九、發明說明： 【發明所屬之技術領域】 本發明係有關於—#上+ ., 種破璃或玻璃-陶瓷組成物之 封接方法’尤指一種以-接〇·、 地试斗、▲ * 一種或二種以上熱性質不同之 ΐΓί:莞材料作為封接材料之玻璃或玻璃-陶 瓷組成物之封接方法。 ％㈣ 【先前技術】 :般而言’利用破璃封接之材料很多，包含有各 诂σ金、陶瓷和結晶化玻璃’其t使用最多係 該玻璃與金屬之封接。 ?玻璃與金屬之封接，係利用加熱該玻璃使其與 =先氧化之金屬或合金表面達到良好之浸潤而緊密地 結合在-起’隨後將該破璃和金屬冷卻至室溫，該玻 填和金屬㈣牢固地封接H成為—個整體。其 I。玄玻璃與金屬材料之種類眾多，若要將其彼此緊 密地結合在一起’必需先考量其基本特性。基本上兩 者之熱膨脹係數（Coefficient of Thermal Expansion， ^TE )值要十分接近’如果兩者之熱膨脹係數值和收 縮速率不同，當溫度變化時，玻璃和金屬都會產生應 力 旦應力值超過破璃之極限強度時，封接處即會 裂開，導致元件良率不佳。 就以往之封接材料在固態氧化物燃料電池運轉時 之應用而言，隨著工作溫度改變，由於不同組件間具 1356046 . 有不同熱膨脹係數值，加上工作溫度分佈不均勾，因 而在熱膨關數差異τ會產生不可純之_力 該熱應力對於”質之電解質與電極而言合促進 陶究材料既存之孔隙或缺陷成長為較大之裂/如此 將造成組件之㈣或破損，進而降低電池之效率。故， -般習用者係無法符合使用者於實際使用時之所需。 【發明内容】 本發明之主要目的係在於，以二種或二種以上熱 性質不同之玻璃或玻璃_陶究材料作為封接材料之方 法。 本發明之次要目的係在於，利用玻璃或玻璃-陶 材料彼此間之軟化溫度與結晶溫度之差異性，施以執 處理之控制’即可在不需要外加墊片之方式下，達到 封接及固定間距之目的。 為達以上之目的，本發明係一種玻璃或玻璃-陶瓷 組成物之封接方法，係選擇一第一基板，並在該第一 基板上排列有—第—、=、三之封接材料’且該第一 封接材料係排列於該第二封接材料與該第三封接材料 之間，並在該第一封接材料上放置一第二基板。對此 欲封接之結構進行加熱至該第一封接材料之軟化溫 度，且施加一負載使該第一封接材料軟化至該第二Z皿 三封接材料之高度後，再持續加熱至該第一封接材料 之結晶溫度並予以持溫，接著再繼續加熱至該第二、 »40 三封接材料之潤濕溫度 與欲封接之第_、_甘 第一、三封接材料 一基板之接著界面達到.剧 完成封接之效果。 卸關潤濕’即可 【實施方式】 明之ιΐ二『程第1 广第4圖』所示’係'分別為本發 圖、本發明之二圖接 接結構示意圖。如圖及本發明之封 陶究组成二:係一種玻璃或破璃-心钌接方法，其至少包括下列步驟： 一當2)排列封接材料1 1 :如第2圖所示，選擇 土板21 ，並在該第一基板2丄上排列有一 料“：一第二封接材料3 2及-第三封接 '、 ，且該第一封接材料3 1係排列於該第二封 材料3 2與該第三封接材料3 3之間，並在該第一 封接材料3 1上放置一第二基板2 2，而該第二封接 材料3 2及該第三封接材料3 3與該第二基板2 2之 間係存有—封接間隙高度，其中，該第…二基板2 1、2 2係為金屬或陶曼；該第-、二、三封接材料 3 1、3 2、3 3係為玻璃或玻璃-陶瓷組成物，又該 第一封接材料3 1之組成係可為二氧切（Si02)約〇 m〇l/〇氧化侧（Β203 )約0〜20 mol%、氧化銘 (Al2〇3)約 〇〜20 _〇/〇、氧化锅（Ba〇)約 〇〜4〇 mol/〇、氧化辦（CaO)、約〇〜i〇m〇i%及氧化鈦（Ti〇2) Ι356Ό46 . 約〇〜l〇mol%;該第二、三封接材料3 2、3 3之組 成係可為二氧化矽約〇〜4〇 m〇l%、氧化硼約〇〜2〇 mol/。、氧化銘約〇〜1〇 m〇i%、氧化鋇約〇〜4〇 、 氧化鈣約〇〜20mol%及氧化錯（Zr〇2)約〇〜5m〇i%; (B )加熱並持溫i 2 ··如第3圖所示，進行加 熱至該第-封接材料3 1為69G°C之軟化溫度，且施 加一負载使該第一封接材料3丄軟化至與該第二、三 封接材料3 2、3 3同冑，此時由於溫度並未到達該 封接材料3 2、3 3之軟化溫度71〇〇c，因 第 此本來由該第一封接材料31支撑之負載將由該第 ' =材料3卜33支撑。當持續加熱至該第 一封接材料3 1之結晶溫度觸。c時，將在 動作’待該第一封接材料31完全結晶後，由於其寺: =及結構強度已增加，因此該負载可轉由該第一封接 二1支撐’其卜該第一封接材料3 1係具有可 t晶性，且其溶點係較該第二、三封接材料32; 而該第二、三封接材料32、3 二 係 結晶性，或係結晶溫度較該第-封接材料31!了 大於900〇C ;以及 〇 π J丄呵， (C )繼續加熱至潤濕溫度2 3 繼續加熱至該第二封接材料3 2及該第三封接圖二示， 3之潤濕溫度’使該第-封接材料3卜嗜第』: 接材料33與欲封接:第:= 1及第-基板22之接著界面達到潤濕，即可 1356046 封接之效果。 當本發明於運用時，係利用二種或二種以上妖性 $不同之破璃或玻璃·陶㈣料作為封接材料用，藉由 破璃或玻璃-陶究材料彼此間之軟 曰 夕圼® k 一 又久、，.〇日曰/J2L度 差異性，可於加熱過程中’利用對熱處理之控制， 在不需要外加墊片之方式 距之目的。 P了達到封接及固定間 =上所述，本發明係—種玻璃或玻璃_陶1 组成物 之封接方法，可有效改善習用之種種缺點以二種或 -種以上玻璃或玻璃-陶免材料作為封接材料用，藉由 玻璃或玻璃-陶究材料彼此間之軟化溫度與結晶』声 之差異性，施以熱處理之控制，即可在不需要外加ς 片之方式下’達到封接及固定間距之目的，進而使本 發明之産生能更進步、更實用、更符合使用者之所項， 確已符合發明專利申請之要件’爰依法提出專利申請。 "惟以上所述者，僅為本發明之較佳實施例而已， 當不能以此限^本發明實施之範圍；&，凡依本發明 申請專利範圍及發明說明書内容所作之簡單的等^變 化與修飾，皆應仍屬本發明專利涵蓋之範圍内。 【圖式簡單說明】 第1圖’係本發日月之製作隸示意圖。 第2圖，係本發明之封接結構排列示意圖。 第3圖，係本發明之第一封接材料軟化示意圖。 第4圖，係本發明之封接結構示意圖。 【主要元件符號說明】 步驟（A)排列封接材料1 1 步驟（B )加熱並持溫1 2 步驟（C )繼續加熱至潤濕溫度1 3 第一基板2 1IX. Description of the invention: [Technical field to which the invention pertains] The present invention relates to a method for sealing a glass- or ceramic-ceramic composition, especially a type of joint-and-ground test. ▲ * One or more different thermal properties: 莞: The sealing method of glass or glass-ceramic composition as a sealing material. % (4) [Prior Art]: Generally speaking, there are many materials that use glass sealing, including various 诂σ gold, ceramics, and crystallized glass. The t is the most used for sealing the glass to metal. The sealing of the glass to the metal is performed by heating the glass to achieve a good wetting with the surface of the metal or alloy which is first oxidized, and then cooling the glass and the metal to room temperature, the glass Filling and metal (4) firmly sealing H into a whole. Its I. There are many kinds of glazed glass and metal materials, and if they are to be closely combined with each other, it is necessary to consider the basic characteristics first. Basically, the coefficient of thermal expansion (^TE) of the two is very close to 'if the coefficient of thermal expansion of the two is different