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研究生: 陳煥煜
Chen, Huan-Yu
論文名稱: 使用不同形態之鋁粉以燃燒合成法製備氮化鋁粉體之製程開發及反應機構探討
Process Development for Combustion Synthesis of Aluminum Nitride Using Aluminum Powders with Different Morphology and Study on the Reaction Mechanism
指導教授: 鍾賢龍
Chung, Shyan-Lung
學位類別: 碩士
Master
系所名稱: 工學院 - 化學工程學系
Department of Chemical Engineering
論文出版年: 2011
畢業學年度: 99
語文別: 中文
論文頁數: 88
中文關鍵詞: 燃燒合成法氮化鋁
外文關鍵詞: Combustion synthesis, Aluminum Nitride
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  • 目前本實驗室以燃燒合成法製備氮化鋁粉其技術已相當成熟,其合成所需之原料-鋁粉,規格為粒狀30~80 μm,純度為99.9 %,雖其純度高且反應性佳,但價格昂貴,為了降低生產成本增加本實驗室氮化鋁生產的競爭力並避免鋁粉來源被壟斷,本論文研究使用不同來源鋁粉以燃燒合成法合成氮化鋁,經探尋數種市售之鋁粉後,選擇兩種價位較低之鋁粉,即粒狀10~50 μm,純度99.0 %和粒狀10~30 μm,純度99.5 %。先前研究指出此兩種鋁粉易熔聚且產物氧含量高。本論文研究主要以粒狀10~50 μm之鋁粉為主,其餘兩種鋁粉為輔,利用不同的表面處理來探討合成反應之燃燒現象,同時使用SEM觀察其晶體成長以作為不同表面處理影響的佐證,並藉由改善氮氣流通通道來克服因堆積密度高所造成較差的反應性,最後合成出與舊有鋁粉的製程相近氧含量的氮化鋁,研磨前氧含量介於0.3~0.6 wt%,研磨至3~4 μm氧含量約在1.4 wt%。

    The technique for synthesis of aluminum nitride powder by self-propagating high temperature synthesis (SHS) has been well developed in our laboratory. The mostly used aluminum powder for the synthesis has been sphere in shape with dimensions of 30~80 μm, and a purity of 99.9 %. This aluminum powder has a high purity and a good reactivity but is relatively costly. In order to reduce the production cost and avoid the monopolization of source of aluminum powder, we searched for other sources for aluminum powder. Two different types of aluminum powder were investigated for synthesis of aluminum nitride: (1) irregular particle, 10~50 μm on average and 99.0 % purity; (2) irregular particle, 10~30 μm and 99.5 % purity. Previous studies indicate that these two type of aluminum powder can easily form aggregates during synthesis reaction and oxygen contents of the products are high. This thesis research focused on synthesis of aluminum nitride powder by using the aluminum powder with 10~50 μm in size, and the results were compared with experimental results of other aluminum powders. The combustion phenomena were found to be related to different surface modification of the aluminum powders, and the results were also proved by SEM observation. Beside, the poor reactivity due to high packing density of the aluminum powder was improved by setting an porous aluminum tube in the reactant compact. Using the aluminum powder and the synthesis technique developed in the present study, the product has an oxygen content of 0.3~0.6 wt% before milling, and about 1.4 wt% after milling.

    摘要 I Abstract II 誌謝 III 目錄 IV 表目錄 X 圖目錄 XII 第一章 緒論 1 1-1 研究背景 1 1-2 氮化鋁簡介 1 1-3 研究動機 5 第二章 原理及文獻回顧 6 2-1 燃燒合成法 6 2-2 燃燒反應動力學 7 2-3 燃燒反應熱力學 8 2-4 反應物孔隙度和壓力對燃燒合成反應的影響 10 2-5 氣相反應成核 12 2-5-1 均勻相成核(Homogeneous nucleation) 12 2-5-2 異質相成核(Heterogeneous nucleation) 14 2-6 燃燒合成之溫度曲線與添加劑之關係 16 2-7 燃燒合成反應引燃過程分析 16 第三章 實驗裝置與藥品 19 3-1 實驗反應裝置 19 3-1-1 小型反應器裝置 19 3-1-2 大型反應器裝置 20 3-1-3 大型研磨機裝置 20 3-2 其他儀器設備 21 3-2-1 輔助儀器設備 21 3-2-2 分析儀器設備 21 3-3 實驗藥品 22 第四章 實驗方法 27 4-1反應錠製備 27 4-2 氮化鋁燃燒合成反應 27 4-3 轉化率量測 28 4-3-1 實驗目的 28 4-3-2 實驗步驟 28 4-3-3 產物轉化率之計算 28 4-4 產物分類 30 第五章 結果與討論 31 5-1 鋁粉來源及其性質 31 第一部分 燃燒合成反應氮化鋁之反應條件探討 32 5-2 使用A2鋁粉之製程開發 32 5-2-1中型反應錠 32 5-2-1-1 表面處理 32 5-2-1-1-1 添加氫氧化鋁 32 5-2-1-1-2 恆溫恆濕處理 33 5-2-1-1-3 添加氯化銨 33 5-2-1-2 稀釋劑-添加氮化鋁(<270 mesh) 34 5-2-1-3 壓力影響 36 5-2-2 大型反應錠 38 5-2-2-1 添加氫氧化鋁 38 5-2-2-1-1 添加量影響 38 5-2-2-1-2 壁厚探討 39 5-2-2-1-3 二次燃燒波現象 39 5-2-2-2 恆溫恆濕處理 42 5-2-2-3 鋁管設置 44 5-2-2-5 共同效應 46 5-2-2-5-1 恆溫恆濕搭配氫氧化鋁 47 5-2-2-5-2 恆溫恆濕搭配3~4 μm APS改質之氮化鋁 47 5-3 使用A3 鋁粉之製程開發 50 5-3-1 小型反應錠 50 5-3-1-1 表面處理 50 5-3-1-1-1 添加氫氧化鋁 50 5-3-1-1-2 添加氯化銨 51 5-3-1-2 稀釋劑-添加氮化鋁(<270 mesh) 51 5-3-2 中型反應錠 51 5-4 研磨 53 第二部分 燃燒合成反應氮化鋁之形態探討 56 5-5 氮化鋁晶體形態 56 5-5-1 未添加添加劑之氮化鋁形態 57 5-5-2 添加氫氧化鋁之氮化鋁形態 58 5-5-3 添加氯化銨之氮化鋁形態 63 5-5-4 添加氮化鋁之氮化鋁形態 68 5-5-5 恆溫恆濕後之氮化鋁形態 72 5-5-6 添加1 wt%氫氧化鋁在不同壓力下之氮化鋁形態 73 5-5-7 氮化反應機制 75 5-6 不同形態鋁粉其合成條件及結果比較 78 5-6-1 中型反應錠 78 5-6-2 大型反應錠 79 5-6-3 熔聚現象 80 5-6-4 二次燃燒波現象 80 5-6-5 產物外觀和硬度 81 第六章 結論 82 參考文獻 85 自述 88

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