kinds of titanium source powders in the present invention are used, the amount of moles in the amount of dioxins [Ti02] of each titanium source powder can be obtained by the formula (B-1)' by summing the amounts of each mole. 'The amount of moles of titanium dioxide [Ti〇2] converted from the titanium source powder used. Next, the magnesium source powder will be described. The magnesium source powder used in the present invention contains one or more hydrotalcite-based compounds. Here, the "hydrotalcite compound" includes hydrotalcite and hydrotalcite compounds. The "hydrotalcite" is a layered double hydroxide of a layered crystal structure represented by the formula: Mg6Al2(〇H) 16C03. 4H20 (Mg and A1 are each a divalent or trivalent). In the present invention, the "hydrotalcite compound" is defined as a compound having a layered crystal structure similar to hydrotalcite, which contains divalent Mg and trivalent A1. When such a hydrotalcite-based compound is used as a magnesium source, an aluminum titanate-based fired body having high mechanical strength can be obtained without using a binder or even if the amount of the binder added is small. Further, since the amount of the binder, particularly the organic binder, can be reduced or omitted, the heat energy during firing can be reduced, and the generation of diacidified carbon during firing and the ash in the fired body can be prevented or suppressed. , carbon residue, etc. Hydrotalcite compounds are relatively easy to obtain, so general formula can be used. -12- 201041824
MgxAly ( OH ) ZC03 · WH20表示之化合物爲佳。於此，在 上述一般式中X爲3〜7左右、y爲1〜3左右、z爲10〜 18左右、w爲2〜6左右。上述一般式表不之水滑石類化 合物係可舉例如協和化學工業（股）製之「DHT-4A」（ Mg4.5Al2 ( OH) 13CO3 · 3.5H20) 、「DHT-6」（Mg6Al2 (OH ) 16C03 · 4H20 )等。 鎂源粉末係可僅由水滑石系化合物組成、或可爲水滑 0 石系化合物與水滑石系化合物以外之鎂源的混合物。然而 ，欲極力削減黏合劑之使用量（較佳爲0 )，鎂源粉末中 水滑石系化合物的含有率儘可能多爲佳，鎂源粉末僅由水 滑石系化合物形成爲更佳。合倂使用水滑石系化合物以外 之鎂源時’該含有率係以鎂源粉末中氧化鎂（M gO )換算 ’可例如爲40質量％以下。水滑石系化合物以外之鎂源 的含有率係以氧化鎂（Mg0 )換算爲30質量％以下爲佳 ’較佳以氧化鎂（MgO )換算爲20質量％以下，更佳爲 〇 以氧化鎂（MgO )換算爲1 0質量％以下，最佳以氧化鎂 (M g Ο )換算爲5質量％以下。 本發明中氧化鎂[MgO]換算之鎂源粉末的質量X3係可 藉由下述式（C)求得。 X3 = Ν3〇χχ3〇 . . · ( C ) 式（C)中N3()係表示MgO之式量，X3Q係表示氧化 鎂[MgO]換算之鎂源粉末的莫耳量。氧化鎂[Mg〇]換算之 -13- 201041824 鎂源粉末的莫耳量Χ3〇係可藉由下述式（C-l )求得。 x3〇 = ( W3XM3 ) /N3 . · . ( C -1 ) 式（C-1 )中w3係表示鎂源粉末之使用量（g) ，m3 係表示鎂源粉末1莫耳中之鎂的莫耳數，N3係表示已使 用之鎂源粉末的式量。使用本發明中2種以上之鎂源粉末 時，可藉由式（C-1)求得各鎂源粉末之氧化鎂[Mg〇]換 算之莫耳量’可藉由合計各莫耳量，求得使用之鎂源粉末 的氧化鎂[MgO]換算之莫耳量。 水滑石系化合物以外之鎂源係可舉例如氧化鎂之粉末 之外，可藉由於大氣中進行燒成而導入氧化鎂之物質的粉 末。後者之例子係可舉例如鎂鹽、烷氧化鎂、氫氧化鎂、 氧化鎂、鎂等。 鎂鹽之具體例如，氯化鎂、高氮酸鎂、磷酸鎂、焦磷 酸鎂、草酸鎂、硝酸鎂、碳酸鎂、乙酸鎂、硫酸鎂、檸檬 酸、乳酸鎂、硬脂酸鎂、水楊酸鎂、肉豆蔻酸鎂、葡糖酸 鎂、二甲基丙烯酸鎂、苯甲酸鎂。 烷氧化鎂之具體例如，甲氧化鎂、乙氧化鎂等。又， 鎂源粉末可含有製造過程中無可避免含有之微量成份。 又，水滑石系化合物以外之鎂源係亦可使用兼具鎂源 與鋁源之化合物的粉末。這般化合物係可舉例如尖晶石（ MgAl204 )與鈦酸鋁鎂。水滑石系化合物以外之鎂源粉末 係可使用僅1種或合倂使用2種以上。 -14- 201041824 鎂源粉末（水滑石系化合物粉末及水滑石系化合物以 外之鎂源粉末）之粒徑係並不特別被限定，但是可藉由雷 射繞射法被測定，可使用體積基準之累積百分比5 0 %相當 粒子徑（D5〇)爲〇·1〜ΙΟμιη爲佳。由有效率地生成鈦酸 鋁鎂之觀點看來，鎂源粉末之D50係〇.1〜2. Ομχη爲更佳 〇 在原料混合物中鎂〔Mg〇〕換算之鎂源粉末的含量相 ❹ 係對於二氧化鈦〔Ti〇2〕換算之鈦源粉末的使用量與氧化 鋁〔Al2〇3〕換算之鋁源粉末之使用量的合計量100質量 份而言，0.1〜15質量份爲佳，更佳爲0.1〜10質量份。 上述原料混合物可尙含有矽源粉末。矽源粉末係，鈦 酸鋁系燒成體所含的矽成份之物質粉末，合倂使用矽源粉 末時可進一步求得提升耐熱分解性之鈦酸鋁系燒成體。矽 源粉末係可舉例如二氧化矽、一氧化矽等氧化矽（二氧化 矽）粉末。 〇 又，矽源粉末係可藉由於空氣中燒成而導入二氧化矽 之物質粉末。如此之物質係可舉例如，含有矽酸、碳化矽 、氧化矽、硫化矽、四氯化矽、乙酸矽、矽酸鈉、原矽酸 鈉、長石、矽及鋁之複合氧化物、玻璃料等。其中，由工 業上容易取得觀點看來，使用長石、玻璃料等爲佳，就工 業上容易取得、組成安定性之點，更佳爲使用玻璃料等。 又玻璃料係將玻璃粉碎而得之片狀或粉末狀玻璃。 使用作爲矽源粉末之玻璃料時，就進一步提升所得的 鈦酸鋁矽燒成體之耐熱分解性觀點，以使用屈伏點爲700 -15- 201041824 °c以上之物爲佳。本發明之玻璃料的屈伏點係被定義爲可 使用熱機械分析裝置 （TMA : Thermo Mechanical Analysis )測定，玻璃料之屈伏點以玻璃料升溫過程中， 停止膨脹後開始收縮之溫度（°C )。 構成上述玻璃料之玻璃可爲，主成份爲矽酸[Si02]( 全成份中超過5 0質量％ )之一般的矽酸玻璃。構成玻璃 料之玻璃係含有其他之含有成份，可含有同一般矽酸玻璃 之氧化鋁[A1203 ]、氧化鈉[Na20]、氧化鉀[K20]、氧化鈣 [CaO]、氧化鎂[MgO]等。又，構成玻璃料之玻璃爲了提 升玻璃本身的耐熱水性，可含有Zr02。 矽源粉末之粒徑並無特別限定，可藉由雷射繞射法測 定，體積基準之累積百分比50%相當粒徑（D50 )爲1〜 20μιη爲佳。由有效地生成鈦酸鋁鎂之觀點看來，矽源粉 末之D50係5〜20μιη爲更佳。 原料混合物含有矽源粉末時，在原料混合物中Si〇2 (二氧化矽）換算之矽源粉末之含量係相對於Al2〇3 (二 氧化鋁）換算之鋁源粉末及Ti02 (氧化鈦）換算之鈦源 粉末之合計値100質量份而言’一般爲0.1質量份〜10質 量份，5質量份以下爲佳。又’矽源粉末可含有製造過程 中無可避免含有的微量成份。 本發明中二氧化矽[Si〇2]換算之矽源粉末之質量X4係 可藉由下述式（D)求得。 ••(D) X4 = N4〇XX40 -16- 201041824 式（D)中N4q係表示Si〇2之式量，Χ4◦係表示二氧 化矽[Si02]換算之矽源粉末的莫耳量。二氧化矽[Si02]換 算之矽源粉末的莫耳量X4 0係可藉由下述式（D-1)求得 x4〇= ( w4xM4) / N4 · . . ( D-1 ) 式（D-1)中W4係表示矽源粉末之使用量（g) 、M4 係表示矽源粉末1莫耳中之矽的莫耳數，N4係表示已使 用之矽源粉末的式量。使用本發明中2種以上之矽源粉末 時’可藉由式（D-1 )求得各矽源粉末之二氧化矽[si〇2] 換算之莫耳量，可藉由合計各莫耳量，求得使用之矽源粉 末的二氧化矽[Si02]換算之莫耳量。The compound represented by MgxAly ( OH ) ZC03 · WH20 is preferred. Here, in the above general formula, X is about 3 to 7, y is about 1 to 3, z is about 10 to 18, and w is about 2 to 6. The hydrotalcite-based compound of the above-mentioned general formula is, for example, "DHT-4A" (Mg4.5Al2 (OH) 13CO3 · 3.5H20) and "DHT-6" (Mg6Al2 (OH)) manufactured by Kyowa Chemical Industry Co., Ltd. 16C03 · 4H20) and so on. The magnesium source powder may be composed only of a hydrotalcite-based compound or may be a mixture of a water-slip 0 stone compound and a magnesium source other than the hydrotalcite-based compound. However, in order to reduce the amount of the binder (preferably 0), the content of the hydrotalcite-based compound in the magnesium source powder is preferably as high as possible, and the magnesium source powder is preferably formed only from the hydrotalcite-based compound. When the magnesium source other than the hydrotalcite-based compound is used in combination, the content ratio is, for example, 40% by mass or less based on the magnesium oxide (M gO ) in the magnesium source powder. The content of the magnesium source other than the hydrotalcite-based compound is preferably 30% by mass