201223662 六、發明說明： 【發明所屬之技術領域】 [0001] 本發明涉及一種金屬與陶瓷的連接方法及製得的連接件 ，尤其涉及一種不鏽鋼與氧化鋁陶瓷的連接方法及製得 的連接件。 【先前技術】 [0002] 不鏽鋼於常溫下具有較好的耐腐蝕性能，被廣泛應用於 製造各種工程結構及機械零件。然，當在高溫、腐蝕性 Ο 等較為惡劣的環境下使用時’不錄鋼已經很難滿足現代 ： 生產技術對材料綜合性能的進一步需求。而氧化鋁陶瓷 具有硬度高、高溫抗腐蝕、，耐磨报、抗沖敍等優點，故 ，不鏽鋼與氧化鋁陶瓷連接耷一起製廣成複合結構，對 於不鑛鋼於惡劣環境中應用具有非常重.要的意義。 [0003]目前採用的不鏽鋼與氧化鋁陶瓷固相擴散連接方法的連 接溫度通常超過800°C ’而且連接時間較長，造成能耗高 、成本上升。即便有習知技術採用鋁箔作為連接介質實 Q 現了不鏽鋼與氧化銘陶瓷的低溫固相擴散連接，然，由 於鋁與不鏽鋼容易生成大量金屬間化合物，當連接時間 較長時，鋁與不鏽鋼之間可能會由於金屬間化合物的大 量生成而先斷裂’從而降低了不鑛鋼與氧化Jg陶究的連 接強度。 【發明内容】 [0004] 有鑒於此，有必要提供一種既能於較低溫度下實現不鑛 鋼與氧化鋁陶瓷的擴散連接，又可防止因過多金屬間化 合物生成而降低連接強度的連接方法。 099143151 表單編號A0101 第3頁/共13頁 0992074738-0 201223662 上述連接方法製得的連接件 [0005]另外，還有必要提供一種由 〇 [0006] [0007] [0008] [0009] [0010] [0011] 099143151 -種不鏽鋼與氧化鋁陶瓷的連接方法，包括以下步驟： 提供待連接料鏽鋼件、氧化m㈣及銀猪； 將氧化㈣兗件、㈣、㈣及不_件放人連接模具 中’使_與銀hm純她喊件與㈣鋼件之間 並且鋁鑌與氧化鋁陶瓷件相鄰接，銀箔與不鏽鋼件相 鄰接； 將連接模具放人熱祕結爐中，於賴氣氛下對氧化紹 陶瓷件、鋁箔、銀箔及不鏽鋼件進行固相擴散連接，以 製成不鏽鋼與氧化鋁陶瓷的連接件。 一種由上述方法製得的不鏽鋼與氧化鋁陶瓷的連接件， 包括不鏽鋼件、氧化鋁陶瓷件及連接該不鏽鋼件與該氧 化鋁陶瓷件的連接部，該連接部包括第一過渡層、鋁層 、第二過渡層、銀層及第三過渡層，該第一過渡層位於 氧化鋁陶瓷件與鋁層之間，第一過渡層由鋁及氧化鋁組 成，该第二過渡層位於鋁層與該銀層之間，第二過渡層 由銀鋁金屬間化合物及銀鋁固熔體組成，該第三過渡層 位於銀層與不鏽鋼件之間，第三過渡由銀鐵金屬間化合 物及銀鐵固熔體組成。 相較於習知技術，上述不鏽鋼與氧化鋁陶瓷的連接方法 於熱壓燒結爐中藉由於氧化鋁陶瓷件一侧施加容易在低 溫下與氧化鋁陶瓷發生反應連接的鋁箔，於不鏽鋼件一 側則施加不容易與不鏽鋼生成金屬間化合物的銀箔共同 表單編號A0101 第4頁/共13頁 0992074738-0 201223662 [0012] Ο [0013] [0014] 作為連接介質，實現氧化鋁陶瓷件與不鏽鋼件的低溫固 相擴散連接。鋁箱與氧化鋁陶瓷件的低溫反應活性較大 ，易於低溫連接；而施加於不鏽鋼件一側的銀箔與不績 鋼的固熔性好，不易與不鏽鋼生成金屬間化合物，有利 於提高連接強度。 【實施方式】 請參閱圖1，本發明較佳實施例的不鏽鋼與氧化銘陶免的 連接方法藉由低溫固相擴散來完成，該方法包括如下蚩 驟： (1) 提供待連接的氧化鋁陶瓷件20與不鏽鋼件3〇，同 提供銘㈣與銀㈣作為連接介f 與銀叫 的厚度大約均為0.卜〇. 5mm，其較佳厚度為〇. 2 〇 3叫 〇 (2) 對氧化鋁陶瓷件20、不鏽鋼件3〇、鋁箱4〇及銀箱 50分別進行打磨、清洗，並吹幹。本實施_金相砂％ 進行打磨，經打磨後氧化銘陶究件2()、不_件3〇、餘 猪40及銀獅表面較為平整，表面粗輪度大約為卜2微米 。然後用盛裝有乙醇的超聲波清洗儀中進行振動清洗、 5~15分鐘，以除去氧化銘陶究件2〇、不鏽鋼件3〇、鋁落 40及銀㈣表面雜質及油污等，清洗後吹幹備用。以下 將氧化銘料件20、不鏽鋼_、料4()及銀㈣_ 為工件。 [0015] (3)將工件按照氧化鋁陶瓷件2〇 —鋁鶴 鐘鋼件30的順序放入一連接模具中， 099143151 '銀箱5 0 —-^ 使鋁箔4 0與銀鶴 50夾置於氧化鋁陶瓷件20與不鏽鋼件3〇之間， 表單編號A0101 第5頁/共13頁 並且銘箔 0992074738-0 201223662 40與氧化鋁陶瓷件20相鄰接，銀箔50與不鏽鋼件30相鄰 接。該連接模具70包括上壓頭72、下壓頭74及中模76。 該中模76具有一模腔（圖未示），用於容置待連接工件 。該上壓頭72與下壓頭74分別從兩側將放置於模腔中的 工件壓緊。該連接模具70可以為石墨材料製成。 [0016] [0017] [0018] (5) 將連接模具70放入一熱壓燒結爐1〇〇中，於保護氣 氛下對工件進行固相擴散連接。連接模具7〇放入熱壓燒 結爐100後對熱壓燒結爐100抽真空至2x1 (T3pa~8x 10_3Pa ’然後充入氬氣作為保護氣氛，充入氬氣後熱壓 燒結爐100内壓力可為〇. 2~G. 5MPa、於保護氣氛下將熱 壓燒結爐100升溫，並於如下工藝參數下對工件進行固相 擴散連接：升溫速率為l〇~5〇°C/min，連接溫度為 600〜655°C，於連接溫度的保溫時間為3〇〜6〇min ,轴向 壓力為20〜50MPa。軸向壓力的具體施加方法為：在溫度 到達300°C時，藉由上壓頭72與下壓頭74開始對工件施加 lOMPa的轴向壓力，之後碴慢痗大軸向壓力，直至溫度為 連接溫度時轴向壓力為最大值 .. . . 於上述溫度及壓力作用下，各工件接觸介面之間充分地 相互擴散；於連接溫度的保溫時間控制在3〇 6〇分鐘範圍 内時，各接觸介面間形成的擴散過渡層厚度對應的連接 強度最大，保溫時間過長時，不利於節約能源，而如果 保溫時間過短，則工件之間擴散不充分，難以形成明顯 的擴散過渡層，使工件之間難以形成良好的連接。 (6) 待冷卻後取出不鏽鋼件3〇與氧化鋁陶瓷件2〇的連接 件。 099143151 表單編號A0101 第6頁/共13頁 0992074738-0 201223662 [0019] Ο [0020] [0021] 〇 [0022] [0023] [0024] 上述不鏽鋼與氧化鋁陶瓷的連接方法於熱壓燒結爐100中 藉由在氧化鋁陶瓷件20—侧設置容易在低溫下與氧化鋁 陶瓷發生反應連接的鋁箔40，於不鏽鋼件30—侧則設置 不容易與不鏽鋼生成金屬間化合物的銀箔50共同作為連 接介質，實現氧化鋁陶瓷件20與不鏽鋼件30的低溫固相 擴散連接。鋁箔40與氧化鋁陶瓷件20的低溫反應活性較 大，易於低溫連接；而設置在不鏽鋼件30—側的銀箔50 與不鏽鋼的固熔性好，不易與不鏽鋼生成金屬間化合物 ，有利於提高連接強度。 圖2所示為由上述連接方法製得的不鏽鋼與氧化鋁陶瓷的 連接件10，包括該氧化鋁陶瓷件20、該不鏽鋼件30及連 接該不鏽鋼件30與該氧化鋁陶瓷件20的連接部80。該連 接部80包括一第一過渡層81、一銘層82、一第二過渡層 83、一銀層84及一第三過渡層85。 該第一過渡層81位於氧化鋁陶瓷件20與鋁層82之間。第 一過渡層81主要由鋁與氧化鋁組成。第一過渡層81由氧 化鋁陶瓷件20與所述鋁層82發生擴散反應形成。 該第二過渡層83位於鋁層82與該銀層84之間，其為鋁層 82與銀層84連接的過渡層。第二過渡層83主要由銀鋁金 屬間化合物及銀鋁固熔體組成。 該第三過渡層85位於銀層84與不鏽鋼件30之間，其為銀 層84與不鏽鋼件30連接的過渡層。第三過渡層85主要由 銀鐵金屬間化合物及銀鐵固熔體組成。 所述第一過渡層81、第二過渡層83及第三過渡層85的厚 099143151 表單編號Α0101 第7頁/共13頁 0992074738-0 201223662 度大約均為10~20/zm，所述铭層82與銀層84的厚度大約 均為 0. 08〜0. 45_。 [0025] 該不鏽鋼與氧化鋁陶瓷的連接件10的連接部80緻密均勻 ，無裂缝，無孔隙。