軟銲是電子產品主要的連接方法，過去常用錫鉛合金作為軟銲銲料，然而因為鉛對環境及身體健康具有危害，無鉛銲料取代錫鉛銲料成為工業界目前主要使用的銲料，包括了錫-銀、錫-銅、錫-銦、錫-鉍、錫-銀-銅、錫-銀-銦...等合金。雖然無鉛銲料已被使用，但是在軟銲溫度與性質上仍存在著許多改進空間，而透過不同元素的摻雜可以改變合金的性質。本研究探討錫-銀-銅-銦-鉍五元合金系統中部分三元與四元子系統的相轉變溫度，合金的液相線溫度及固相線溫度，與軟銲的加工溫度直接相關，為銲料的重要性質。相平衡的資料可以由實驗測定及以Calphad方法計算獲得。目前文獻中雖然有上述五元合金的Calphad熱力學資料庫，但是初步的計算結果顯示與實驗量測結果存在著顯著誤差。
本研究進行相關三元系統的不變反應(invariant)附近以及四元系統合金的熱分析實驗。本研究所使用的熱力學資料庫分別為NIST與Gierlotka公開的database與CompuTerm所提供的database，再以上述三者的計算結果與實驗量測的結果進行比較，進行了錫-銀-銅、錫-銀-鉍、錫-銀-銦、錫-銅-銦及錫-鉍-銦五個三元系統與錫¬¬-銀-銅-鉍、錫-銀-銅-銦兩個四元系統的量測，結果顯示錫-銅-銦三元系統中，以Computherm提供的data base所計算之不變反應(invariant)溫度低於實驗結果約8℃，錫-鉍二元系統以Computherm提供的data base所計算的共晶溫度高於實驗結果約4℃外，其餘三元合金不變反應(invariant)溫度的實驗結果與計算結果接近，而液化溫度則有明顯差距，四元系統中計算的液化溫度與固化溫度與實驗結果皆有差距。本研究中提供之實驗數據可做為Calphad模型參數優化的參考依據，並幫助建立出錫-銀-銅-銦-鉍五元系統的Calphad模型。

Soldering is the main connection method for electronic packaging. Tin-lead solder alloys were commonly used in the past. However, because lead is harmful to the environment and health, lead-free solder replaces tin-lead solder as the main solder currently used in the industry, including tin-silver, tin-copper, tin-indium, tin-bismuth, tin-silver-copper, tin-silver-indium... and other alloys. Although lead-free solder has been used, there are still many room for improvement in the soldering temperature and properties, and the properties of the alloy can be changed through the doping of different elements. The purpose of this study is to discuss the phase transformation temperature of some of the ternary and quaternary subsystems, the liquidus temperature and solidus temperature of solder alloys are directly related to the processing temperature of soldering, which are important properties of solder. The data of phase equilibrium can be obtained by experimental determination and calculation by Calphad method. Although there is a Calphad thermodynamic database of the above-mentioned five-element alloy in the literature, significant differences of the phase transformation temperature are observed between those calculated and experimental determined.
In this study, the thermal analysis of the alloy near the invariant reaction of the related ternary system was carried out. The thermodynamic database used in this research is the database published by NIST and Gierlotka and the database provided by CompuTerm, the calculation results of the above three are compared with the results of experimental measurements. Phase transformation termperatures of five ternary systems, tin-silver-copper, tin-silver-bismuth, tin-silver-indium, tin-copper-indium and tin-bismuth-indium and two quaternary systems, tin-silver-copper-bismuth and tin-silver-copper-indium are carried out in this study. The experimental results show that in the tin-copper-indium ternary system, the invariant reaction temperature calculated by using the data base of Computherm is about 8℃ lower than the experimental result, in the tin-bismuth binary system, the eutectic temperature calculated by using the data base of Computherm is about 4℃ higher than the experimental results. The experimental results of the invariant reaction temperature of the other ternary alloys are in good agreement with the calculated results, while significant deviations are observed regarding their liquidus temperatures. In the two quaternary systems, significant deviations are observed both in their liquidus temperatures and solidus temperatures. The Calphad modeling requires experimental data to fine tune their parameters. The experimental data provided in this study certainly contribute to the validity of the Calphad modeling of Ag-Bi-Cu-In-Sn quinary system.

目錄

摘要 2
Abstract 3
目錄 6
表目錄 10
圖目錄 12
一、前言 20
二、文獻回顧 23
2-1 液相線投影 23
2-2 二元系統 27
2-2-1 Ag-Cu二元系統 27
2-2-2 Sn-Ag二元系統 27
2-2-3 Sn-Cu二元系統 29
2-2-4 Sn-Bi二元系統 30
2-2-5 Ag-Bi二元系統 31
2-2-6 Bi-Cu二元系統 32
2-2-7 Sn-In二元系統 33
2-2-8 Ag-In二元系統 34
2-2-9 Bi-In二元系統 36
2-2-10 Cu-In二元系統 37
2-3三元相圖 39
2-3-1 Sn-Ag-Cu三元系統 39
2-3-2 Sn-Ag-Bi三元系統 42
2-3-3 Sn-Cu-Bi三元系統 43
2-3-4 Ag-Cu-Bi三元系統 45
2-3-5 Sn-Ag-In三元系統 46
2-3-6 Sn-In-Cu三元系統 49
2-3-7 Sn-Bi-In三元系統 51
2-3-8 Ag-Cu-In三元系統 53
2-3-9 Cu-Bi-In三元系統 56
2-3-10 Ag-Bi-In三元系統 58
2-4四元相圖 60
2-4-1 Sn-Ag-Bi-Cu四元系統 60
2-4-2 Sn-Ag-Bi-In四元系統 61
2-4-3 Sn-Bi-Cu-In四元系統 62
2-4-4 Sn-Ag-Cu-In四元系統 63
2-4-5 Ag-Bi-Cu-In四元系統 64
2-5五元相圖 64
2-5-1 Sn-Ag-Bi-Cu-In五元系統 64
2-6相圖計算 65
三、研究方法 67
3-1 合金之製備 67
3-2 DSC熱分析 67
3-3 相圖計算 67
四、結果與討論 68
4-1 DSC熱分析結果 68
4-1-1 Sn 68
4-1-2 In 69
4-1-3 Pb 71
4-1-4 Sn-Ag二元系統 73
4-1-5 Sn-Bi二元系統 74
4-1-6 Sn-Cu二元系統 74
4-1-7 Sn-In二元系統 75
4-1-8 Sn-Ag-Cu三元合金 76
4-1-9 Sn-Ag-In三元系統 88
4-1-10 Sn-Cu-In三元系統 98
4-1-11 Sn-Ag-Bi三元系統 109
4-1-12 Sn-Bi-In三元系統 122
4-1-13 Sn-Ag-Bi-Cu四元系統 133
4-1-14 Sn-Ag-Cu-In四元系統 139
五、結論 148
六、參考文獻 150

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