or less in terms of magnesium oxide (Mg0), preferably 20% by mass or less in terms of magnesium oxide (MgO), and more preferably magnesium oxide (〇). The content of MgO is 10% by mass or less, and is preferably 5% by mass or less in terms of magnesium oxide (M g Ο ). In the present invention, the mass X3 of the magnesium source powder in terms of magnesium oxide [MgO] can be obtained by the following formula (C). X3 = Ν3〇χχ3〇 . . . (C) In the formula (C), N3() represents the formula of MgO, and X3Q represents the molar amount of the magnesium source powder in terms of magnesium oxide [MgO]. Magnesium oxide [Mg〇] conversion -13- 201041824 The molar amount of the magnesium source powder can be determined by the following formula (C-1). X3〇=( W3XM3 ) /N3 . ( C -1 ) In the formula (C-1 ), w3 represents the amount of magnesium source powder used (g), and m3 represents magnesium in the magnesium source powder. The number of ears, N3, represents the formula of the magnesium source powder that has been used. When two or more types of magnesium source powders in the present invention are used, the amount of magnesium oxide in terms of magnesium oxide [Mg〇] of each of the magnesium source powders can be determined by the formula (C-1) by summing the amount of each mole. The amount of magnesium oxide in terms of magnesium oxide [MgO] of the magnesium source powder used was determined. The magnesium source other than the hydrotalcite-based compound may be, for example, a powder of magnesium oxide, which may be introduced into the atmosphere by firing in the atmosphere. Examples of the latter include magnesium salts, magnesium alkoxides, magnesium hydroxide, magnesium oxide, magnesium, and the like. Specific examples of the magnesium salt are, for example, magnesium chloride, magnesium permanganate, magnesium phosphate, magnesium pyrophosphate, magnesium oxalate, magnesium nitrate, magnesium carbonate, magnesium acetate, magnesium sulfate, citric acid, magnesium lactate, magnesium stearate, magnesium salicylate. , magnesium myristate, magnesium gluconate, magnesium dimethacrylate, magnesium benzoate. Specific examples of the magnesium alkoxide are, for example, magnesium oxide, magnesium oxide and the like. Further, the magnesium source powder may contain trace components which are inevitably contained in the manufacturing process. Further, as the magnesium source other than the hydrotalcite-based compound, a powder having a compound of a magnesium source and an aluminum source can also be used. Examples of such a compound include spinel (MgAl204) and aluminum magnesium titanate. The magnesium source powder other than the hydrotalcite-based compound may be used alone or in combination of two or more. -14- 201041824 The particle size of the magnesium source powder (the hydrotalcite-based compound powder and the magnesium source powder other than the hydrotalcite-based compound) is not particularly limited, but can be measured by a laser diffraction method, and a volume standard can be used. The cumulative percentage of 50% is equivalent to the particle diameter (D5〇) of 〇·1~ΙΟμιη. From the viewpoint of efficiently producing aluminum magnesium titanate, the D50 of the magnesium source powder is 〇.1~2. Ομχη is more preferable. The content of the magnesium source powder in terms of magnesium [Mg〇] in the raw material mixture is 0.1 to 15 parts by mass, more preferably 100 parts by mass of the total amount of the titanium source powder in terms of titanium oxide [Ti〇2] and the amount of the aluminum source powder in terms of alumina [Al2〇3]. It is 0.1 to 10 parts by mass. The above raw material mixture may contain a cerium source powder. The material powder of the bismuth component contained in the bismuth powder type or the aluminum titanate-based fired body can be further obtained by further improving the thermal decomposition resistance of the aluminum titanate-based fired body. The cerium source powder may, for example, be cerium oxide (cerium oxide) powder such as cerium oxide or cerium oxide. Further, the ruthenium source powder is a substance powder which is introduced into the cerium oxide by firing in the air. Such a substance may, for example, be a composite oxide containing citric acid, lanthanum carbide, cerium oxide, cerium sulfide, cerium tetrachloride, cerium acetate, sodium citrate, sodium decanoate, feldspar, lanthanum and aluminum, and glass frit. Wait. Among them, it is better to use feldspar and glass frit, and it is easy to obtain industrially and form stability, and it is more preferable to use glass frit. Further, the glass frit is a sheet-like or powdery glass obtained by pulverizing glass. When a glass frit is used as the source of the powder, the viewpoint of heat decomposition resistance of the obtained aluminum barium strontium sulphide fired body is further improved, and it is preferable to use a material having a yield point of 700 -15 to 201041824 ° C or more. The yield point of the glass frit of the present invention is defined as a temperature (°C) which can be measured by a thermomechanical analysis device (TMA: Thermo Mechanical Analysis), where the yield point of the frit is increased during the temperature rise of the glass frit and the expansion is stopped. . The glass constituting the above glass frit may be a general tannic acid glass whose main component is citric acid [SiO 2 ] (more than 50% by mass in the