經測試，該不鏽鋼與氧化鋁陶瓷的 連接件10的不鏽鋼/氧化鋁陶瓷介面的剪切強度大約為 20〜30MPa，抗拉強度大約為40〜50MPa。 【圖式簡單說明】 [0026] 圖1為本發明較佳實施例不鏽鋼與氧化鋁陶瓷的連接方法 原理示意圖。 [0027] 圖2為本發明較佳實施例的不鏽鋼與氧化鋁陶瓷的連接件 的剖面示意圖。 【主要元件符號說明】 [0028] 不鏽鋼與氧化鋁陶瓷的連接件：10 [0029] 氧化鋁陶瓷件：20 [0030] 不鏽鋼件：30 [0031}鋁箔：40 [0032] 銀箔：50 [0033] 連接模具：70 [0034] 上壓頭：72 [0035] 下壓頭：74 [0036] 中模：76 連接部：80 099143151 表單編號A0101 第8頁/共13頁 0992074738-0 [0037] 201223662 [0038] [0039] [0040] [0041] [0042] [0043] Ο 第一過渡層：81 鋁層：82 第二過渡層：83 銀層：84 第三過渡層·· 85 熱壓燒結爐：100 ο 099143151 表單編號Α0101 第9頁/共13頁 0992074738-0201223662 VI. Description of the Invention: [Technical Field] [0001] The present invention relates to a method for joining metal and ceramics and a connector for the manufacture thereof, and more particularly to a method for joining stainless steel and alumina ceramics and a connector for the same . [Prior Art] [0002] Stainless steel has good corrosion resistance at room temperature and is widely used in the manufacture of various engineering structures and mechanical parts. However, when used in harsh environments such as high temperatures and corrosive ’, it is difficult to meet modern requirements without the use of steel: production technology has further demand for the comprehensive performance of materials. Alumina ceramics have the advantages of high hardness, high temperature corrosion resistance, wear resistance, anti-crushing, etc. Therefore, stainless steel and alumina ceramics are combined to form a composite structure, which is very heavy for non-mineral steel applications in harsh environments. The meaning of the meaning. [0003] The connection temperature of the stainless steel and alumina ceramic solid phase diffusion bonding method currently used generally exceeds 800 ° C ' and the connection time is long, resulting in high energy consumption and high cost. Even with the conventional technology of using aluminum foil as the connection medium, the low-temperature solid-phase diffusion connection between stainless steel and oxidized ceramics is achieved. However, aluminum and stainless steel are prone to generate a large amount of intermetallic compounds. When the connection time is long, aluminum and stainless steel are used. There may be a breakage due to the large amount of intermetallic compound formation, which reduces the joint strength between the non-mineral steel and the oxidized Jg. SUMMARY OF THE INVENTION [0004] In view of the above, it is necessary to provide a connection method capable of achieving diffusion bonding of non-mineral steel and alumina ceramic at a lower temperature, and preventing connection strength due to excessive intermetallic formation. . 099143151 Form No. A0101 Page 3 of 13 0992074738-0 201223662 Connector made by the above connection method [0005] In addition, it is also necessary to provide a type [0006] [0007] [0008] [0009] [0010] [0011] 099143151 - a method for joining stainless steel and alumina ceramics, comprising the steps of: providing rust steel pieces to be connected, oxidizing m (four) and silver pigs; placing oxidized (four) enamel pieces, (four), (four) and non-pieces into a joint mold In the 'make _ with silver hm pure her shouting and (four) steel between the aluminum enamel and alumina ceramic parts adjacent, silver foil and stainless steel parts adjacent; the connection mold placed in the hot secret furnace, Yu Lai The solid phase diffusion connection of the oxidized ceramic parts, the aluminum foil, the silver foil and the stainless