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以作者查詢圖書館館藏 、以作者查詢臺灣博碩士 、以作者查詢全國書目 、勘誤回報 、線上人數：69 、訪客IP：18.223.172.122
姓名 黃啓明(Qi-Ming Huang) 查詢紙本館藏 畢業系所 化學工程與材料工程學系 論文名稱 熱電材料碲化錫與銅電極之界面反應 相關論文 檔案 [Endnote RIS 格式]
[相關文章]
[文章引用]
[完整記錄]
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至系統瀏覽論文 (2029-7-31以後開放)
摘要(中) 近年來，隨著科技的迅速發展和環保意識的提升，對綠色能源來源的需求顯著增加。熱電模組，這種將廢熱轉換為電能的技術在再生能源領受到關注。其中，由碲化錫（SnTe）為基礎材料的中溫熱電模組在400至800K範圍內的高性能尤其引人注目。雖然在熱電性能上略遜於碲化鉛（PbTe），但碲化錫因其安全無毒的特性而更受青睞。 在實際應用中，中溫熱電模組會經歷長時間的高溫環境，導致熱電材料與電極之間發生劇烈的界面反應，這可能會顯著地降低模組性能，甚至可能導致模組失效。而在本研究中，將使用市售的銀銅鋅錫高溫銲膏，在973K條件下焊接1分鐘來接合碲化錫與銅電極。然後，樣品將在500K與600K溫度下進行0、1、5和15天的熱時效測試。本
研究旨在探討不同溫度下的界面反應，並評估中溫SnTe 熱電模組在長期運行條件下的可靠性。並嘗試加入電鍍鈷(Co)作為阻障層來改善接合狀況，在600K溫度下、0、1、5和15天的熱時效測試來評估電鍍鈷作為阻障層對於界面反應以及接點機械性質之影響。 由實驗結果得知，以此方式接合可以成功結合碲化錫與銅電極並且在500K、15天的熱時效測試下維持一定的接點強度，但在600K的情況下，因界面反應過於劇烈導致接點處大量銅擴散導致機械強度大幅下降，但在引入電鍍鈷擴散阻障層後不僅提升接點強度，經熱時效測試後亦維持良好的接點強度。摘要(英) Recent advancements in technology and growing environmental awareness have increased the demand for green energy sources. Thermoelectric modules, which convert waste heat into electricity, are gaining attention. Mid-temperature modules made of tin telluride (SnTe) are notable for their high performance in the 400-800 K range. Although lead telluride has slightly better thermoelectric properties, SnTe is preferred for its safety and non-toxicity. In practical applications, mid-temperature thermoelectric modules undergo long term thermal aging, leading to interfacial reactions between the thermoelectric materials and electrodes. This can significantly reduce module performance or even cause failure. In this study, commercial AgCuZnSn braze paste will be used to bond SnTe with Cu electrodes under the
condition of 973 K for 1 minute. The samples will then undergo thermal aging tests at 500 K and 600 K for 1, 5, and 15 days. This research aims to investigate interfacial reactions at different temperatures and assess the reliability of mid-temperature SnTe thermoelectric
modules under long-term operational conditions. Additionally, cobalt (Co) electroplating will be attempted as a barrier layer to improve joint conditions. Thermal aging tests at 600 K for 1, 5, and 15 days will be conducted to evaluate the effect of Co electroplating on interfacial reactions and joint mechanical properties. Experimental results indicate that this bonding method can successfully bond SnTe and
Cu electrodes, maintaining a certain level of joint strength after thermal aging tests at 500 K for 15 days. However, at 600 K, intense interfacial reactions cause significant Cu diffusion at the joint, leading to a substantial decrease in joint strength. Introducing a Co diffusion barrier not
only improves joint strength but also maintains good joint strength after thermal aging tests.關鍵字(中) ★ 熱電材料
★ 碲化錫
★ 鈷阻障層
★ 硬焊接合
★ 老化測試
★ 推力測試關鍵字(英) ★ thermoelectric device
★ SnTe
★ Co diffusion barrier
★ brazing
★ aging test
★ shear test論文目次 目錄
摘要 ............................................................................................................................................. i
Abstract ....................................................................................................................................... ii
致謝 ...........................................................................................................................................iii
目錄 ............................................................................................................................................ v
圖目錄 ...................................................................................................................................... vii
表目錄 ....................................................................................................................................... ix
第一章 緒論 ............................................................................................................................ 1
1-1 能源議題 ..................................................................................................................... 1
1-2 熱電材料 ..................................................................................................................... 3
1-2-1 熱電效應基礎原理.......................................................................................... 3
1-2-2 熱電模組裝置應用.......................................................................................... 5
1-3 碲化錫中溫熱電材料 ................................................................................................. 8
1-4 熱電材料界面接合 ................................................................................................... 10
1-4-1 熱壓接合........................................................................................................ 10