total composition). The glass constituting the glass frit contains other components, and may contain alumina [A1203], sodium oxide [Na20], potassium oxide [K20], calcium oxide [CaO], magnesium oxide [MgO], etc., which are similar to general citrate glass. . Further, the glass constituting the glass frit may contain ZrO 2 in order to improve the hot water resistance of the glass itself. The particle diameter of the ruthenium source powder is not particularly limited and can be determined by a laser diffraction method, and the cumulative percentage of the volume basis is 50%, and the particle diameter (D50) is preferably 1 to 20 μm. From the viewpoint of efficiently producing aluminum magnesium titanate, the D50 of the Wuyuan powder is preferably 5 to 20 μm. When the raw material mixture contains the cerium source powder, the content of the cerium source powder in terms of Si 〇 2 (cerium oxide) in the raw material mixture is converted to the aluminum source powder and Ti02 (titanium oxide) in terms of Al 2 〇 3 (dia alumina). The total amount of the titanium source powder is generally 0.1 parts by mass to 10 parts by mass, and preferably 5 parts by mass or less, based on 100 parts by mass. Moreover, the Wuyuan powder can contain trace elements that are inevitably contained in the manufacturing process. The mass X4 of the cerium source powder in terms of cerium oxide [Si〇2] in the present invention can be obtained by the following formula (D). ••(D) X4 = N4〇XX40 -16- 201041824 In the formula (D), N4q represents the formula of Si〇2, and Χ4◦ represents the molar amount of the tantalum powder in terms of cerium dioxide [Si02]. The molar amount X4 0 of the cerium oxide [Si02]-derived cerium source powder can be obtained by the following formula (D-1): x4 〇 = ( w4 x M 4 ) / N 4 · ( D-1 ) -1) Medium W4 indicates the amount of use of the source powder (g), M4 indicates the number of moles of the ruthenium powder in the source, and N4 indicates the formula of the used source powder. When two or more kinds of cerium source powders of the present invention are used, the molar amount of cerium oxide [si〇2] in each of the cerium source powders can be determined by the formula (D-1), and the molar amount can be obtained by adding each mole. The amount of the cerium oxide [Si02] in terms of the amount of the cerium source powder used was determined.
又’本發明中上述氧化鎂尖晶石（MgAl2〇4 )、欽酸 銘、欽酸銘錶等之複合氧化合物，可以欽、鋁、錶及丨夕中 2種以上之金屬元素爲成份之化合物作爲原料粉末用。推 斷此時之使用這般化合物可與混合各金屬源粉末者相同。 基於該推斷係將原料混合物中鋁源粉末、欽'源粉末、錶源 粉末及矽粉末之含量調整爲上述範圍內。 上述原料混合物係可藉由混合例如鈦源粉末、錦源粉 。混合時，可使 ' Loedige mixer 空氣混合機；球 末、鎂源粉末及任意使用之砂源粉末求得^ 用一般使用之混合機，例如諾塔混合；f幾 混合機等之攪拌混合機；快速混合機等之 -17- 201041824 磨機、振動磨等。混合方法係可爲乾式混合、濕式混合中 任一種。 實行乾式混合時’例如混合鈦源粉末、鋁源粉末、鎂 源粉末及任意被使用之矽源粉末，使其分散於液體介質中 ，於粉碎容器內攪拌，即可一般於粉碎介質之共存下於粉 碎容器內進行攪拌。 一般粉碎容器係可使用被不鏽鋼等之金屬材料構成者 ’內表面可被氟樹脂、矽樹脂、胺基甲酸乙酯樹脂等塗佈 。粉碎容器之內容積係對於原料粉末（鈦源粉末、鋁源粉 末、鎂源粉末及任意使用之矽源粉末）及粉碎介質之合計 容積而言，一般爲1容量倍〜4容量倍、1.2容量倍〜3容 量倍爲佳。 粉碎介質係可舉例如粒子徑 1mm〜1 00mm、5mm〜 5 0mm之氧化鋁珠、氧化鉻珠等爲佳。粉碎介質之使用量 係對於原料粉末之合計使用量而言，一般爲1質量倍〜 1 00 0質量倍' 5質量倍〜100質量倍爲佳。 廪料粉末之混合-粉碎係例如於粉碎容器內，投入上 述原料粉末及粉碎介質後，可使粉碎容器振動，使其回轉 或是藉由該兩者進行。藉由使粉碎容器振動或回轉，使原 料粉末與粉碎介質同時地攪拌混合，同時粉碎。欲使粉碎 容器振動或回轉，可使用例如振動磨、球磨機、行星式球 磨機（等這般一般之粉碎機，以工業上規模之容易實施的 點’可使用振動磨爲佳。使粉碎容器振動時，該振幅一般 爲2mm〜20mm，12mm以下爲佳。混合-粉碎係可以連續 -18 - 201041824 式進行或間歇式進行’但是就工業上規模之容易實施的點 ，以連續式進行爲佳。混合-粉碎需要之時間，—般爲1 分〜6小時、1 . 5分〜2小時爲佳。 將原料粉末以乾式進行混合及粉碎時，可加入助磨劑 、解膠劑等之添加劑。助磨劑係可舉例如單元醇類（甲醇 、乙醇、丙醇等）、二元醇類（丙二醇、聚丙二醇、乙二 醇等）等之醇類；三乙醇胺等之胺類；棕櫚酸、硬脂酸、 0 油酸等之高級脂肪酸類；碳黑、石墨等之碳材料等。此等 係可各自單獨或組合2種以上使用。 使用添加劑時，該合計使用量係原料粉末之合計使用 量’即’對於鈦源粉末、鋁源粉末、鎂源粉末及矽源粉末 之合計使用量100質量份而言，一般爲0.1〜10質量份、 0.5〜5質量份爲佳、更佳爲0.75〜2質量份。 另一方面，以濕式進行混合時，使例如鈦源粉末、鋁 源粉末、鎂源粉末及任意使用之矽源粉末分散於溶劑中之 Q 狀態混合即可。混合方法係可於液體介質中之攪拌處理或 於粉碎介質之共存下於粉碎容器內攪拌。粉碎介質及粉碎 容器、及粉碎機係可使用上述者。於粉碎介質之共存下， 與粉碎容器內進行混合-粉碎時、乾式混合時相同，可合 倂使用助磨劑等之添加劑。 上述溶劑係可使用例如單元醇類（甲醇、乙醇、丙醇 、丁醇等）、二元醇類（丙二醇、聚丙二醇、乙二醇等） 等之醇類；及水等。其中，可使用水爲佳，就雜質少之點 ’使用離子交換水爲更佳。溶劑之使用量係對於鈦源粉末 -19- 201041824 、鋁源粉末、鎂源粉末及矽源粉末之合計量100質量份而 言，一般爲20質量份〜1000質量份，30質量份〜300質 量份爲佳。 以濕式進行混合時，於溶劑中可添加分散劑。分散劑 係可舉例如硝酸、鹽酸、硫酸等之無機酸；草酸、檸檬酸 、乙酸、蘋果酸、乳酸等之有機酸；甲醇、乙醇、丙醇等 之醇類；多元羧酸銨等之界面活性劑等。使用分散劑時， 該使用量係溶劑每100質量份，一般爲0.1質量份〜20質 量份，0.2質量份〜1 0質量份爲佳。 在濕式混合時，可藉由混合後，除去溶劑，求得原料 混合物。溶劑之除去，一般可藉由餾去溶劑實施。餾去溶 劑之方法係並不特別限制，可以室溫風乾、真空乾燥或加 熱乾燥。乾燥方法係可靜置乾燥或流動乾燥。進行加熱乾 燥時之溫度係並不特別限制，但是一般爲50°C以上25 0°C 以下。可使用於加熱乾燥之機器係可舉例如盤式乾燥器、 泥漿乾燥器（slurry dryer )、噴霧乾燥器等。 又，以濕式進行混合時，亦依據使用之銘源粉末的種 類，溶解於溶劑，但是溶解於溶劑之鋁源粉末等係藉由溶 劑餾去，再進行析出爲固形分。 本發明中，將含有上述鋁源粉末、鈦源粉末、鎂源粉 末及任意使用之矽源粉末的原料混合物成形得到成形體後 ，藉由進行燒成該成形體，求得鈦酸鋁系燒成體。成形後 藉由進行燒成，相較於直接燒成原料混合物時，由抑制燒 成中之收縮，可有效果地抑制所得之鈦酸鋁系燒成體之破 -20- 201041824 裂’又’可得藉由燒成而生成之多孔質性的鈦酸鋁結晶之 細孔形狀被維持之鈦酸鋁系燒成體。成形體之形狀並不特 別限制’但是可舉例如蜂窩形狀、棒狀、管狀、板狀、坩 堝形狀等。 使用於原料混合物之成形之成形機係可舉單軸壓製機 (uniaxial press molding)、擠壓機、打錠機、造粒機等 。實行擠壓成形時’於原料混合物中，可添加例如孔洞成 0 形劑、潤滑劑及可塑劑、分散劑、及溶劑等之添加劑進行 成形。又’實施擠壓成形時，於原料混合物中可添加黏合 劑，但於本發明中即使不添加黏合劑、或黏合劑之添加量 稍少時，可製作具有良好的機械特性之鈦酸鋁系燒成體。 又’依據物質而有兼具孔洞成形劑與黏合劑之兩者的角色 。這般物質’可於成形時黏接粒子彼此使成形體維持成形 ，之後之燒成時，可使其本身燃燒形成空孔，具體而言之 ，可爲聚乙烯等。 〇 上述孔洞成形劑係可舉例如石墨等之碳材；聚乙烯、 聚丙烯、聚甲基丙烯酸甲脂等之樹脂類；澱粉、堅果殼、 核桃殻、玉米等之植物系材料；冰；及乾冰等。孔洞形成 劑之添加量係對於鋁源粉末、鈦源粉末、鎂源粉末及矽源 粉末之合計量100質量份而言，一般爲〇〜40質量份，0 〜2 5質量份爲佳。 上述潤滑劑及可塑劑係可舉例如，甘油等醇類：癸酸 、月桂酸、棕櫚酸、花生酸、油酸、硬脂酸等之高級脂肪 酸；硬脂酸鋁等之硬脂酸金屬鹽等。潤滑劑及可塑劑之添 -21 - 201041824 加量相對於鋁源粉末、鈦源粉未、鎂源粉末及矽源粉末之 合計量100質量份而言，一般爲〇〜1〇質量份，1〜5質 量份爲佳。 上述分散劑係可舉例如，硝酸、鹽酸、硫酸等無機酸 ;草酸、檸檬酸、乙酸、蘋果酸、乳酸等之有機酸；甲醇 、乙醇、丙醇等之醇類；聚羧酸錶、聚氧化烯烴烷醚等之 界面活性劑等。分散劑之添加量係相對於鋁源粉末、鈦源 粉末、鎂源粉末及矽源粉末之合計量100質量份而言，一 般爲0〜20質量份，2〜8質量份爲佳。 又，上述溶劑可使用例如單醇類（甲醇、乙醇、丁醇 、丙醇等）、二元醇類（丙二醇、聚丙二醇、乙二醇等） 等之醇類；及水等。其中，水爲佳，就不純物較少之觀點 ，更佳爲使用離子交換水。溶劑之使用量相對於鋁源粉末 、鈦源粉末、鎂源粉末及矽源粉末之合計量1 00質量份而 言，一般爲10〜100質量份，20〜80質量份爲佳。 