steel parts is carried out under the atmosphere to form a joint of stainless steel and alumina ceramics. A joint of stainless steel and alumina ceramic prepared by the above method, comprising a stainless steel member, an alumina ceramic member and a connecting portion connecting the stainless steel member and the alumina ceramic member, the connecting portion comprising a first transition layer and an aluminum layer a second transition layer, a silver layer and a third transition layer, the first transition layer being located between the alumina ceramic piece and the aluminum layer, the first transition layer being composed of aluminum and aluminum oxide, and the second transition layer being located in the aluminum layer and Between the silver layers, the second transition layer is composed of a silver-aluminum intermetallic compound and a silver-aluminum solid solution, the third transition layer is located between the silver layer and the stainless steel member, and the third transition is composed of the silver-iron intermetallic compound and the silver iron. Solid solution composition. Compared with the prior art, the above-mentioned method of joining stainless steel and alumina ceramics is carried out in a hot press sintering furnace by applying an aluminum foil which is easily connected to the alumina ceramic at a low temperature on the side of the alumina ceramic member, on the side of the stainless steel member. Then, a silver foil which is not easily formed with an intermetallic compound of stainless steel is applied. Form No. A0101 Page 4 of 13 0992074738-0 201223662 [0012] [0014] As a connecting medium, an alumina ceramic piece and a stainless steel piece are realized. Low temperature solid phase diffusion bonding. The aluminum box and the alumina ceramics have high reactivity at low temperature and are easy to be connected at low temperature. The silver foil applied to the side of the stainless steel member has good solid-melt property with the non-performance steel, and it is difficult to form an intermetallic compound with the stainless steel, which is advantageous for improving the joint strength. . [Embodiment] Referring to Figure 1, a method for joining stainless steel and oxidized ceramics in accordance with a preferred embodiment of the present invention is accomplished by low temperature solid phase diffusion, the method comprising the following steps: (1) providing alumina to be connected The ceramic part 20 and the stainless steel piece 3〇 are provided with the same (4) and silver (4) as the connection medium f and the thickness of the silver is about 0. 〇. 5mm, the preferred thickness is 〇. 2 〇3 〇 〇 (2) The alumina ceramic member 20, the stainless steel member 3, the aluminum box 4, and the silver box 50 are respectively ground, cleaned, and blown dry. This implementation _ metallographic sand% grinding, after polishing, oxidized Ming ceramics pieces 2 (), not _ pieces 3 〇, Yu pig 40 and silver lion surface is relatively flat, the surface coarse round is about 2 microns. Then use a ultrasonic cleaning device filled with ethanol for vibration cleaning for 5 to 15 minutes to remove the surface defects of the oxidized Ming ceramics, stainless steel 3 〇, aluminum 40 and silver (4) surface impurities and oil stains, etc. spare. The following will oxidize the name material 20, stainless steel _, material 4 () and silver (four) _ as the