from the rate of shrinkage, when the temperature changes, the stress and stress of the glass and the metal will exceed the value of the glass. At the ultimate strength, the seal will crack, resulting in poor component yield. In the past, the application of sealing materials in the operation of solid oxide fuel cells, as the operating temperature changes, due to the different thermal expansion coefficient values of different components, plus the uneven distribution of operating temperature, so in the heat The difference in the number of turbulences τ will result in impureness. The thermal stress is proportional to the electrolyte and the electrode. The existing pores or defects of the ceramic material grow into larger cracks/this will result in (4) or damage to the component. Further, the efficiency of the battery is lowered. Therefore, the conventional user cannot meet the needs of the user in actual use. SUMMARY OF THE INVENTION The main object of the present invention is to use two or more kinds of glass having different thermal properties or Glass-ceramic material as a method of sealing material. The secondary object of the present invention is to utilize the difference between the softening temperature and the crystallization temperature of glass or glass-ceramic materials, and to apply the control of the treatment The purpose of sealing and fixing the spacing is not required in the form of a gasket. For the above purpose, the invention is a glass or glass-ceramic composition. In the sealing method, a first substrate is selected, and a sealing material of the first, the third, and the third is arranged on the first substrate, and the first sealing material is arranged on the second sealing material and the Between the third sealing materials, and placing a second substrate on the first sealing material, heating the structure to be sealed to a softening temperature of the first sealing material, and applying a load to the first After the bonding material is softened to the height of the third sealing material of the second D dish, heating is continued to the crystallization temperature of the first sealing material and the temperature is maintained, and then heating is continued to the second, »40 The wetting temperature of the bonding material is the same as the sealing interface of the first and third sealing materials to be sealed. The effect of the sealing is completed. The sealing and wetting 'can be used 【Embodiment】 The 'systems' shown in the following figure are the schematic diagrams of the connection diagram of the second diagram of the present invention. The figure and the invention of the invention are composed of two types: a glass or a broken glass- A cardiac splicing method comprising at least the following steps: First, when 2) arranging the sealing material 1 1 : 2, the soil plate 21 is selected, and a material "a second sealing material 3 2 and a third sealing material" is arranged on the first substrate 2 , and the first sealing material 3 1 Arranging between the second sealing material 3 2 and the third sealing material 3 3 , and placing a second substrate 2 2 on the first sealing material 31 , and the second sealing material 3 2 And a gap height between the third sealing material 3 3 and the second substrate 2 2, wherein the second substrate 2 1 , 2 2 is metal or Taman; the first -, The second sealing material 3 1 , 3 2 , 3 3 is a glass or glass-ceramic composition, and the composition of the first sealing material 31 can be dioxo (Si02) about 〇m〇l/ The oxidized side (Β203) is about 0~20 mol%, the oxidation is (Al2〇3) about 20~20 _〇/〇, the oxidation pot (Ba〇) is about 〇~4〇mol/〇, the oxidation office (CaO), About 〇~i〇m〇i% and titanium oxide (Ti〇2) Ι356Ό46. about 〇~l〇mol%; the second and third sealing materials 3 2, 3 3 may be cerium oxide ~4〇m〇l%, boron oxide about 〇~2〇mol/. , oxidation 