上述黏合劑係可舉例如甲基纖維素、羧基甲基纖維素 、鈉羧基甲基纖維素等之纖維素類；聚乙烯醇等之醇類； 木質磺酸鹽等之鹽；石蠟、微晶蠟之蠟；EVA、聚乙烯、 聚苯乙烯、液晶聚合物、工程塑膠等之熱可塑性樹脂等。 黏合劑之添加量係對於鋁源粉末、鈦源粉末、鎂源粉末及 砍源粉末之合計量100質量份而言，0.3質量份以下爲佳 。添加黏合劑時，黏合劑係藉由被燒成爲C02與H20之 氣體成份散佈於燒成體之外，但是黏合劑被燒成、除去之 後，具有存在空隙、給予燒成體之機械強度不良影響。由 -22- 201041824 此等之觀點，不添加黏合劑爲更佳。 在燒成成形體之燒成溫度，一般爲1300 °C以上， l4〇0°C以上爲佳。又，將被生成之鈦酸鋁系燒成體爲容易 進行加工者，故燒成溫度一般爲1650 °C以下，1600 °C以 下爲佳，更佳爲1 550°C以下。到達燒成溫度之升溫速度 並無特別限定，但是一般爲2°C/小時至500°C/小時。使 用矽源粉末時，燒成步驟前較佳爲設有11 00〜1300 °C之 0 溫度範圍內保持3小時以上的步驟。該步驟可促進矽源粉 末熔化及擴散。原料混合物含有黏合劑等時，燒成過程中 係包含去除該物用之脫脂步驟。典型的脫脂係到達燒成溫 度之升溫階段（例如1 5〇〜400 °c的範圍）進行。脫脂步 驟較佳爲極力抑制升溫速度。 燒成一般係於大氣中進行，但是可依所使用的原料粉 末（即鋁源粉末、鈦源粉末、鎂源粉末及矽源粉末）之種 類及使用量比，可於氮氣、氬氣等不活性氣體中燒成，或 Q 可於一氧化碳氣體、氫氣等還原性氣體中燒成。又，可於 降低水蒸氣分壓之環境中進行燒成。 燒成一般係使用管狀電爐、箱型電爐、隧道爐、遠紅 外線爐、微波加熱爐、軸爐、反射爐、回轉爐、滾筒室爐 等一般燒成爐進行。燒成可以分批式進行，或以連續式進 行。又，可以靜置式進行，或以流動式進行。 燒成所需要的時間可爲’原物料混合物之成形體能充 分遷移至鈦酸鋁鎂結晶之時間，即可依據原料混合物量， 燒成爐之形式、燒成溫度、燒成環境等而異，但是一般爲 -23- 201041824 1 0分〜7 2小時。 由上述可得之鈦酸鋁系燒成體。該鈦酸酸鋁系 具有幾乎可維持成形後成形體之形狀的形狀。所得 鋁系燒成物可藉由硏削加工等，亦可加工爲所希望 〇 由本發明之方法而得的鈦酸鋁系燒成體於X 光譜中，除了鈦酸鋁鎂之結晶圖型外，可含有二氧 氧化鋁、二氧化鈦等之結晶圖型。本發明之鈦酸鋁 體係可以組成式：Al2(i-x)MgxTi(1+x)05表示。X 0.01以上，〇.〇1以上0.7以下爲佳，更佳爲〇·〇2 t 以下。 【實施方式】 [實施例] 以下，將本發明藉由實施例更詳細說明本發明 發明非限定於此等。又’所得到之鈦酸鋁系燒成體 鋁化率（AT化率）、三點彎曲強度及所使用原料 粒度分布係以下述方法測定。 (1 ) AT化率 鈦酸鋁化率（AT化率）係，由粉末X射線繞 中出現於2 0 = 27.4°位置之峰〔歸屬於二氧化鈦― 相（1 1 0 )面〕的積分強度（It )，與出現於2 0 位置之峰〔歸屬於纟太酸銘鎂相（230 )面〕的積分 燒成體 的鈦酸 之形狀 線繞射 化砂、 系燒成 之値爲 〔上 0.5 ，但本 之鈦酸 粉末之 射光譜 金紅石 =33.7' 強度（ -24- 201041824Further, in the present invention, the composite oxygen compound such as the above-mentioned magnesia spinel (MgAl2〇4), chin acid, and cinnamic acid can be composed of two or more metal elements of the group, the aluminum, the watch, and the enamel. The compound is used as a raw material powder. It is inferred that the use of such a compound at this time can be the same as that of mixing the respective metal source powders. Based on this estimation, the content of the aluminum source powder, the Qin's source powder, the surface source powder, and the cerium powder in the raw material mixture was adjusted to the above range. The above raw material mixture can be mixed by, for example, a titanium source powder or a brocade powder. When mixing, the 'Loedige mixer air mixer; the ball end, the magnesium source powder and the sand source powder of any use can be obtained by using a commonly used mixer, such as a mixture of Nota mixing; a mixer such as a few mixers; Fast mixers, etc. -17- 201041824 Mills, vibratory mills, etc. The mixing method may be either dry mixing or wet mixing. When dry mixing is carried out, for example, a titanium source powder, an aluminum source powder, a magnesium source powder, and any used source powder are dispersed in a liquid medium and stirred in a pulverization container, generally in the coexistence of a pulverization medium. Stirring was carried out in a pulverization container. In general, the pulverization container can be formed of a metal material such as stainless steel. The inner surface can be coated with a fluororesin, an anthracene resin, a urethane resin or the like. The internal volume of the pulverization container is generally 1 capacity doubling to 4 capacity doubling and 1.2 capacity for the total volume of the raw material powder (titanium source powder, aluminum source powder, magnesium source powder, and arbitrarily used cerium source powder) and the pulverizing medium. Double ~ 3 capacity times is better. The pulverization medium may preferably be, for example, alumina beads having a particle diameter of 1 mm to 1 00 mm and 5 mm to 50 mm, or chrome oxide beads. The amount of the pulverization medium to be used is generally 1 mass% to 100 00 mass times '5 mass times to 100 mass times. The mixing and pulverization of the dip powder is carried out, for example, in a pulverization container, and after the raw material powder and the pulverization medium are introduced, the pulverization container can be vibrated to be rotated or both. The raw material powder and the pulverizing medium are simultaneously stirred and mixed while being pulverized by vibrating or rotating the pulverizing container. In order to vibrate or rotate the pulverizing container, it is preferable to use a vibrating mill such as a vibration mill, a ball mill, a planetary ball mill (such as a general pulverizer, which is easy to implement at an industrial scale). When the pulverizing container is vibrated The amplitude is generally 2 mm to 20 mm, preferably 12 mm or less. The mixing-pulverizing system can be carried out continuously or intermittently in the form of -18 - 201041824 'but it is preferably carried out in a continuous manner at a point where industrial scale is easy to carry out. - The time required for the pulverization is generally 1 minute to 6 hours, and 1.5 minutes to 2 hours. When the raw material powder is mixed and pulverized in a dry manner, an additive such as a grinding aid or a debonding agent may be added. Examples of the grinding agent include alcohols such as a unit alcohol (methanol, ethanol, propanol, etc.), glycols (propylene glycol, polypropylene glycol, ethylene glycol, etc.); amines such as triethanolamine; palmitic acid and hard Higher fatty acids such as fatty acid, oleic acid, and the like; carbon materials such as carbon black and graphite, etc. These may be used alone or in combination of two or more. When the additive is used, the total amount used is the total of the raw material powders. The amount of the 'that is' is generally 