1-4-2 火花電漿燒結................................................................................................ 12
1-4-3 固液擴散接合................................................................................................ 13
1-4-4 硬焊................................................................................................................ 15
1-5 擴散阻障層 ............................................................................................................... 17
1-5-1 電鍍沉積擴散阻障層.................................................................................... 20
第二章 研究目的與動機 ...................................................................................................... 22
第三章 實驗方法 .................................................................................................................. 23
3-1 碲化錫熱電材料製備 ............................................................................................... 23
3-2 電鍍鈷擴散阻障層 ................................................................................................... 23
3-3 硬焊接合 ................................................................................................................... 23
3-4 推力測試 ................................................................................................................... 24
3-5 熱時效測試 ............................................................................................................... 24
3-6 試片分析 ................................................................................................................... 24
3-6-1 X光光電子能譜儀 (X-ray photoelectron spectroscopy, XPS) ..................... 24
3-6-2 掃描式電子顯微鏡 (Scanning electronic microscope, SEM) ...................... 25
3-6-3 能量散佈光譜儀 (Energy Dispersive Spectrometer, EDS) .......................... 26
3-6-4 場發式電子微探儀 (Field Emission Electron Probe Microanalyzer, FE-
EPMA) ...................................................................................................................... 27
第四章 結果與討論 .............................................................................................................. 28
4-1 碲化錫熱電塊材製備 ............................................................................................... 28
4-2 SnTe/AgCuZnSn/Cu硬焊接合之接點 ...................................................................... 30
4-2-1 SnTe/AgCuZnSn/Cu接點之熱時效測試 ...................................................... 33
vi
4-2-2 SnTe/AgCuZnSn/Cu接點之推力測試與破斷面分析 .................................. 34
4-3 SnTe/Co/AgCuZnSn/Cu硬焊接合之接點 ................................................................ 38
4-3-1 SnTe/Co/AgCuZnSn/Cu接點熱時效測試 .................................................... 41
4-3-2 SnTe/Co/AgCuZnSn/Cu接點之推力測試與破斷面分析 ............................ 48
第五章 結論 .......................................................................................................................... 55
參考文獻與資料 ...................................................................................................................... 57
vii
圖目錄
圖 1-1 全球能源消耗來源圖[1] .............................................................................................. 1
圖 1-2 車輛能源損失比例圖[2] .............................................................................................. 2
圖 1-3 典型的熱電裝置圖[8] .................................................................................................. 6
圖 1-4 TEC與TEG簡單示意圖[9] ......................................................................................... 7
圖 1-5 SnTe的三種晶體結構[20] ............................................................................................ 9
圖 1-6 SnTe-based熱電材料zT值時間線[20] ..................................................................... 10
圖 1-7 PbTe對Cu接合截面SEM圖[33] ............................................................................. 11
圖 1-8 Pb0.6Sn0.4Te對Cu接合截面SEM圖[33] .................................................................. 11
圖 1-9 SPS接合Mg2Si與Cu流程圖與截面圖[37] ............................................................. 12
圖 1-10 Mg2Si對Cu接合截面SEM圖[37] ......................................................................... 13
圖 1-11 TLP示意圖[41] ......................................................................................................... 13
圖 1-12 (a)TLP方式接合Sn0.88Mn0.12Li0.01Te與銅電極接點SEM圖、不同條件熱處理
BSE圖、(b)523K持溫15分鐘、(c) 773K持溫10分鐘、(d) 773K持溫24小時與
(e) 873K持溫24小時[42] .............................................................................................. 14
圖 1-13 Hf0.75Zr0.25NiSn0.99Sb0.01(n-type)與Hf0.5Zr0.5CoSb0.8Sn0.2 (p-type)對銅接點及元素
分析位置[45].................................................................................................................... 15