铭 〇 〇 〇 〇 〇 〇 〇 〇 〇 〇 〇 〇 钡 钡 〇 〇 〇 〇 〇 〇 〇 〇 〇 〇 〇 〇 〇 〇 〇 〇 〇 〇 〇 〇 〇 〇 〇 〇 〇 〇 20 20 20 20 20 20 20 20 20 20 20 20 20 Temperature i 2 ·· as shown in FIG. 3, heating to the first sealing material 31 is a softening temperature of 69 G ° C, and applying a load to soften the first sealing material 3 与 to the second The three sealing materials 3 2, 3 3 are the same, at this time, since the temperature does not reach the softening temperature 71〇〇c of the sealing material 3 2, 3 3 , because the first sealing material 31 is originally supported by the first sealing material 31 The load will be supported by the 'material 3' 33. When it is continuously heated to the crystallization temperature of the first bonding material 3 1 . c, will be in action 'after the first sealing material 31 is completely crystallized, because its temple: = and structural strength has increased, so the load can be transferred by the first sealing two 1 support' The sealing material 31 has t-crystallinity, and its melting point is compared with the second and third sealing materials 32; and the second and third sealing materials 32, 3 are two-layer crystalline or crystallization temperature The first sealing material 31! is greater than 900 〇C; and 〇π J 丄, (C) continues to heat to the wetting temperature 2 3 to continue heating to the second sealing material 3 2 and the third sealing diagram Secondly, the wetting temperature of 3 'makes the first sealing material 3 to be the same": the bonding material 33 and the interface to be sealed: the first interface of the first layer and the first substrate 22 are wetted, that is, 1356046 The effect is connected. When the present invention is used, it is used as a sealing material by using two or more kinds of glazed or different glass or ceramic (four) materials, which are softened by glass or glass-ceramic materials.圼® k One-and-a-half, 〇 曰 曰/J2L degree difference, can be used in the heating process to control the heat treatment, without the need for additional gaskets. P has reached the sealing and fixing room = the above, the invention is a sealing method of the glass or glass_ceramic 1 composition, which can effectively improve various disadvantages of the conventional two or more kinds of glass or glass-ceramic The free material is used as a sealing material, and the difference between the softening temperature and the crystallization sound of the glass or the glass-ceramic material is controlled by the heat treatment, so that the sealing can be achieved without the need for additional slabs. The purpose of connecting and fixing the spacing, so that the invention can be made more progressive, more practical, and more in line with the user's requirements, has indeed met the requirements of the invention patent application '爰 patent application. The above is only the preferred embodiment of the present invention, and is not intended to limit the scope of the present invention; &, simple, etc. according to the scope of the present invention and the contents of the invention ^Changes and modifications should still fall within the scope of the invention patent. [Simple description of the diagram] Figure 1 is a schematic diagram of the production of the sun and the moon. Fig. 2 is a schematic view showing the arrangement of the sealing structure of the present invention. Figure 3 is a softened schematic view of the first sealing material of the present invention. Figure 4 is a schematic view of the sealing structure of the present invention. [Description of main component symbols] Step (A) Arrange the sealing material 1 1 Step (B) Heat and hold the temperature 1 2 Step (C) Continue heating to the wetting temperature 1 3 First substrate 2 1
第一基板2 2 第一封接材料3 1 第二封接材料3 2 第三封接材料3 3First substrate 2 2 first bonding material 3 1 second sealing material 3 2 third sealing material 3 3