0.1 to 10 parts by mass, preferably 0.5 to 5 parts by mass, more preferably 0.75, based on 100 parts by mass of the total amount of the titanium source powder, the aluminum source powder, the magnesium source powder, and the lanthanum powder. On the other hand, when mixing is carried out in a wet manner, for example, a titanium source powder, an aluminum source powder, a magnesium source powder, and a ruthenium powder of any use may be mixed in a solvent in a Q state. The mixture may be stirred in a liquid medium or stirred in a pulverization container in the presence of a pulverization medium. The pulverization medium, the pulverization container, and the pulverizer may be used in the same manner as in the pulverization medium, and mixed with the pulverization container - In the case of pulverization or dry mixing, an additive such as a grinding aid may be used in combination. Examples of the solvent include unit alcohols (methanol, ethanol, propanol, butanol, etc.) and glycols (propylene glycol, polypropylene glycol). Alcohols such as ethylene glycol, etc.; and water, etc. Among them, water can be used, and it is preferable to use ion-exchanged water with less impurities. The amount of solvent used is for titanium source powder-19-2010 41824, 100 parts by mass of the total of the aluminum source powder, the magnesium source powder, and the yttrium source powder are generally 20 parts by mass to 1000 parts by mass, preferably 30 parts by mass to 300 parts by mass. When mixing in a wet form, A dispersing agent may be added to the solvent, and examples of the dispersing agent include inorganic acids such as nitric acid, hydrochloric acid, and sulfuric acid; organic acids such as oxalic acid, citric acid, acetic acid, malic acid, and lactic acid; and alcohols such as methanol, ethanol, and propanol; When a dispersing agent is used, the amount of the solvent is usually 0.1 parts by mass to 20 parts by mass per 100 parts by mass, and preferably 0.2 parts by mass to 10 parts by mass. When mixing, the solvent mixture can be removed to obtain a raw material mixture. The removal of the solvent can be generally carried out by distilling off the solvent. The method of distilling off the solvent is not particularly limited, and it can be air-dried at room temperature, vacuum dried or heated. dry. The drying method can be either standing dry or flowing dry. The temperature at the time of heating and drying is not particularly limited, but is generally 50 ° C or more and 25 ° ° C or less. The machine which can be used for heat drying can be, for example, a tray dryer, a slurry dryer, a spray dryer or the like. Further, when it is mixed in a wet form, it is dissolved in a solvent depending on the type of the source powder used, but the aluminum source powder or the like dissolved in the solvent is distilled off by a solvent and precipitated as a solid component. In the present invention, a raw material mixture containing the aluminum source powder, the titanium source powder, the magnesium source powder, and the cerium source powder arbitrarily used is molded to obtain a molded body, and then the formed body is fired to obtain an aluminum titanate-based fired product. Adult. By firing after molding, it is possible to effectively suppress the breakage of the obtained aluminum titanate-based fired body by suppressing the shrinkage during firing as compared with the direct firing of the raw material mixture. An aluminum titanate-based fired body in which the pore shape of the porous aluminum titanate crystal formed by the firing is maintained can be obtained. The shape of the molded body is not particularly limited, but may be, for example, a honeycomb shape, a rod shape, a tubular shape, a plate shape, a crucible shape or the like. The molding machine used for forming the raw material mixture may be a uniaxial press molding, an extruder, a tableting machine, a granulator or the like. When extrusion molding is carried out, an additive such as a void-forming agent, a lubricant, a plasticizer, a dispersant, and a solvent may be added to the raw material mixture for molding. Further, when the extrusion molding is carried out, a binder may be added to the raw material mixture. However, in the present invention, even if no binder is added or the amount of the binder is slightly added, an aluminum titanate having good mechanical properties can be produced. Burned body. Further, depending on the substance, there is a role of both a hole forming agent and a binder. Such a substance can be formed by adhering particles to each other at the time of molding, and then, when fired, it can be burned to form pores, and specifically, polyethylene or the like can be used. The above-mentioned pore forming agent may, for example, be a carbon material such as graphite; a resin such as polyethylene, polypropylene or polymethyl methacrylate; a plant material such as starch, nut shell, walnut shell or corn; ice; Dry ice, etc. The amount of the pore-forming agent to be added is generally 〇40 to 40 parts by mass, and preferably 0 to 25 parts by mass, based on 100 parts by mass of the total of the aluminum source powder, the titanium source powder, the magnesium source powder, and the cerium source powder. Examples of the lubricant and the plasticizer include alcohols such as glycerin: higher fatty acids such as capric acid, lauric acid, palmitic acid, arachidic acid, oleic