圖 1-14 Hf0.75Zr0.25NiSn0.99Sb0.01(n-type)與Hf0.5Zr0.5CoSb0.8Sn0.2 (p-type)對銅接點各點元
素分析位置與EDS mapping結果 .................................................................................. 16
圖 1-15熱電材料之EPMA截面圖(a)無Ni阻障層(b)1μm Ni阻障層[47] ........................ 18
圖 1-16不同Ni層厚度下的熱電模組發電效率[47] ........................................................... 18
圖 1-17 n-type與p-type有無阻障層之seebeck係數比值[48] ........................................... 19
圖 1-18(a)Ni/PbTe接點在400℃持溫60天之BSE圖 (b)Co/PbTe接點在400℃持溫60
天之EPMA元素分布圖 (c)Ni/Ag-Ge在400℃持溫7天之BSE圖 (d) Co/Ag-Ge在
400℃持溫7天之BSE圖 (e) Ni/Ag-Ge在750℃持溫30分鐘之BSE圖 (f) Co/Ag
Ge在750℃持溫30分鐘之BSE圖[52]........................................................................ 21
圖 3-1電子束撞擊試片時各類型訊號產生範圍示意圖[58] ............................................... 26
圖 4-1 各條件下SEM與EDS位置圖(a)為剛熔煉完之碲化錫(b)為熱壓完成之碲化錫 28
圖 4-2碲化錫熱壓前後的繞射峰圖譜 .................................................................................. 29
圖 4-3 (a)SnTe/AgCuZnSn/Cu接點之截面圖 (b)角落缺陷處放大圖 (c)
SnTe/AgCuZnSn/Cu截面放大圖 .................................................................................... 30
圖 4-4 SnTe經過700K熱時效測試1分鐘結果與碲化錫相圖[60] ................................... 31
圖 4-5 SnTe/AgCuZnSn/Cu截面EPMA mapping元素分布圖 ............................................ 31
圖 4-6 SnTe/AgCuZnSn/Cu截面EPMA點分析位置 .......................................................... 32
圖 4-7 SnTe/AgCuZnSn經過1、5、15天不同溫度下熱時效測試截面圖(a)500K(b)600K
.......................................................................................................................................... 33
圖 4-8 各條件下SnTe/AgCuZnSn/Cu接點強度 .................................................................. 34
viii
圖 4-9 SnTe/AgCuZnSn/Cu接合後推力測試破斷面 ............................................................ 35
圖 4-10 SnTe/AgCuZnSn/Cu斷裂位置截面圖 ...................................................................... 36
圖 4-11 SnTe/AgCuZnSn/Cu接點經過500K熱時效測試1、5與15天後的破斷面 ....... 36
圖 4-12 SnTe/AgCuZnSn/Cu接點經過600K熱時效測試1、5與15天後的破斷面 ....... 37
圖 4-13(a)為SnTe/Co/AgCuZnSn/Cu接點之截面圖 (b)角落處放大圖 (c)
SnTe/Co/AgCuZnSn/Cu接點之截面放大圖 .................................................................. 38
圖 4-14 SnTe/Co/AgCuZnSn之(a)SEM與(b)EDS點分析位置圖 ....................................... 39
圖 4-15 接合後EDS mapping圖 .......................................................................................... 40
圖 4-16接合後結構變化示意圖 ............................................................................................ 40
圖 4-17經過600K熱時效測試1天後SnTe/Co/AgCuZnSn之(a)SEM與(b)EDS點分析
位置圖 .............................................................................................................................. 42
圖 4-18經過600K熱時效測試1天後EDS mapping圖 .................................................... 42
圖 4-19經過600K熱時效測試1天後結構變化示意圖 ..................................................... 43
圖 4-20經過600K熱時效測試5天後SnTe/Co/AgCuZnSn之(a)SEM與EDS點分析位
置圖(b)放大倍率SEM與EDS點分析位置圖 .............................................................. 44
圖 4-21經過600K熱時效測試5天後EDS mapping圖 .................................................... 45
圖 4-22經過600K熱時效測試5天後結構改變示意圖 ..................................................... 45
圖 4-23經過600K熱時效測試15天後SnTe/Co/AgCuZnSn之(a)SEM與EDS點分析位
置圖(b)放大倍率SEM與EDS點分析位置圖 .............................................................. 46
圖 4-24經過600K熱時效測試15天後EDS mapping圖 .................................................. 47
圖 4-25經過600K熱時效測試15天後結構改變示意圖 ................................................... 47
圖 4-26 600K熱時效測試下是否添加Co層的推力強度 ................................................... 49
圖 4-27 SnTe /Co/AgCuZnSn/Cu硬焊接合後推力測試破斷面 ........................................... 50
圖 4-28 SnTe /Co/AgCuZnSn/Cu斷裂位置示意圖 ............................................................... 50
圖 4-29 SnTe/Co/AgCuZnSn/Cu經過600K溫度下熱時效測試1天之推力測試後破斷面
.......................................................................................................................................... 51
圖 4-30 SnTe/Co/AgCuZnSn/Cu經過600K溫度下熱時效測試1天後斷裂截面圖 ......... 51
圖 4-31 SnTe /Co/AgCuZnSn/Cu經過600K溫度下熱時效測試5天之推力測試後破斷面
.......................................................................................................................................... 52
圖 4-32 SnTe /Co/AgCuZnSn/Cu經過600K溫度下熱時效測試5天斷裂位置截面圖 .... 53
圖 4-33 SnTe /Co/AgCuZnSn/Cu經過600K溫度下熱時效測試15天之推力測試後破斷
面 ...................................................................................................................................... 53
圖 4-34 SnTe /Co/AgCuZnSn/Cu經過600K溫度下熱時效測試15天斷裂位置截面圖 .. 54
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[61] https://next-gen.materialsproject.org/materials (accessed 0616, 2024).指導教授 吳子嘉(Albert T. Wu) 審核日期 2024-8-19 推文 plurk
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