workpiece. [0015] (3) The workpiece is placed in a joint mold according to the order of the alumina ceramic piece 2〇-aluminum bell steel piece 30, 099143151 'silver box 5 0 —-^ to sandwich the aluminum foil 40 and the silver crane 50 Between the alumina ceramic member 20 and the stainless steel member 3, Form No. A0101, Page 5 of 13 and Ming Foil 0992074738-0 201223662 40 are adjacent to the alumina ceramic member 20, and the silver foil 50 is adjacent to the stainless steel member 30. Pick up. The joint mold 70 includes an upper ram 72, a lower ram 74, and a middle mold 76. The middle mold 76 has a cavity (not shown) for accommodating the workpiece to be joined. The upper ram 72 and the lower ram 74 respectively press the workpiece placed in the cavity from both sides. The joining mold 70 may be made of a graphite material. [0018] (5) The joining mold 70 is placed in a hot press sintering furnace 1 to perform solid phase diffusion bonding of the workpiece under a protective atmosphere. After the mold 7 is placed in the hot press sintering furnace 100, the hot press sintering furnace 100 is evacuated to 2x1 (T3pa~8x10_3Pa' and then argon gas is charged as a protective atmosphere. After the argon gas is filled, the pressure in the hot press sintering furnace 100 can be filled. 2〇G. 5MPa, the hot press sintering furnace 100 is heated under a protective atmosphere, and the workpiece is subjected to solid phase diffusion connection under the following process parameters: heating rate is l〇~5〇°C/min, connection temperature It is 600~655°C, the holding time at the connection temperature is 3〇~6〇min, and the axial pressure is 20~50MPa. The specific application method of axial pressure is: when the temperature reaches 300°C, by the upper pressure The head 72 and the lower pressing head 74 start to apply an axial pressure of 10 MPa to the workpiece, and then slowly reduce the axial pressure until the temperature is the connecting temperature, and the axial pressure is the maximum. . . under the above temperature and pressure, The workpiece contact interfaces are sufficiently inter-diffused; when the holding time of the connection temperature is controlled within a range of 3〇6〇 minutes, the thickness of the diffusion transition layer formed between the contact interfaces is the largest, and when the holding time is too long, Not conducive to saving energy, and if it is guaranteed If the time is too short, the diffusion between the workpieces is insufficient, and it is difficult to form a distinct diffusion transition layer, which makes it difficult to form a good connection between the workpieces. (6) After cooling, the stainless steel piece 3〇 is connected to the alumina ceramic piece 2〇 099143151 Form No. A0101 Page 6 of 13 0992074738-0 201223662 [0019] [0022] [0024] [0024] [0024] The above method of joining stainless steel and alumina ceramics is hot-pressed In the furnace 100, an aluminum foil 40 which is easily connected to the alumina ceramic at a low temperature is disposed on the side of the alumina ceramic member 20, and a silver foil 50 which is not easily formed with an intermetallic compound of stainless steel is provided on the side of the stainless steel member 30. The medium is connected to realize low temperature solid phase diffusion bonding of the alumina ceramic member 20 and the stainless steel member 30. The aluminum foil 40 and the alumina ceramic member 20 have