acid, and stearic acid; and stearic acid metal salts such as aluminum stearate. Wait. Addition of Lubricant and Plasticizer-21 - 201041824 The amount is generally 〇~1〇 by mass, based on 100 parts by mass of the total of aluminum source powder, titanium source powder, magnesium source powder and lanthanum powder. ~5 parts by mass is preferred. Examples of the dispersant include inorganic acids such as nitric acid, hydrochloric acid, and sulfuric acid; organic acids such as oxalic acid, citric acid, acetic acid, malic acid, and lactic acid; alcohols such as methanol, ethanol, and propanol; A surfactant such as an oxidized olefin alkyl ether or the like. The amount of the dispersant added is usually from 0 to 20 parts by mass, preferably from 2 to 8 parts by mass, per 100 parts by mass of the total of the aluminum source powder, the titanium source powder, the magnesium source powder and the yttrium source powder. Further, as the solvent, for example, an alcohol such as a monool (methanol, ethanol, butanol or propanol), a glycol (such as propylene glycol, polypropylene glycol or ethylene glycol), or water can be used. Among them, water is preferred, and it is better to use ion-exchanged water from the viewpoint that it is less pure. The amount of the solvent to be used is preferably 10 to 100 parts by mass, and preferably 20 to 80 parts by mass, based on 100 parts by mass of the total of the aluminum source powder, the titanium source powder, the magnesium source powder and the yttrium source powder. Examples of the binder include celluloses such as methyl cellulose, carboxymethyl cellulose, and sodium carboxymethyl cellulose; alcohols such as polyvinyl alcohol; salts such as lignosulfonates; and paraffin waxes and crystallites; Wax wax; thermoplastic resin such as EVA, polyethylene, polystyrene, liquid crystal polymer, engineering plastics, etc. The amount of the binder added is preferably 0.3 parts by mass or less based on 100 parts by mass of the total of the aluminum source powder, the titanium source powder, the magnesium source powder, and the chopped source powder. When the binder is added, the binder is dispersed outside the fired body by the gas component which is burned to be CO 2 and H 20 , but after the binder is fired and removed, there is a void and the mechanical strength of the fired body is adversely affected. . From the point of view of -22- 201041824, it is better not to add a binder. The firing temperature of the fired molded body is usually 1300 ° C or higher, preferably l4 〇 0 ° C or higher. Further, since the aluminum titanate-based fired body to be produced is easily processed, the firing temperature is usually 1650 ° C or lower, preferably 1600 ° C or lower, more preferably 1 550 ° C or lower. The rate of temperature rise to the firing temperature is not particularly limited, but is generally from 2 ° C / hour to 500 ° C / hour. When the tantalum powder is used, it is preferred to maintain the temperature in the temperature range of 1100 to 1300 °C for 3 hours or more before the firing step. This step promotes melting and diffusion of the source powder. When the raw material mixture contains a binder or the like, the degreasing step for removing the material is included in the firing process. A typical degreasing system is carried out at a temperature rising stage (e.g., a range of 15 Torr to 400 ° C) at which the firing temperature is reached. The degreasing step is preferably such as to suppress the temperature increase rate as much as possible. The firing is generally carried out in the air, but may be based on the type and amount of the raw material powder (i.e., aluminum source powder, titanium source powder, magnesium source powder, and ruthenium source powder) used, and may be nitrogen, argon, or the like. The active gas is fired, or Q can be fired in a reducing gas such as carbon monoxide gas or hydrogen gas. Further, the firing can be carried out in an environment where the partial pressure of water vapor is lowered. The firing is generally carried out using a general firing furnace such as a tubular electric furnace, a box type electric furnace, a tunnel furnace, a far red outer furnace, a microwave heating furnace, a shaft furnace, a reverberatory furnace, a rotary furnace, and a drum chamber furnace. The firing can be carried out batchwise or in a continuous manner. Further, it can be carried out in a static manner or in a fluid manner. The time required for the calcination may be a time when the shaped body of the raw material mixture can sufficiently migrate to the magnesium aluminum titanate crystal, which may vary depending on the amount of the raw material mixture, the form of the firing furnace, the firing temperature, the firing environment, and the like. But generally it is -23- 201041824 1 0 minutes ~ 7 2 hours. The aluminum titanate-based fired body obtainable as described above. The aluminum titanate has a shape that can almost maintain the shape of the molded body after molding. The obtained aluminum-based fired product can be processed into a desired aluminum titanate-based calcined body by the boring process or the like in the X spectrum, except for the crystal form of the aluminum magnesium titanate. It may contain a crystal pattern of aluminum oxide, titanium dioxide or the like. The aluminum titanate system of the present invention can be represented by the formula: Al2(i-x)MgxTi(1+x)05. X 0.01 or more, 〇.