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研究生:季皖郁
研究生(外文):CHI, WAN-YU
論文名稱:透過3D列印製備氮化硼(BN)/熱塑性聚氨酯(TPU)熱介面材料之研究
論文名稱(外文):3D printing of Thermal Interface Material Using Boron Nitride (BN)/ Thermoplastic Polyurethane (TPU) Filaments
指導教授:蘇程裕蘇程裕引用關係楊哲化
指導教授(外文):SU, CHERNG-YUHYANG, CHE-HUA
口試委員:蘇程裕汪家昌張忠傑
口試委員(外文):SU, CHERNG-YUHWANG, JIA-CHANGCHANG, CHUNG-CHIEH
口試日期:2020-07-22
學位類別:碩士
校院名稱:國立臺北科技大學
系所名稱:機械工程系機電整合碩士班
學門:工程學門
學類:機械工程學類
論文種類:學術論文
論文出版年:2020
畢業學年度:108
語文別:中文
論文頁數:77
中文關鍵詞:氮化硼熱塑性聚氨酯複合材料熱介面材料熔融沉積成型
外文關鍵詞:Boron NitrideThermoplastic PolyurethaneCompositeTIMFDM
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開發同時具有高導熱率和優異機械性能的聚合物複合材料的需求日益增加。通過增加導熱填料含量來提高聚合物複合材料的導熱性是常用策略。然而,這將會導致複合材料的機械性能下降,且極大地限制了複合材料的實際工程應用。
故在本研究中,首先透過改質之氮化硼(bBN)作為導熱填料,提高熱塑性聚氨酯(TPU)基材的導熱性,並使用熔融混合技術製備bBN/TPU導熱複合線材。最後,利用熔融沉積成型系統(FDM)設計可壓縮結構之bBN/TPU複合熱介面結構材。研究結果顯示經改質後羥基化的bBN表現出良好的分散性和與基質的強介面粘附性,更提供連續的熱傳路徑。在填料含量10 wt%下,bBN/TPU複合材的熱傳導係數可達0.791 W/m‧K,相較於純TPU提升約達3.97倍。值得一提的是,透過FDM製備之bBN/TPU複合熱介面結構材,經壓縮循環試驗能維持原來應力的80.69%,且由動態力學分析儀(DMA)顯示儲能模量明顯提升。在這項研究中開發的過程非常簡便並且可進行客製化處理,此為傳統熱介面材料領域的設計和製備提供了一條新穎的途徑。

In recent years, the demand for polymer composites application in different fields has been significantly increasing, and thus developing polymer composites with both high thermal conductivity and excellent mechanical properties has become an important issue. Incorporation of the thermally conductive fillers in the polymeric matrix is one of the common strategies to improve the thermal conductivity of composites. However, as the excess amount of filler content added to the polymeric matrix, it will lead to some problems such as reduced processability of the composite and increased cost of the filler. These problems dramatically limit the use of composite materials in large‐scale manufacturing and engineering applications.
In this work, modified boron nitride (bBN) was used as the thermally conductive filler to enhance the thermal conductivity of the thermoplastic polyurethane (TPU) substrate. Then, TPU/BN composite filaments were fabricated by melt-compounding. Finally, compressible TPU/BN composites were prepared by Fused Deposition Modeling (FDM). The research results show that hydroxylated bBN exhibits good dispersion and strong interface adhesion with the matrix. Moreover, hydroxylated bBN can help form the continuous heat conduction paths in multiple dimensions. As the filler with 10 wt% content, the thermal conductivity of bBN / TPU can reach 0.791 Wm-1 K-1, which is nearly four times higher than that of neat TPU. It is noted that FDM printed TPU/BN composites can maintain 80.69% of the initial stress after the compression test. Furthermore, results collected from Dynamic Mechanical Analysis (DMA) also indicates the enhancement of storage modulus. The method developed in this work is facile to adopt and can be applied to various materials. Hence, this work provides a new path for the design and preparation of traditional thermal interface materials.

摘要 i
Abstract ii
誌謝 iv
目錄 v
圖目錄 viii
表目錄 x
第一章 緒論 1
1.1 前言 1
1.2 研究動機與目的 2
第二章 文獻回顧 4
2.1 熱介面材料(TIM) 4
2.2 熱傳遞機制 4
2.2.1 導熱陶瓷 6
2.3 導熱絕緣層複合材料 7
2.3.1 複合材料 7
2.3.2 導熱高分子複合材料 8
2.4 複合材料之原料 10
2.4.1 六方氮化硼(h-BN) 10
2.4.2 熱塑性聚氨酯(TPU) 12
2.5 氮化硼表面改質方法 13
2.6 氮化硼/高分子複合材料 18
2.7 熔融沉積成型(FDM) 22
2.7.1 高分子聚合物應用於FDM 23
2.7.2 陶瓷/高分子聚合物應用於FDM 24
第三章 實驗方法與步驟 26
3.1 實驗流程 26
3.2 氮化硼粉體表面改質 28
3.2.1 粉體原料 28
3.2.2 實驗藥品 28
3.2.3 粉體表面改質 28
3.3 h-BN/TPU複合線材製備 30
3.3.1 聚合物原料 30
3.3.2 TPU複合線材製備 30
3.3.2.1 雙螺桿押出機製備複合料粒 30
3.3.2.2 單螺桿押出機製備複合線材 31
3.4 h-BN/TPU複合材應用於FDM系統 31
3.4.1 結構模型與理念 32
3.4.2 FDM製程原理 33
3.4.3 FDM列印參數設定 33
3.5 分析儀器及原理 34
3.5.1 掃描式電子顯微鏡(SEM) 34
3.5.2 XRD相態分析 34
3.5.3 傅立葉轉換紅外線光譜分析儀(FT-IR) 35
3.5.4 熱傳導係數量測儀(Hot-Disk) 35
3.5.5 示差掃描量熱分析儀(DSC) 36
3.5.6 熱重損失分析儀(TGA) 36
3.5.7 拉伸試驗機 36
3.5.8 介電性質 37
3.5.9 熱顯像分析 37
3.5.10 壓縮疲勞試驗 38
3.5.11 動態機械性質分析儀(DMA) 38
第四章 結果與討論 39
4.1 傅立葉轉換紅外線光譜分析儀(FT-IR) 39
4.2 XRD相態分析 41
4.2.1 粉體XRD相態分析 42
4.2.2 複合材XRD相態分析 43
4.3 表面形貌分析 44
4.3.1 粉體表面形貌分析 44
4.3.2 複合材微結構分析 45
4.3.2.1 熱壓試片微結構分析 45
4.3.2.2 複合線材微結構分析 46
4.4 熱傳導特性分析(Hot-Disk) 48
4.5 複合材機械強度分析 50
4.5.1 拉伸試驗 50
4.5.2 拉伸斷面微結構分析 52
4.6熱性質分析 53
4.6.1熱重損失分析儀(TGA) 53
4.6.2示差掃描量熱分析儀(DSC) 55
4.7介電性質分析 55
4.8 複合熱介面結構材性質分析 57
4.8.1 熱顯像分析 57
4.8.2 壓縮循環試驗分析 61
4.8.3 動態機械性質分析(DMA) 65
第五章 結論 67
參考文獻 68
符號彙編 77

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