high reactivity at low temperature and are easy to be connected at a low temperature; and the silver foil 50 disposed on the side of the stainless steel member 30 is 50. It has good solid-melt property with stainless steel, and it is not easy to form intermetallic compounds with stainless steel, which is beneficial to improve the joint strength. Figure 2 shows the stainless steel and oxygen produced by the above connection method. The aluminum ceramic connecting member 10 includes the alumina ceramic member 20, the stainless steel member 30, and a connecting portion 80 connecting the stainless steel member 30 and the alumina ceramic member 20. The connecting portion 80 includes a first transition layer 81, a An inscription layer 82, a second transition layer 83, a silver layer 84 and a third transition layer 85. The first transition layer 81 is located between the alumina ceramic member 20 and the aluminum layer 82. The first transition layer 81 is mainly made of aluminum. Composition with alumina. The first transition layer 81 is formed by diffusion reaction of the alumina ceramic member 20 with the aluminum layer 82. The second transition layer 83 is between the aluminum layer 82 and the silver layer 84, which is a transition layer between the aluminum layer 82 and the silver layer 84. The second transition layer 83 is mainly composed of a silver-aluminum intermetallic compound and a silver-aluminum solid solution. The third transition layer 85 is located between the silver layer 84 and the stainless steel member 30, which is a transition layer in which the silver layer 84 is joined to the stainless steel member 30. The third transition layer 85 is mainly composed of a silver-iron intermetallic compound and a silver-iron solid solution. The thickness of the first transition layer 81, the second transition layer 83, and the third transition layer 85 is 099143151. Form number Α0101, page 7 / total 13 pages 0992074738-0 201223662 degrees are about 10~20/zm, the layer The thickness of the layer 82 is about 0. 08~0. 45_. [0025] The connecting portion 80 of the connecting member 10 of the stainless steel and the alumina ceramic is dense and uniform without cracks and voids. The stainless steel/alumina ceramic interface of the stainless steel and alumina ceramic connector 10 has been tested to have a shear strength of about 20 to 30 MPa and a tensile strength of about 40 to 50 MPa. BRIEF DESCRIPTION OF THE DRAWINGS [0026] Fig. 1 is a schematic view showing the principle of connecting a stainless steel and an alumina ceramic according to a preferred embodiment of the present invention. 2 is a cross-sectional view showing a joint of a stainless steel and an alumina ceramic according to a preferred embodiment of the present invention. [Main component symbol description] [0028] Connector of stainless steel and alumina ceramic: 10 [0029] Alumina ceramic member: 20 [0030] Stainless steel member: 30 [0031} Aluminum foil: 40 [0032] Silver foil: 50 [0033] Connection mould: 70 [0034] Upper head: 72 [0035] Lower head: 74 [0036] Medium mould: 76 Connection: 80 099143151 Form number A0101 Page 8 of 13 0992074738-0 [0037] 201223662 [ [0043] [0043] [0043] [0043] Ο first transition layer: 81 aluminum layer: 82 second transition layer: 83 silver layer: 84 third transition layer · · 85 hot pressing sintering furnace: 100 ο 099143151 Form number Α 0101 Page 9 / Total 13 pages 0992074738-0