〇1 or more and 0.7 or less is preferable, and more preferably 〇·〇2 t or less. [Embodiment] [Examples] Hereinafter, the present invention will be described in more detail by way of examples. Further, the obtained aluminum titanate-based fired body having an aluminizing ratio (AT conversion ratio), three-point bending strength, and a raw material particle size distribution were measured by the following methods. (1) AT conversion rate The degree of titanation of the titanate (AT rate) is the integrated intensity of the peak at the position of 20 = 27.4° (attributed to the surface of the titanium dioxide - phase (1 1 0 )) by the powder X-ray. (It ), in the shape of the titanic acid of the integral sintered body which is present at the peak of 20 (the surface of the yttrium acid magnesium (230) surface), is entangled in the sand, and is fired. 0.5, but the emission spectrum of the titanic acid powder is rutile = 33.7' strength ( -24- 201041824
Iat )，以下述式算出。 AT 化率= Ιατ/ (Ιτ+Ιατ) χ100(%) (2 )三點彎曲強度 將各實施例及比較例得到之鈦酸鋁系燒成體的三點_ 曲強度，依據JIS R 1001爲準進行測定，評價該機械強度 〇 (3 )原料粉末之粒度分布 體積基準之累積百分比5 0 %相當粒子徑（D 5 0 )係使 用雷射粒徑分析儀（Laser Diffraction Particle Size Analyzer)、[日機裝公司製造「Micro trac HR A ( X-100) 」]測定。 Q 〈實施例l > 原料粉末及添加劑係使用以下者。下述表示之「質量 份」係將原料粉末（鋁源粉末、鈦源粉末' 鎂源粉末及矽 源粉末）、添加劑、及水之合計量爲100質量份時之値。 下述之原料粉末的添加組成係以氧化鋁[A丨2 0 3 ]、二氧化 鈦[Ti〇2]、氧化鎂[Mg0]及二氧化矽[Si〇2]換算之莫耳比， 爲[A1203] / [Ti〇2] / [Mg〇] / [Si02] = 34.3% / 50.2% / 9.4 % / 6 · 1 %。 -25- 201041824 (1 )鋁源粉末 氧化鋁粉末（α型結晶、D 5 0 ·· 0.5 μπι ) 1 9.5質量份 (2 )鈦源粉末 氧化鈦粉末（金紅石型結晶、D 5 0 : 0.5 μπι ) 2 4.3質量份 (3 )鎂源粉末 水滑石類化合物粉末（協和化學工業（股）、「 DHT-4A」、D50 : 〇.4μπι ) 3.6質量份 (4 )矽源粉末 玻璃料（takara-standard 公司製作「CK0832」、D50 ：6 . Ο μπι ) 2.0質量份 (5 )添加劑 黏合劑（聚乙烯醇） 0.1質量份 (6 )水 5 0.5質量份 將上述鋁源粉末、鈦源粉末、鎂源粉末、矽源粉末、 添加劑及水（合計量1 98g )，與氧化鋁珠[直徑 15mm]500g同時投入塑膠製容器中[內容積il]。之後’將 該容器藉由球磨機，以振動數3 0Hz藉由使其回轉4小時 -26- 201041824 ，混合容器內之原料，得到前驅物混合物。將得到之前驅 物混合物以1 2 〇 °c，使其乾燥4小時後，使用乳缽進行粉 碎，得到原料混合物。將得到之原料混合物的2 g藉由以 單軸壓製機於〇.31/ cm2之壓力下進行成形，製作長約 5 0mm、寬約5mm、厚約4mm之成形體。接著，將該成形 體以箱型電氣爐箱型於昇溫速度300t/h下昇溫至1450 °C爲止，藉由於同溫度保持4小時，得到鈦鋁鎂系燒成體 Q 。將得到之燒成體以組成式：Α12 (MgxTi ( 1 + x) 05表示 時之χ的値係0.24。 將得到之燒成體以乳缽進行粉碎，藉由粉末X射線 繞射法’測定得到之粉末之衍射光譜時，該粉末係表示鈦 酸鋁鎂之結晶峰。求取該粉末之AT化率，結果爲1 00% 。又，燒成體之三點彎曲強度係lOMPa，表示良好的機械 強度。 〇 〈實施例2 > 不添加黏合劑（聚乙烯醇）以外係與實施例丨相同， 得到鈦鋁鎂系燒成體。 將得到之燒成體以乳缽進行粉碎，藉由粉末χ射線 繞射法’測定得到之粉末之衍射光譜時，該粉末係表示欽 酸銘鎂之結晶峰。求得該粉末之AT化率時，結果爲 100%。又，燒成體之三點彎曲強度係12MPa，表示良好 的機械強度。 -27- 201041824 <比較例I > 原料粉末係使用以下者。下述表示之「質量份」係轉 原料粉末（鋁源粉末、鈦源粉末、鎂源粉末及矽源粉未） 及水之合計量爲100質量份時之値。下述之原料粉末的添 加組成係以氧化鋁[Α12〇3]、二氧化鈦[Ti〇2]、氧化鎂 [Mg〇]及二氧化矽[si〇2]換算之莫耳比，爲[ai2o3] / [Ti〇2]/ [MgO]/ [Si02] = 3 4.3% / 50.2% / 9.4% / 6.1 %。 (1 )鋁源粉末 氧化鋁粉末（α型結晶、D 5 0 : 0 · 5 μηι ) 14.6質量份 (2 )鈦源粉末 氧化鈦粉末（金紅石型結晶、D 5 0 : 0.5 μΐη ) 2 5 . 1質量份 (3 )鎂源粉末 氧化鎂尖晶石粉末（D50: 5·5μπι) 9.3質量份 (4 )矽源粉末 玻璃料（takara-standard公司製作製作「CK0832」、 D50: 6.0 μηι ) (5 )水 2.0質量份 4 9 . 〇質量份 -28- 201041824 將上述鋁源粉末、鈦源粉末、鎂源粉末、矽源粉末及 水（合計量204g)與氧化鋁珠[直徑15mm]5〇〇g，同時地 投入於塑膠製容器[內容積1L]中。之後，將該容器藉由球 磨機以振動數3 0Hz使其回轉4小時，混合容器內之原料 ，得到前驅物混合物。將得到之前驅物混合物以1 2 0 °C , 使其乾燥4小時後，使用乳缽進行粉碎，得到原料混合物 。將得到之原料混合物的2g藉由以單軸壓製機於〇.3t/ 〇 cm2之壓力下進行成形，製作長約50mm、寬約5mm、厚 約4mm之成形體。接著，將該成形體以箱型電氣爐於昇 溫速度3〇〇°C/h下昇溫至1450°C爲止，藉由於同溫度保 持4小時’得到鈦鋁鎂系燒成體。得到之燒成體以組成： Al2( u MgxTi( 1+x) 〇5 表示時之 X 的値係 〇·24。 將所得到的燒成體以乳缽粉碎後，利用粉末X線繞 射法測定所得到粉末之繞射光譜時，該粉末係表示鈦酸鋁 鎂之結晶峰。求取該粉末之AT化率，結果爲100%。又 〇 ’燒成體之三點彎曲強度係被確認爲7.5 Μ P a、機械強度 爲低。 此次所揭示的實施形態及實施例之全部的點均爲例示 ’並無限制。本發明之範圍除了上述說明可包含如申請專 利範圍所示’均等於申請專利範圍之含義及範圍內之全部 作適當變更。 [產業上之利用可能性] 本發明所得的鈦酸鋁燒成體適用於，例如坩堝、耐火 -29- 201041824 架子、乳缽、爐材等燒成爐用器具；柴油機、汽油機等內 燃機關之排氣氣體淨化用的排氣過濾器或排氣轉換器、觸 媒載體、啤酒等飲用物過濾用之過濾器、精製石油時選擇 性使所生成之氣體成份，例如一氧化碳、二氧化碳、氮、 氧等透過用之選擇透過濾器等陶瓷濾器；基板、電容器等 電子構件等。 -30 -Iat ) is calculated by the following formula. AT conversion rate = Ιατ / (Ιτ + Ιατ) χ 100 (%) (2) Three-point bending strength The three-point bending strength of the aluminum titanate-based fired body obtained in each of the examples and the comparative examples is based on JIS R 1001. The measurement is performed to evaluate the mechanical strength 〇(3) The cumulative percentage of the particle size distribution volume basis of the raw material powder is 50%. The equivalent particle diameter (D 5 0) is a Laser Diffraction Particle Size Analyzer. Nikkiso Co., Ltd. manufactures "Micro trac HR A (X-100)"]. Q <Example 1 > The following materials were used as the raw material powder and the additive. The "mass portion" shown below is obtained by measuring the total amount of the raw material powder (aluminum source powder, titanium source powder 'magnesium source powder and tantalum source powder), additives, and water in 100 parts by mass. The additive composition of the raw material powder described below is a molar ratio in terms of alumina [A丨2 0 3 ], titanium dioxide [Ti〇2], magnesium oxide [Mg0], and cerium oxide [Si〇2], which is [A1203] ] / [Ti〇2] / [Mg〇] / [Si02] = 34.3% / 50.2% / 9.4 % / 6 · 1 %. -25- 201041824 (1) Aluminium source powdered alumina powder (α-type crystal, D 5 0 ·· 0.5 μπι ) 1 9.5 parts by mass (2 ) Titanium source powder titanium oxide powder (rutile crystal, D 5 0 : 0.5 Μπι ) 2 4.3 parts by mass (3 ) Magnesium source powder hydrotalcite compound powder (Xiehe Chemical Industry Co., Ltd., "DHT-4A", D50: 〇.4μπι) 3.6 parts by mass (4) Wuyuan powder glass frit (takara -standard company produces "CK0832", D50:6 . Ο μπι ) 2.0 parts by mass (5) additive binder (polyvinyl alcohol) 0.1 parts by mass (6) water 5 0.5 parts by mass of the above aluminum source powder, titanium source powder, Magnesium source powder, bismuth source powder, additive and water (total amount 1 98 g) were placed in a plastic container together with alumina beads [diameter 15 mm] 500 g [integral il]. Thereafter, the container was mixed with a raw material in a container by a ball mill at a vibration number of 30 Hz by rotating it for 4 hours -26 to 201041824 to obtain a precursor mixture. The precursor mixture was obtained at 12 ° C for 4 hours, and then pulverized using a mortar to obtain a raw material mixture. 2 g of the obtained raw material mixture was molded by a uniaxial pressing machine under a pressure of 〇.31 / cm 2 to prepare a molded body having a length of about 50 mm, a width of about 5 mm, and a thickness of about 4 mm. Then, the molded body was heated to 1,450 °C in a box-type electric oven type at a temperature rising rate of 300 t/h, and maintained at the same temperature for 4 hours to obtain a titanium aluminum-magnesium-based fired body Q. The obtained calcined body is of a composition formula: 値12 (MgxTi (1 + x) 05 represents a ruthenium system of 0.24. The obtained fired body is pulverized by a mortar, and is determined by powder X-ray diffraction method' In the diffraction spectrum of the obtained powder, the powder represents a crystallization peak of aluminum magnesium titanate. The AT conversion rate of the powder was found to be 100%. Further, the three-point bending strength of the fired body was 10 MPa, indicating good. (Example 2) The titanium-aluminum-based calcined body was obtained in the same manner as in Example 不 except that no binder (polyvinyl alcohol) was added. The obtained calcined body was pulverized in a mortar. When the diffraction spectrum of the powder obtained by the powder enthalpy diffraction method is measured, the powder represents a crystallization peak of the acid of magnesium, and when the AT conversion rate of the powder is determined, the result is 100%. The three-point bending strength is 12 MPa, which indicates good mechanical strength. -27- 201041824 <Comparative Example I > The raw material powder is the following. The "mass portion" shown below is a raw material powder (aluminum source powder, titanium source). Powder, magnesium source powder and Wuyuan powder) and water In the case of 100 parts by mass, the additive composition of the following raw material powder is converted into alumina [Α12〇3], titanium dioxide [Ti〇2], magnesium oxide [Mg〇], and cerium oxide [si〇2]. The ear ratio is [ai2o3] / [Ti〇2] / [MgO] / [Si02] = 3 4.3% / 50.2% / 9.4% / 6.1 %. (1) Aluminium source powdered alumina powder (alpha type crystal, D 5 0 : 0 · 5 μηι ) 14.6 parts by mass (2) Titanium source powder titanium oxide powder (rutile crystal, D 5 0 : 0.5 μΐη ) 2 5 . 1 part by mass (3 ) Magnesium source powder magnesia spinel Powder (D50: 5·5μπι) 9.3 parts by mass (4) Wuyuan powder glass frit (produced by takara-standard company "CK0832", D50: 6.0 μηι) (5) Water 2.0 parts by mass 4 9 . 〇 mass parts -28 - 201041824 The above-mentioned aluminum source powder, titanium source powder, magnesium source powder, yttrium source powder and water (total amount 204g) and alumina beads [diameter 15mm] 5〇〇g are simultaneously put into a plastic container [integral volume 1L After that, the container was rotated by a ball mill at a vibration number of 30 Hz for 4 hours, and the raw materials in the container were mixed to obtain a precursor mixture. After drying at 20 ° C for 4 hours, it was pulverized using a mortar to obtain a raw material mixture, and 2 g of the obtained raw material mixture was formed by molding under a pressure of t 3 t / 〇 cm 2 by a uniaxial pressing machine. A molded body having a length of about 50 mm, a width of about 5 mm, and a thickness of about 4 mm. Then, the molded body was heated to 1,450 °C in a box-type electric furnace at a temperature rising rate of 3 °C / h, and the titanium aluminum magnesium-based fired body was obtained by maintaining the same temperature for 4 hours. The obtained fired body is composed of: Al2( u MgxTi( 1+x) 〇5 represents the 値 system 〇·24 of X. The obtained fired body is pulverized by a mortar, and the powder X-ray diffraction method is used. When the diffraction spectrum of the obtained powder was measured, the powder showed a crystallization peak of aluminum magnesium titanate. The AT conversion rate of the powder was found to be 100%, and the three-point bending strength of the sintered body was confirmed. 7.5 Μ P a, mechanical strength is low. All the embodiments and examples of the present disclosure are exemplified as 'not limited. The scope of the present invention may be included as described in the patent application scope. All of the meanings and ranges within the scope of the patent application are appropriately changed. [Industrial Applicability] The aluminum titanate fired body obtained by the present invention is suitable for use in, for example, enamel, refractory -29-201041824 shelf, mortar, furnace Appliances such as materials for firing furnaces, exhaust filters for exhaust gas purification such as diesel engines and gasoline engines, exhaust gas converters, catalyst carriers, filters for drinking materials such as beer, and selective petroleum refining Make the generated gas into ., Such as carbon monoxide, carbon dioxide, nitrogen, oxygen selective permeation through the filter with ceramic filters and the like; electronic substrate member, such as a capacitor and the like -30--